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Several publications have reported that total column ozone (TCO) may oscillate with an amplitude of up to 10 DU (Dobson units) during a solar eclipse, whereas other researchers have not seen evidence that an eclipse leads to variations in TCO beyond the typical natural variability. Here, we try to resolve these contradictions by measuring short-term variations (of seconds to minutes) in TCO using "global" (Sun and sky) and direct-Sun observations in the ultraviolet (UV) range with filter radiometers (GUVis-3511 and Microtops II®). Measurements were performed during three solar eclipses: the "Great American Eclipse" of 2024, which was observed in Mazatlán, Mexico, on 8 April 2024; a partial solar eclipse that took place in the United States on 14 October 2023 and was observed at Fort Collins, Colorado (40.57° N, 105.10° W); and a total solar eclipse that occurred in Antarctica on 4 December 2021 and was observed at Union Glacier (79.76° S, 82.84° W). The upper limits of the amplitude of oscillations in TCO observed at Mazatlán, Fort Collins, and Antarctica were 0.4 %, 0.3 %, and 0.03 %, respectively. The variability at all sites was within that observed during times not affected by an eclipse. The slightly larger variability at Mazatlán is due to cirrus clouds occurring throughout the day of the eclipse and the difficulty of separating changes in the ozone layer from cloud effects. These results support the conclusion that a solar eclipse does not lead to variations in TCO of more than ± 1.2 DU and that these variations are likely much lower, drawing into question reports of much larger oscillations. In addition to calculating TCO, we also present changes in the spectral irradiance and aerosol optical depth during eclipses and compare radiation levels observed during totality. The new results augment our understanding of the effect of a solar eclipse on the Earth's upper atmosphere. [ABSTRACT FROM AUTHOR]

We investigate the formation mechanism of a tropopause cirrus cloud layer observed during the Balloon measurement campaigns of the Asian Tropopause Aerosol Layer (BATAL) over Hyderabad (17.47° N, 78.58° E), India, on 23 August 2017. Simultaneous measurements from a backscatter sonde and an optical particle counter on board a balloon flight revealed the presence of a subvisible cirrus cloud layer (optical thickness ∼ 0.025) at the cold-point tropopause (temperature ∼ - 86.4 °C, altitude ∼ 17.9 km). Ice crystals in this layer are smaller than 50 µm with a layer mean ice crystal number concentration of about 46.79 L-1. Simultaneous backscatter and extinction coefficient measurements allowed us to estimate the range-resolved extinction to backscatter coefficient ratio (lidar ratio) inside this layer with a layer mean value of about 32.18 ± 6.73 sr, which is in good agreement with earlier reported values at similar cirrus cloud temperatures. The formation mechanism responsible for this tropopause cirrus is investigated using a combination of three-dimensional back trajectories, satellite observations, and ERA5 reanalysis data. Satellite observations revealed that the overshooting convection associated with a category 3 typhoon, Hato, which hit Macau and Hong Kong on 23 August 2017, injected ice into the lower stratosphere. This caused a hydration patch that followed the Asian summer monsoon anticyclone to subsequently move towards Hyderabad. The presence of tropopause cirrus cloud layers in the cold temperature anomalies and updrafts along the back trajectories suggested the role of typhoon-induced waves in their formation. This case study highlights the role of typhoons in influencing the formation of tropopause cirrus clouds through stratospheric hydration and waves. [ABSTRACT FROM AUTHOR]

Warm conveyor belts (WCBs) are coherent ascending airstreams in extratropical cyclones. They are a major source of moisture for the extratropical upper troposphere and lower stratosphere (UTLS), where moisture acts as a potent greenhouse gas and WCB-associated cirrus clouds contribute to cloud radiative forcing. However, the processes controlling WCB moisture transport and cloud properties are poorly characterised. Furthermore, recent studies have revealed (embedded) convection as a ubiquitous feature of WCBs, highlighting the importance of understanding their updraught and microphysical structure. We present a Lagrangian investigation of WCB moisture transport for a case from the WISE (Wave-driven ISentropic Exchange) campaign based on a convection-permitting simulation. Lagrangian non-dimensional metrics of the moisture budget suggest that the ascent timescale (τ600) strongly controls the end-of-ascent total moisture content, which is largest for slowly ascending trajectories (τ600≥20h , 30 % of all WCB trajectories). This is due to relatively warm end-of-ascent temperatures and the strong temperature control on transported water vapour. Deviations from equilibrium water vapour condensate partitioning are largest for slow trajectories due to faster glaciation and lower ice crystal numbers. A local moisture transport minimum at intermediate τ600 results from a shift towards a riming-dominated precipitation formation pathway and decreasing outflow temperatures with decreasing τ600. The fastest trajectories (τ600≤5h , 5 % of all WCB trajectories) transport the largest condensate mass to the UTLS due to less efficient condensate loss and produce the longest-lived outflow cirrus clouds. Models that parameterise convection may under-represent these processes, potentially impacting weather forecasts and climate predictions. [ABSTRACT FROM AUTHOR]

Globally, emissions from aviation affect Earth's climate via complex processes. Contrail cirrus and carbon dioxide emissions are the largest factors contributing to aviation's radiative forcing on climate. Contrail cirrus, like natural cirrus clouds, impacts Earth's climate. Even with the extensive ongoing research, the relative importance of the climate effects of contrails compared to other aviation effects on climate still has major uncertainties requiring further research. Contrail cirrus encompasses linear contrails and the associated cirrus clouds; these are characterized by ice particle properties, e.g., size, concentration, mixing, extinction, ice water content, optical depth, geometrical depth, and cloud coverage. The climate impact of contrails may intensify due to projected increases in air traffic. The radiative forcing from global contrail cirrus has the potential to triple and could reach as much as 160 mWm-2 by 2050. This projection is based on anticipated growth in air traffic and a potential shift to higher altitudes. The future climate impact of contrail cirrus is influenced by factors like the magnitude and geographical spread in air traffic, advancements in fuel efficiency, the effects of the use of alternative fuels, and the effects of the changing climate on the background atmosphere. This study reviews the microphysical processes affecting contrail formation and the aging of contrails and contrail cirrus. Furthermore, the study explores global observational datasets for contrails, current analyses, and future projections and will aid in evaluating the effectiveness and tradeoffs associated with various mitigation strategies. The research highlights gaps in knowledge and uncertainties while outlining research priorities for the future. [ABSTRACT FROM AUTHOR]

Global warming is amplified in the Arctic. However, numerical models struggle to represent key processes that determine Arctic weather and climate. To collect data that help to constrain the models, the HALO–(AC) 3 aircraft campaign was conducted over the Norwegian and Greenland seas, the Fram Strait, and the central Arctic Ocean in March and April 2022. The campaign focused on one specific challenge posed by the models, namely the reasonable representation of transformations of air masses during their meridional transport into and out of the Arctic via northward moist- and warm-air intrusions (WAIs) and southward marine cold-air outbreaks (CAOs). Observations were made over areas of open ocean, the marginal sea ice zone, and the central Arctic sea ice. Two low-flying and one long-range, high-altitude research aircraft were flown in colocated formation whenever possible. To follow the air mass transformations, a quasi-Lagrangian flight strategy using trajectory calculations was realized, enabling us to sample the same moving-air parcels twice along their trajectories. Seven distinct WAI and 12 CAO cases were probed. From the quasi-Lagrangian measurements, we have quantified the diabatic heating/cooling and moistening/drying of the transported air masses. During CAOs, maximum values of 3 K h -1 warming and 0.3 g kg -1 h -1 moistening were obtained below 1 km altitude. From the observations of WAIs, diabatic cooling rates of up to 0.4 K h -1 and a moisture loss of up to 0.1 g kg -1 h -1 from the ground to about 5.5 km altitude were derived. Furthermore, the development of cloud macrophysical (cloud-top height and horizontal cloud cover) and microphysical (liquid water path, precipitation, and ice index) properties along the southward pathways of the air masses were documented during CAOs, and the moisture budget during a specific WAI event was estimated. In addition, we discuss the statistical frequency of occurrence of the different thermodynamic phases of Arctic low-level clouds, the interaction of Arctic cirrus clouds with sea ice and water vapor, and the characteristics of microphysical and chemical properties of Arctic aerosol particles. Finally, we provide a proof of concept to measure mesoscale divergence and subsidence in the Arctic using data from dropsondes released during the flights. [ABSTRACT FROM AUTHOR]

Tropical tropopause layer (TTL) clouds have a significant impact on the Earth's radiative budget and regulate the amount of water vapor entering the stratosphere. Estimating the total coverage of tropical cirrus clouds is challenging, since the range of their optical depth spans several orders of magnitude, from thick opaque cirrus detrained from convection to sub-visible clouds just below the stratosphere. During the Strateole-2 observation campaign, three microlidars were flown on board stratospheric superpressure balloons from October 2021 to late January 2022, slowly drifting only a few kilometers above the TTL. These measurements have unprecedented sensitivity to thin cirrus and provide a fine-scale description of cloudy structures both in time and in space. Case studies of collocated observations with the spaceborne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) show very good agreement between the instruments and highlight the Balloon-borne Cirrus and convective overshOOt Lidar's (BeCOOL) higher detection sensitivity. Indeed, the microlidar is able to detect optically very thin clouds (optical depth τ<2×10-3) that are undetected by CALIOP. Statistics on cloud occurrence show that TTL cirrus appear in about 50 % of the microlidar profiles and have a mean geometrical depth of 1 km. Ultrathin TTL cirrus (τ<2×10-3) have a significant coverage (23 % of the profiles), and their mean geometrical depth is 0.5 km. [ABSTRACT FROM AUTHOR]

Warm-air intrusions (WAIs) are responsible for the transportation of warm and moist air masses from the mid-latitudes into the high Arctic (> 70° N). In this work, we study cirrus clouds that form during WAI events (WAI cirrus) and during undisturbed Arctic conditions (AC cirrus) and investigate possible differences between the two cloud types based on their macrophysical and optical properties with a focus on relative humidity over ice (RHi). We use airborne measurements from the combined high-spectral-resolution and differential-absorption lidar, WALES, performed during the HALO-(AC) 3 campaign. We classify each research flight and the measured clouds as either AC or WAI, based on the ambient conditions, and study the macrophysical, geometrical and optical characteristics for each cirrus group. As our main parameter we choose the relative humidity over ice (RHi), which we calculate RHi by combining the lidar water vapor measurements with model temperatures. Ice formation occurs at certain RHi values depending on the dominant nucleation process taking place. RHi can thus be used as an indication of the nucleation process and the structure of cirrus clouds. We find that during WAI events the Arctic is warmer and moister and WAI cirrus clouds are both geometrically and optically thicker compared to AC cirrus. WAI cirrus clouds and the layer directly surrounding them are more frequently supersaturated, also at high supersaturations over the threshold for homogeneous ice nucleation (HOM). AC cirrus clouds have a supersaturation-dominated cloud top and a subsaturated cloud base. WAI cirrus clouds also have high supersaturations at cloud top but also at cloud base. [ABSTRACT FROM AUTHOR]

The ice phase impacts many cloud properties as well as cloud lifetime. Ice particles that sediment into a lower cloud from an upper cloud (external seeder–feeder process) or into the mixed-phase region of a deep cloud from cirrus levels (internal seeder–feeder process) can influence the ice phase of the lower cloud, amplify cloud glaciation and enhance surface precipitation. Recently, numerical weather prediction modeling studies have aimed at representing the ice crystal number concentration in mixed-phase clouds more accurately by including secondary ice formation processes. The increase in the ice crystal number concentration can impact the number of ice particles that sediment into the lower cloud and alter its composition and precipitation formation. In the Swiss Alps, the orography permits the formation of orographic clouds, making it ideal for studying the occurrence of multi-layered clouds and the seeder–feeder process. We present results from a case study on 18 May 2016, showing the occurrence frequency of multi-layered clouds and the seeder–feeder process. About half of all observed clouds were categorized as multi-layered, and the external seeder–feeder process occurred in 10 % of these clouds. Between cloud layers, ≈60 % of the ice particle mass was lost due to sublimation or melting. The external seeder–feeder process was found to be more important than the internal seeder–feeder process with regard to the impact on precipitation. In the case where the external seeder–feeder process was inhibited, the average surface precipitation and riming rate over the domain were both reduced by 8.5 % and 3.9 %, respectively. When ice–graupel collisions were allowed, further large reductions were seen in the liquid water fraction and riming rate. Inhibiting the internal seeder–feeder process enhanced the liquid water fraction by 6 % compared to a reduction of 5.8 % in the cloud condensate, therefore pointing towards the de-amplification in cloud glaciation and a reduction in surface precipitation. Adding to the observational evidence of frequent seeder–feeder situations, at least over Switzerland, our study highlights the extensive influence of sedimenting ice particles on the properties of feeder clouds as well as on precipitation formation. [ABSTRACT FROM AUTHOR]

Ice-nucleating particles catalyze ice formation in clouds, affecting climate through radiative forcing from aerosol–cloud interactions. Aviation directly emits particles into the upper troposphere where ice formation conditions are favorable. Previous studies have used proxies of aviation soot to estimate their ice nucleation activity; however, investigations with commercial aircraft soot from modern in-use aircraft engines have not been quantified. In this work, we sample aviation soot particles at ground level from different commercial aircraft engines to test their ice nucleation ability at temperatures ≤228 K as a function of engine thrust and soot particle size. Additionally, soot particles were catalytically stripped to reveal the impact of mixing state on their ice nucleation ability. Particle physical and chemical properties were further characterized and related to the ice nucleation properties. The results show that aviation soot nucleates ice at or above relative humidity conditions required for homogeneous freezing of solution droplets (RH hom). We attribute this to a mesopore paucity inhibiting pore condensation and the sulfur content which suppresses freezing. Only large soot aggregates (400 nm) emitted under 30 %–100 % thrust conditions for a subset of engines (2 out of 10) nucleate ice via pore condensation and freezing. For those specific engines, the presence of hydrophilic chemical groups facilitates the nucleation. Aviation soot emitted at thrust ≥ 100 % (sea level thrust) nucleates ice at or above RH hom. Overall, our results suggest that aviation soot will not contribute to natural cirrus formation and can be used in models to update impacts of soot–cirrus clouds. [ABSTRACT FROM AUTHOR]

Atmospheric aerosols can act as ice-nucleating particles (INPs) and influence the formation and the microphysical properties of cirrus clouds, resulting in distinct climate effects. We employ a global aerosol–climate model, including a two-moment cloud microphysical scheme and a parameterization for aerosol-induced ice formation in cirrus clouds, to quantify the climate impact of INPs on cirrus clouds (simulated period 2001–2010). The model considers mineral dust, soot, crystalline ammonium sulfate, and glassy organics as INPs in the cirrus regime. Several sensitivity experiments are performed to analyse various aspects of the simulated INP–cirrus effect regarding (i) the ice-nucleating potential of the INPs, (ii) the inclusion of ammonium sulfate and organic particles as INPs in the model, and (iii) the model representations of vertical updraughts. The resulting global radiative forcing of the total INP–cirrus effect, considering all different INP types, assuming a smaller and a larger ice-nucleating potential of INPs, to explore the range of possible forcings due to uncertainties in the freezing properties of INPs, is simulated as -28 and -55 mW m -2 , respectively. While the simulated impact of glassy organic INPs is mostly small and not statistically significant, ammonium sulfate INPs contribute a considerable radiative forcing, which is nearly as large as the combined effect of mineral dust and soot INPs. Additionally, the anthropogenic INP–cirrus effect is analysed considering the difference between present-day (2014) and pre-industrial conditions (1750) and amounts to -29 mW m -2 , assuming a larger ice-nucleating potential of INPs. In a further sensitivity experiment we analyse the effect of highly efficient INPs proposed for cirrus cloud seeding as a means to reduce global warming by climate engineering. However, the results indicate that this approach risks an overseeding of cirrus clouds and often results in positive radiative forcings of up to 86 mW m -2 depending on number concentration of seeded INPs. Idealized experiments with prescribed vertical velocities highlight the crucial role of the model dynamics for the simulated INP–cirrus effects. For example, resulting forcings increase about 1 order of magnitude (-42 to -340 mW m -2) when increasing the prescribed vertical velocity (from 1 to 50 cm s -1). The large discrepancy in the magnitude of the simulated INP–cirrus effect between different model studies emphasizes the need for future detailed analyses and efforts to reduce this uncertainty and constrain the resulting climate impact of INPs. [ABSTRACT FROM AUTHOR]

Sea spray aerosols (SSAs) represent one of the most abundant aerosol types on a global scale and have been observed at all altitudes including the upper troposphere. SSA has been explored in recent years as a source of ice-nucleating particles (INPs) in cirrus clouds due to the ubiquity of cirrus clouds and the uncertainties in their radiative forcing. This study expands upon previous works on low-temperature ice nucleation of SSA by investigating the effects of atmospheric aging of SSA and the ice-nucleating activity of newly formed secondary marine aerosols (SMAs) using an oxidation flow reactor. Polydisperse aerosol distributions were generated from a marine aerosol reference tank (MART) filled with 120 L of real or artificial seawater and were dried to very low relative humidity to crystallize the salt constituents of SSA prior to their subsequent freezing, which was measured using a continuous flow diffusion chamber (CFDC). Results show that for primary SSA (pSSA), as well as aged SSA and SMA (aSSA + SMA) at temperatures >220 K, homogeneous conditions (92 %–97 % relative humidity with respect to water – RH w) were required to freeze 1 % of the particles. However, below 220 K, heterogeneous nucleation occurs for both pSSA and aSSA + SMA at much lower RH w , where up to 1 % of the aerosol population freezes between 75 % and 80 % RH w. Similarities between freezing behaviors of the pSSA and aSSA + SMA at all temperatures suggest that the contributions of condensed organics onto the pSSA or alteration of functional groups in pSSA via atmospheric aging did not hinder the major heterogeneous ice nucleation process at these cirrus temperatures, which have previously been shown to be dominated by the crystalline salts. Occurrence of a 1 % frozen fraction of SMA, generated in the absence of primary SSA, was observed at or near water saturation below 220 K, suggesting it is not an effective INP at cirrus temperatures, similar to findings in the literature on other organic aerosols. Thus, any SMA coatings on the pSSA would only decrease the ice nucleation behavior of pSSA if the organic components were able to significantly delay water uptake of the inorganic salts, and apparently this was not the case. Results from this study demonstrate the ability of lofted primary sea spray particles to remain an effective ice nucleator at cirrus temperatures, even after atmospheric aging has occurred over a period of days in the marine boundary layer prior to lofting. We were not able to address aging processes under upper-tropospheric conditions. [ABSTRACT FROM AUTHOR]

Cirrus clouds play an important role in the radiation budget of the Earth; nonetheless, the radiative effect of ultra-thin cirrus clouds in the tropopause region and in the lowermost stratosphere remains poorly constrained. These clouds have a small vertical extent and optical depth and are frequently neither observed even by sensitive sensors nor considered in climate model simulations. In addition, their short-wave (cooling) and long-wave (warming) radiative effects are often in approximate balance, and their net effect strongly depends on the shape and size of the cirrus particles. However, the CRyogenic Infrared Spectrometers and Telescopes for the Atmosphere instrument (CRISTA-2) allows ultra-thin cirrus clouds to be detected. Here we use CRISTA-2 observations in summer 1997 in the Northern Hemisphere midlatitudes together with the Suite Of Community RAdiative Transfer codes based on Edwards and Slingo (SOCRATES) radiative transfer model to calculate the radiative effect of observed ultra-thin cirrus. Using sensitivity simulations with different ice effective particle size and shape, we provide an estimate of the uncertainty in the radiative effect of ultra-thin cirrus in the extratropical lowermost stratosphere and tropopause region during summer and – by extrapolation of the summer results – for winter. Cloud top height and ice water content are based on CRISTA-2 measurements, while the cloud vertical thickness was predefined to be 0.5 or 2 km. Our results indicate that if the ice crystals of these thin cirrus clouds are assumed to be spherical, their net cloud radiative effect is generally positive (warming). In contrast, assuming aggregates or a hexagonal shape, their net radiative effect is generally negative (cooling) during summer months and very likely positive (warming) during winter. The radiative effect is in the order of ± (0.1–0.01) Wm-2 for a realistic global cloud coverage of 10 %, similar to the magnitude of the contrail cirrus radiative forcing (of ∼ 0.1 Wm-2). The radiative effect is also dependent on the cloud vertical extent and consequently the optically thickness and effective radius of the particle size distribution (e.g. effective radius increase from 5 to 30 µm results in a factor ∼ 6 smaller long- and short-wave effects, respectively). The properties of ultra-thin cirrus clouds in the lowermost stratosphere and tropopause region need to be better observed, and ultra-thin cirrus clouds need to be evaluated in climate model simulations. [ABSTRACT FROM AUTHOR]

A significant share of aviation's climate impact is due to persistent contrails. Thus, avoiding the creation of contrails that exert a warming impact is a crucial step in approaching the goal of sustainable air transportation. For this purpose, a reliable forecast of when and where persistent contrails are expected to form is needed (i.e. a reliable prediction of ice supersaturation). With such a forecast at hand, it would be possible to plan aircraft routes on which the formation of persistent contrails can be avoided. One problem on the way to these forecasts is the current systematic underestimation of the frequency and degree of ice supersaturation at cruise altitudes in numerical weather prediction due to the practice of "saturation adjustment". In this common parameterisation, the air inside cirrus clouds is assumed to be exactly at ice saturation, while measurement studies have found cirrus clouds to be quite often out of equilibrium. In this study, we propose a new ice-cloud scheme that overcomes saturation adjustment by explicitly modelling the decay of the in-cloud humidity after nucleation, thereby allowing for both in-cloud super- and subsaturation. To achieve this, we introduce the in-cloud humidity as a new prognostic variable and derive the humidity distribution in newly generated cloud parts from a stochastic box model that divides a model grid box into a large number of air parcels and treats them individually. The new scheme is then tested against a parameterisation that uses saturation adjustment, where the stochastic box model serves as a benchmark. It is shown that saturation adjustment underestimates humidity, both shortly after nucleation, when the actual cloud is still highly supersaturated, and also in aged cirrus if the temperature keeps decreasing, as the actual cloud remains in a slightly supersaturated state in this case. The new parameterisation, on the other hand, closely follows the behaviour of the stochastic box model in any considered case. The improvement in comparison with saturation adjustment is largest if slow updraughts occur in relatively clean air in models with a high spatial and temporal resolution. We conclude that our parameterisation is promising but needs further testing in more realistic frameworks. [ABSTRACT FROM AUTHOR]

Tropical cirrus clouds, i.e., any type of ice cloud with tops above 400 hPa, play a critical role in the climate system and are a major source of uncertainty in our understanding of global warming. Tropical cirrus clouds involve processes spanning a wide range of spatial and temporal scales, from ice microphysics on cloud scales to mesoscale convective organization and planetary wave dynamics. This complexity makes tropical cirrus clouds notoriously difficult to model and has left many important questions stubbornly unanswered. At the same time, their multi-scale nature makes them well-positioned to benefit from the rise of global, high-resolution simulations of Earth's atmosphere and a growing abundance of remotely sensed and in situ observations. Rapid progress on our understanding of tropical cirrus requires coordinated efforts to take advantage of these modern computational and observational abilities. In this opinion paper, we review recent progress in cirrus studies, highlight important unanswered questions, and discuss promising paths forward. Significant progress has been made in understanding the life cycle of convectively generated "anvil" cirrus and the response of their macrophysical properties to large-scale controls. On the other hand, much work remains to be done to fully understand how small-scale anvil processes and the climatological anvil radiative effect will respond to global warming. Thin, in situ formed cirrus clouds are now known to be closely tied to the thermal structure and humidity of the tropical tropopause layer, but microphysical uncertainties prevent a full understanding of this link, as well as the precise amount of water vapor entering the stratosphere. Model representation of ice-nucleating particles, water vapor supersaturation, and ice depositional growth continue to pose great challenges to cirrus modeling. We believe that major advances in the understanding of tropical cirrus can be made through a combination of cross-tool synthesis and cross-scale studies conducted by cross-disciplinary research teams. [ABSTRACT FROM AUTHOR]

Tropical deep convective clouds, particularly their large cirrus outflows, play an important role in modulating the energy balance of the Earth's atmosphere. Whilst the cores of these deep convective clouds have a significant short-wave (SW) cooling effect, they dissipate quickly. Conversely, the thin cirrus that flow from these cores can persist for days after the core has dissipated, reaching hundreds of kilometres in extent. These thin cirrus have a potential for large warming in the tropics. Understanding the evolution of air parcels from deep convection, clouds along these trajectories, and how they change in response to anthropogenic emissions is therefore important to understand past and future climate change. This work uses a novel approach to investigate the evolution of tropical convective clouds by introducing the concept of "time since convection" (TSC). This is used to build a composite picture of the lifecycle of air parcels from deep convection. Cloud properties are a strong function of TSC, showing decreases in the optical thickness, cloud-top height, and cloud fraction over time, thereby driving the latitudinal structure of cloudiness. After an initial dissipation of the convective core, changes in thin cirrus cloud amount were seen beyond 200 h from convection. Changes in cloud are shown to be a strong function of TSC and not simply reflective of latitudinal changes as air moves from the tropics to the extratropics. Finally, in the initial stages of convection there was a large net negative cloud radiative effect (CRE). However, once the convective core had dissipated, the sign of the CRE flipped and there was a sustained net warming CRE beyond 120 h from the convective event. Changes are present in the cloud properties long after the main convective activities have dissipated, signalling the need to continue further analysis at longer timescales than previously studied. [ABSTRACT FROM AUTHOR]

Natural cirrus clouds and contrails cover about 30 % of the Earth's mid-latitudes and up to 70 % of the tropics. Due to their widespread occurrence, cirrus clouds have a considerable impact on the Earth energy budget, which, on average, leads to a warming net radiative effect (solar + thermal infrared). However, whether the instantaneous radiative effect (RE), which in some cases corresponds to a radiative forcing, of natural cirrus or contrails is positive or negative depends on their microphysical, macrophysical, and optical properties, as well as the radiative properties of the environment. This is further complicated by the fact that the actual ice crystal shape is often unknown, and thus, ice clouds remain one of the components that are least understood in the Earth's radiative budget. The present study aims to investigate the dependency of the effect on cirrus RE on eight parameters, namely solar zenith angle, ice water content, ice crystal effective radius, cirrus temperature, surface albedo, surface temperature, cloud optical thickness of an underlying liquid water cloud, and three ice crystal shapes. In total, 283 500 plane-parallel radiative transfer simulations have been performed, not including three-dimensional scattering effects. Parameter ranges are selected that are typically associated with natural cirrus and contrails. In addition, the effect of variations in the relative humidity profile and the ice cloud geometric thickness have been investigated for a sub-set of the simulations. The multi-dimensionality and complexity of the eight-dimensional parameter space makes it impractical to discuss all potential configurations in detail. Therefore, specific cases are selected and discussed. For a given parameter combination, the largest impact on solar, thermal-infrared (TIR), and net RE is related to the ice crystal effective radius. The second most important parameter is ice water content, which equally impacts the solar and terrestrial RE. The solar RE of cirrus is also determined by solar zenith angle, surface albedo, liquid cloud optical thickness, and ice crystal shape (in descending priority). RE in the TIR spectrum is dominated by surface temperature, ice cloud temperature, liquid water cloud optical thickness, and ice crystal shape. Net RE is controlled by surface albedo, solar zenith angle, and surface temperature in decreasing importance. The relative importance of the studied parameters differs, depending on the ambient conditions. Furthermore, and during nighttime the net RE is equal to the TIR RE. The data set generated in this work is publicly available. It can be used as a lookup table to extract the RE of cirrus clouds, contrails, and contrail cirrus instead of full radiative transfer calculations. [ABSTRACT FROM AUTHOR]

To date the climate intervention (CI) proposal of cirrus cloud thinning (CCT) was only assessed in general circulation models (GCMs) using a globally uniform distribution of artificial ice nucleating particles (INPs). In this study, we made the first attempt using the ECHAM–HAM (Hamburg Aerosol Module) GCM to simulate CCT using a fully prognostic cirrus seeding aerosol species. Seeding particles were assumed to be made of bismuth triiodide and were emitted into the atmosphere following aircraft emissions of black carbon (soot). This new approach drastically reduced the number concentration of seeding particles available as INPs in our cirrus ice nucleation sub-model compared to the globally uniform approach. As a result, we found that in order to achieve a significant signal we needed to reduce the assumed radius of emitted seeding particles by an order of magnitude to 0.01 µm and scale the mass emissions of seeding particles by at least a factor of 100 or 1000. This latter scaling factor led to a large net top-of-atmosphere (TOA) warming effect of 5.9 W m -2. This warming effect was a clear response to overseeding with a large concentration of seeding particles (>105 L -1 in the Northern Hemisphere) that was most evident in the tropics. Due to this undesired effect, in a second series of simulations we avoided seeding the tropics by restricting emissions to only the Northern Hemisphere (NH) during winter. We also found a small and insignificant effect, or overseeding, which for the extreme case was reduced compared to the global aircraft emission scenario (2.2 W m -2). Ice crystal radius anomalies were not what we expected, with the largest reduction in size found for the case with a mass scaling factor of 10 instead of the extreme, × 1000, scenario. We attributed this peculiar behavior to the differences in the competition between different seeding particle concentrations and background particles. Finally, we also found that seeding with such large concentrations increased the albedo effect of mixed-phase clouds in the NH due to less efficient cloud droplet consumption, consistent with previous findings from our model. Overall, however, based on this study it is recommended to pause further modeling efforts of CCT unless more observational-based evidence of aerosol–ice-cloud interactions indicates favorable conditions for producing the desired outcome of this CI proposal. [ABSTRACT FROM AUTHOR]

The role of gravity waves on microphysics of tropical cirrus clouds and air-parcel dehydration was studied using the combination of Lagrangian observations of temperature fluctuations and a 1.5D model. High-frequency measurements during isopycnal balloon flights were used to resolve the gravity-wave signals with periods ranging from a few days to 10 min. The detailed microphysical simulations with homogeneous freezing, sedimentation, and a crude horizontal mixing represent the slow ascent of air parcels in the tropical tropopause layer (TTL). A reference simulation describes the slow ascent of air parcels in the tropical tropopause layer, with nucleation occurring only below the cold-point tropopause with a small ice-crystal density. The inclusion of the gravity waves drastically modifies the vertical profile of low ice concentration and weak dehydration found during the ascent alone, with the increased ice-crystal number and size distribution agreeing better with observations. Numerous events of nucleation occur below and above the cold-point tropopause, efficiently restoring the relative humidity over ice to equilibrium with respect to the background temperature, as well as increasing the cloud fraction in the vicinity of the cold-point tropopause. The corresponding decrease in water vapor is estimated at 2 ppmv around the cold-point tropopause. [ABSTRACT FROM AUTHOR]

Dusty cirrus clouds are extended optically thick cirrocumulus decks that occur during strong mineral dust events. So far they have mostly been documented over Europe associated with dust-infused baroclinic storms. Since today's global numerical weather prediction models neither predict mineral dust distributions nor consider the interaction of dust with cloud microphysics, they cannot simulate this phenomenon. We postulate that the dusty cirrus forms through a mixing instability of moist clean air with drier dusty air. A corresponding sub-grid parameterization is suggested and tested in the ICOsahedral Nonhydrostatic model with Aerosol and Reactive Trace gases (ICON-ART). Only with the help of this parameterization is ICON-ART able to simulate the formation of the dusty cirrus, which leads to substantial improvements in cloud cover and radiative fluxes compared to simulations without this parameterization. A statistical evaluation over six Saharan dust events with and without observed dusty cirrus shows robust improvements in cloud and radiation scores. The ability to simulate dusty cirrus formation removes the linear dependency on mineral dust aerosol optical depth from the bias of the radiative fluxes. For the six Saharan dust episodes investigated in this study, the formation of dusty cirrus clouds is the dominant aerosol–cloud–radiation effect of mineral dust over Europe. [ABSTRACT FROM AUTHOR]

Ice growth from vapor deposition is an important process for the evolution of cirrus clouds, but the physics of depositional ice growth at the low temperatures (<235 K) characteristic of the upper troposphere and lower stratosphere is not well understood. Surface attachment kinetics, generally parameterized as a deposition coefficient αD , control ice crystal habit and also may limit growth rates in certain cases, but significant discrepancies between experimental measurements have not been satisfactorily explained. Experiments on single ice crystals have previously indicated the deposition coefficient is a function of temperature and supersaturation, consistent with growth mechanisms controlled by the crystal's surface characteristics. Here we use observations from cloud chamber experiments in the Aerosol Interactions and Dynamics in the Atmosphere (AIDA) aerosol and cloud chamber to evaluate surface kinetic models in realistic cirrus conditions. These experiments have rapidly changing temperature, pressure, and ice supersaturation such that depositional ice growth may evolve from diffusion limited to surface kinetics limited over the course of a single experiment. In Part 1, we describe the adaptation of a Lagrangian parcel model with the Diffusion Surface Kinetics Ice Crystal Evolution (DiSKICE) model to the AIDA chamber experiments. We compare the observed ice water content and saturation ratios to that derived under varying assumptions for ice surface growth mechanisms for experiments simulating ice clouds between 180 and 235 K and pressures between 150 and 300 hPa. We found that both heterogeneous and homogeneous nucleation experiments at higher temperatures (>205 K) could generally be modeled consistently with either a constant deposition coefficient or the DiSKICE model assuming growth on isometric crystals via abundant surface dislocations. Lower-temperature experiments showed more significant deviations from any depositional growth model, with different ice growth rates for heterogeneous and homogeneous nucleation experiments. [ABSTRACT FROM AUTHOR]

The Geoengineering Model Intercomparison Project (GeoMIP) is a coordinating framework, started in 2010, that includes a series of standardized climate model experiments aimed at understanding the physical processes and projected impacts of solar geoengineering. Numerous experiments have been conducted, and numerous more have been proposed as "test-bed" experiments, spanning a variety of geoengineering techniques aimed at modifying the planetary radiation budget: stratospheric aerosol injection, marine cloud brightening, surface albedo modification, cirrus cloud thinning, and sunshade mirrors. To date, more than 100 studies have been published that used results from GeoMIP simulations. Here we provide a critical assessment of GeoMIP and its experiments. We discuss its successes and missed opportunities, for instance in terms of which experiments elicited more interest from the scientific community and which did not, and the potential reasons why that happened. We also discuss the knowledge that GeoMIP has contributed to the field of geoengineering research and climate science as a whole: what have we learned in terms of intermodel differences, robustness of the projected outcomes for specific geoengineering methods, and future areas of model development that would be necessary in the future? We also offer multiple examples of cases where GeoMIP experiments were fundamental for international assessments of climate change. Finally, we provide a series of recommendations, regarding both future experiments and more general activities, with the goal of continuously deepening our understanding of the effects of potential geoengineering approaches and reducing uncertainties in climate outcomes, important for assessing wider impacts on societies and ecosystems. In doing so, we refine the purpose of GeoMIP and outline a series of criteria whereby GeoMIP can best serve its participants, stakeholders, and the broader science community. [ABSTRACT FROM AUTHOR]

The tropical tropopause layer (TTL) is a sea of vertical motions. Convectively generated gravity waves create vertical winds on scales of a few to thousands of kilometers as they propagate in a stable atmosphere. Turbulence from gravity wave breaking, radiatively driven convection, and Kelvin–Helmholtz instabilities stirs up the TTL on the kilometer scale. TTL cirrus clouds, which moderate the water vapor concentration in the TTL and stratosphere, form in the cold phases of large-scale (> 100 km) wave activity. It has been proposed in several modeling studies that small-scale (< 100 km) vertical motions control the ice crystal number concentration and the dehydration efficiency of TTL cirrus clouds. Here, we present the first observational evidence for this. High-rate vertical winds measured by aircraft are a valuable and underutilized tool for constraining small-scale TTL vertical wind variability, examining its impacts on TTL cirrus clouds, and evaluating atmospheric models. We use 20 Hz data from five National Aeronautics and Space Administration (NASA) campaigns to quantify small-scale vertical wind variability in the TTL and to see how it varies with ice water content, distance from deep convective cores, and height in the TTL. We find that 1 Hz vertical winds are well represented by a normal distribution, with a standard deviation of 0.2–0.4 m s -1. Consistent with a previous observational study that analyzed two out of the five aircraft campaigns that we analyze here, we find that turbulence is enhanced over the tropical west Pacific and within 100 km of convection and is most common in the lower TTL (14–15.5 km), closer to deep convection, and in the upper TTL (15.5–17 km), further from deep convection. An algorithm to classify turbulence and long-wavelength (5 km < λ < 100 km) and short-wavelength (λ < 5 km) gravity wave activity during level flight legs is applied to data from the Airborne Tropical TRopopause EXperiment (ATTREX). The most commonly sampled conditions are (1) a quiescent atmosphere with negligible small-scale vertical wind variability, (2) long-wavelength gravity wave activity (LW GWA), and (3) LW GWA with turbulence. Turbulence rarely occurs in the absence of gravity wave activity. Cirrus clouds with ice crystal number concentrations exceeding 20 L -1 and ice water content exceeding 1 mg m -3 are rare in a quiescent atmosphere but about 20 times more likely when there is gravity wave activity and 50 times more likely when there is also turbulence, confirming the results of the aforementioned modeling studies. Our observational analysis shows that small-scale gravity waves strongly influence the ice crystal number concentration and ice water content within TTL cirrus clouds. Global storm-resolving models have recently been run with horizontal grid spacing between 1 and 10 km, which is sufficient to resolve some small-scale gravity wave activity. We evaluate simulated vertical wind spectra (10–100 km) from four global storm-resolving simulations that have horizontal grid spacing of 3–5 km with aircraft observations from ATTREX. We find that all four models have too little resolved vertical wind at horizontal wavelengths between 10 and 100 km and thus too little small-scale gravity wave activity, although the bias is much less pronounced in global SAM than in the other models. We expect that deficient small-scale gravity wave activity significantly limits the realism of simulated ice microphysics in these models and that improved representation requires moving to finer horizontal and vertical grid spacing. [ABSTRACT FROM AUTHOR]

Water vapor measurements of midlatitude cirrus clouds, obtained by the WAter vapour Lidar Experiment in Space (WALES) lidar system during the Mid-Latitude Cirrus (ML-CIRRUS) airborne campaign, which took place in the spring of 2014 over central Europe and the NE Atlantic Ocean, are combined with model temperatures from the European Centre for Medium-Range Weather Forecasts (ECMWF) and analyzed. Our main focus is to derive the distribution and temporal evolution of humidity with respect to ice within cirrus clouds and in their adjacent cloud-free air. We find that 34.1 % of in-cloud data points are supersaturated with respect to ice. Supersaturation is also detected in 6.8 % of the cloud-free data points. When the probability density of the relative humidity over ice (RHi) is calculated with respect to temperature for the in-cloud data points from the ML-CIRRUS dataset, there are two peaks: one around 225 K and close to saturation, RHi = 100 %, and a second one at colder temperatures around 218 K in subsaturation, RHi = 79 %. These two regions seem to represent two cirrus cloud categories: in situ formed and liquid origin. Regarding their vertical structure, most clouds have higher supersaturations close to the cloud top and become subsaturated near the cloud bottom. Finally, we find that the vertical structure of RHi within the clouds is also indicative of their life stage. RHi skewness tends to go from positive to negative values as the cloud ages. RHi modes are close to saturation in young clouds, supersaturated in mature clouds and subsaturated in dissipating clouds. [ABSTRACT FROM AUTHOR]

Cirrus clouds that form in the tropical tropopause layer (TTL) can play a key role in vertical transport through the upper troposphere and lower stratosphere, which can significantly impact the radiative energy budget and stratospheric chemistry. However, the lack of realistic representation of natural ice cloud habits in microphysical parameterizations can lead to uncertainties in cloud-related processes and cloud–climate feedbacks. The main goal of this study is to investigate the role of different cloud regimes and the associated ice habits in regulating the properties of the TTL. We compare aircraft measurements from the StratoClim field campaign to a set of numerical experiments at the scale of large-eddy simulations (LESs) for the same case study that employ different microphysics schemes. Aircraft measurements over the southern slopes of the Himalayas captured high ice water content (HIWC) up to 2400 ppmv and ice particle aggregates exceeding 700 µ m in size with unusually long residence times. The observed ice particles were mainly of liquid origin, with a small amount formed in situ. The corresponding profile of ice water content (IWC) from the ERA5 reanalysis corroborates the presence of HIWC detrained from deep-convective plumes in the TTL but underestimates HIWC by an order of magnitude. In the TTL, only the scheme that predicts ice habits can reproduce the observed HIWC, ice number concentration, and bimodal ice particle size distribution. The lower range of particle sizes is mostly represented by planar and columnar habits, while the upper range is dominated by aggregates. Large aggregates with sizes between 600 and 800 µ m have fall speeds of less than 20 cm s -1 , which explains the long residence time of the aggregates in the TTL. Planar ice particles of liquid origin contribute substantially to HIWC. The columnar and aggregate habits are in the in situ range with lower IWC and number concentrations. For all habits, the ice number concentration increases with decreasing temperature. For the planar ice habit, relative humidity is inversely correlated with fall speed. This correlation is less evident for the other two ice habits. In the lower range of supersaturation with respect to ice, the columnar habit has the highest fall speed. The difference in ice number concentration across habits can be up to 4 orders of magnitude, with aggregates occurring in much smaller numbers. We demonstrate and quantify the linear relationship between the differential sedimentation of pristine ice crystals and the size of the aggregates that form when pristine crystals collide. The slope of this relationship depends on which pristine ice habit sediments faster. Each simulated ice habit is associated with distinct radiative and latent heating rates. This study suggests that a model configuration nested down to LES scales with a microphysical parameterization that predicts ice shape evolution is crucial to provide an accurate representation of the microphysical properties of TTL cirrus and thus the associated (de)hydration process. [ABSTRACT FROM AUTHOR]

Microphysical, optical, and environmental properties of contrail cirrus and natural cirrus were investigated by applying a new, statistically based contrail–cirrus separation method to 14.7 h of cirrus cloud measurements (sampling frequency 1 Hz, max. ∼ 290 m s -1 , total length of sampled in-cloud space ∼ 15 000 km) during the airborne campaign ML-CIRRUS in central Europe and the northeast Atlantic flight corridor in spring 2014. We find that pure contrail cirrus appears frequently at the aircraft cruising altitude (CA) range with ambient pressure varying from 200 to 245 hPa. It exhibits a higher median ice particle number concentration (Nice), a smaller median mass mean radius (Rice), and lower median ice water content (IWC) (median: Nice=0.045 cm -3 , Rice=16.6 µ m, IWC = 3.5 ppmv), and it is optically thinner (median extinction coefficient Ext = ∼ 0.056 km -1) than the cirrus mixture of contrail cirrus, natural in situ-origin and liquid-origin cirrus found around the CA range (median: Nice=0.038 cm -3 , Rice=24.1 µ m, IWC = 8.3 ppmv, Ext = ∼ 0.096 km -1). The lowest and thickest cirrus, consisting of a few large ice particles, are identified as pure natural liquid-origin cirrus (median: Nice=0.018 cm -3 , Rice=42.4 µ m, IWC = 21.7 ppmv, Ext = ∼ 0.137 km -1). Furthermore, we observe that, in particular, contrail cirrus occurs more often in slightly ice-subsaturated instead of merely ice-saturated to supersaturated air as often assumed, thus indicating the possibility of enlarged contrail cirrus existence regions. The enlargement is estimated, based on IAGOS long-term observations of relative humidity with respect to ice (RH ice) aboard passenger aircraft, to be approximately 10 % for Europe and the North Atlantic region, with the RH ice threshold for contrail cirrus existence decreased from 100 % to 90 % RH ice and a 4 h lifetime of contrail cirrus in slight ice subsaturation assumed. This increase may not only lead to a non-negligible change in contrail cirrus coverage and radiative forcing, but also affect the mitigation strategies of reducing contrails by rerouting flights. [ABSTRACT FROM AUTHOR]

Contrail cirrus constitute the largest radiative forcing (RF) component to the total aviation effect on climate. However, the microphysical properties and radiative effects of contrail cirrus and natural cirrus clouds in the same meteorological conditions are still not completely resolved. Motivated by these uncertainties, we investigate an extended cirrus region perturbed by aviation in the North Atlantic region (NAR) on 26 March 2014 during the Midlatitude Cirrus (ML-CIRRUS) experiment. On that day, high air traffic density in the NAR combined with large scale cold and humid ambient conditions favored the formation of a contrail cirrus outbreak situation. In addition, low coverage by low-level water clouds and the homogeneous oceanic albedo increased the sensitivity for retrieving cirrus properties and their radiative effect from satellite remote sensing. This allowed us to extend the current knowledge on contrail cirrus by combining airborne in situ, lidar and satellite observations. In the synoptic context of a ridge cirrus, an extended thin ice cloud with many persistent contrails and contrail cirrus has been observed for many hours with the geostationary Meteosat Second Generation (MSG)/Spinning Enhanced Visible and InfraRed Imager (SEVIRI) from the early morning hours until dissipation after noon. Airborne lidar observations aboard the German High Altitude and LOng Range Research Aircraft (HALO) suggest that this cirrus has a significant anthropogenic contribution from aviation. A new method based on in situ measurements was used to distinguish between contrails, contrail cirrus and natural cirrus based on ice number and gas phase NO concentrations. Results show that contrail effective radii (Reff) reach at most 11 µ m, while contrail cirrus Reff can be as large as 51 µ m. Contrail and contrail cirrus mean Reff is 18 % smaller than that of natural cirrus. We find that a difference in Reff between contrail cirrus and natural cirrus survives in this contrail cirrus outbreak event. As for radiative effects, a new method to estimate top-of-atmosphere instantaneous RF in the solar and thermal range is developed based on radiative transfer model simulations exploiting in situ and lidar measurements, satellite observations and ERA5 reanalysis data for both cirrus and cirrus-free regions. Broadband irradiances estimated from our simulations compare well with satellite observations from MSG, indicating that our method provides a good representation of the real atmosphere and can thus be used to determine the RF of ice clouds. For a larger spatial area around the flight path, we find that the contrail cirrus outbreak is warming in the early morning and cooling during the day. The methods presented here and the results will be valuable for future research to constrain uncertainties in the assessment of radiative impacts of contrail cirrus and natural cirrus and for the formulation and evaluation of contrail mitigation options. [ABSTRACT FROM AUTHOR]

Atmospheric aerosol particles play a key role in air pollution, health, and climate. Particles from biomass burning emissions are an important source of ambient aerosols, have increased over the past few decades, and are projected to further surge in the future as a result of climate and land use changes. Largely as a result of the variety of organic fuel materials and combustion types, particles emitted from biomass burning are often complex mixtures of inorganic and organic materials, with soot, ash, and charcoal having previously been identified as main particle types being emitted. Despite their importance for climate, their ice nucleation activities remain insufficiently understood, in particular for charcoal particles, whose ice nucleation activity has not been reported. Here, we present experiments of the ice nucleation activities of 400 nm size-selected charcoal particles, derived from the pyrolysis of two different biomass fuels, namely a grass charcoal and a wood charcoal. We find that the pyrolysis-derived charcoal types investigated do not contribute to ice formation via immersion freezing in mixed-phase cloud conditions. However, our results reveal considerable heterogeneous ice nucleation activity of both charcoal types at cirrus temperatures. An inspection of the ice nucleation results together with dynamic vapor sorption measurements indicates that cirrus ice formation proceeds via pore condensation and freezing. We find wood charcoal to be more ice-active than grass charcoal at cirrus temperatures. We attribute this to the enhanced porosity and water uptake capacity of the wood compared to the grass charcoal. In support of the results, we found a positive correlation of the ice nucleation activity of the wood charcoal particles and their chemical composition, specifically the presence of (inorganic) mineral components, based on single-particle mass spectrometry measurements. Even though correlational in nature, our results corroborate recent findings that ice-active minerals could largely govern the aerosol–cloud interactions of particles emitted from biomass burning emissions. [ABSTRACT FROM AUTHOR]

Aerosols affect cirrus formation and evolution, yet quantification of these effects remain difficult based on in situ observations due to the complexity of nucleation mechanisms and large variabilities in ice microphysical properties. This work employed a method to distinguish five evolution phases of cirrus clouds based on in situ aircraft-based observations from seven U.S. National Science Foundation (NSF) and five NASA flight campaigns. Both homogeneous and heterogeneous nucleation were captured in the 1 Hz aircraft observations, inferred from the distributions of relative humidity in the nucleation phase. Using linear regressions to quantify the correlations between cirrus microphysical properties and aerosol number concentrations, we found that ice water content (IWC) and ice crystal number concentration (Ni) show strong positive correlations with larger aerosols (>500 nm) in the nucleation phase, indicating strong contributions of heterogeneous nucleation when ice crystals first start to nucleate. For the later growth phase, IWC and Ni show similar positive correlations with larger and smaller (i.e., >100 nm) aerosols, possibly due to fewer remaining ice-nucleating particles in the later growth phase that allows more homogeneous nucleation to occur. Both 200 m and 100 km observations were compared with the nudged simulations from the National Center for Atmospheric Research (NCAR) Community Atmosphere Model version 6 (CAM6). Simulated aerosol indirect effects are weaker than the observations for both larger and smaller aerosols for in situ cirrus, while the simulated aerosol indirect effects are closer to observations in convective cirrus. The results also indicate that simulations overestimate homogeneous freezing, underestimate heterogeneous nucleation and underestimate the continuous formation and growth of ice crystals as cirrus clouds evolve. Observations show positive correlations of IWC, Ni and ice crystal mean diameter (Di) with respect to Na in both the Northern and Southern Hemisphere (NH and SH), while the simulations show negative correlations in the SH. The observations also show higher increases of IWC and Ni in the SH under the same increase of Na than those shown in the NH, indicating higher sensitivity of cirrus microphysical properties to increases of Na in the SH than the NH. The simulations underestimate IWC by a factor of 3–30 in the early/later growth phase, indicating that the low bias of simulated IWC was due to insufficient continuous ice particle formation and growth. Such a hypothesis is consistent with the model biases of lower frequencies of ice supersaturation and lower vertical velocity standard deviation in the early/later growth phases. Overall, these findings show that aircraft observations can capture both heterogeneous and homogeneous nucleation, and their contributions vary as cirrus clouds evolve. Future model development is also recommended to evaluate and improve the representation of water vapor and vertical velocity on the sub-grid scale to resolve the insufficient ice particle formation and growth after the initial nucleation event. [ABSTRACT FROM AUTHOR]

Diurnal variations in cloud cover and cloud vertical distribution are of great importance to Earth–atmosphere system radiative budgets and climate change. However, thus far these topics have received insufficient attention, especially on the Tibetan Plateau (TP). This study focuses on the diurnal variations in total cloud cover, cloud vertical distribution, and cirrus clouds and their relationship to meteorological factors over the TP based on active and passive satellite observations, reanalysis data, and CMIP6 outputs. Our results are consistent with previous studies but provide new insights. The results show that total cloud cover peaks at 06:00–09:00 UTC, especially over the eastern TP, but the spatial and temporal distributions of clouds from different datasets are inconsistent. This could to some extent be attributed to subvisible clouds missed by passive satellites and models. Compared with satellite observations, the amplitudes of the diurnal variations in total cloud cover obtained by the reanalysis and CMIP6 models are obviously smaller. CATS can capture the varying pattern of the vertical distribution of clouds and corresponding height of peak cloud cover at middle and high atmosphere levels, although it underestimates the cloud cover of low-level clouds, especially over the southern TP. Compared with CATS, ERA5 cannot capture the complete diurnal variations in vertical distribution of clouds and MERRA-2 has a poorer performance. We further find that cirrus clouds, which are widespread over the TP, show significant diurnal variations with averaged peak cloud cover over 0.35 at 15:00 UTC. Unlike in the tropics, where thin cirrus (0.03< optical depth <0.3) dominate, opaque cirrus clouds (0.3< optical depth <3) are the dominant cirrus clouds over the TP. The seasonal and regional averaged cloud cover of opaque cirrus reaches a daily maximum of 0.18 at 11:00 UTC, and its diurnal cycle is strong positive correlation with that of 250 hPa relative humidity and 250 hPa vertical velocity. Although subvisible clouds (optical depth <0.03), which have a potential impact on the radiation budget, are the fewest among cirrus clouds over the TP, the seasonal and regional averaged peak cloud cover can reach 0.09 at 22:00 UTC, and their diurnal cycle correlates with that of the 250 hPa relative humidity, 2 m temperature, and 250 hPa vertical velocity. Our results will be helpful to improve the simulation and retrieval of total cloud cover and cloud vertical distribution and further provide an observational constraint for simulations of the diurnal cycle of surface radiation budget and precipitation over the TP region. [ABSTRACT FROM AUTHOR]

The radiative energy budget in the Arctic undergoes a rapid transformation compared with global mean changes. Understanding the role of cirrus clouds in this system is vital, as they interact with short- and long-wave radiation, and the presence of cirrus can be decisive as to a net gain or loss of radiative energy in the polar atmosphere. In an effort to derive the radiative properties of cirrus in a real scenario in this sensitive region, we use in situ measurements of the ice water content (IWC) performed during the Polar Stratosphere in a Changing Climate (POLSTRACC) aircraft campaign in the boreal winter and spring 2015–2016 employing the German High Altitude and Long Range Research Aircraft (HALO). A large dataset of IWC measurements of mostly thin cirrus at high northern latitudes was collected in the upper troposphere and also frequently in the lowermost stratosphere. From this dataset, we select vertical profiles that sampled the complete vertical extent of cirrus cloud layers. These profiles exhibit a vertical IWC structure that will be shown to control the instantaneous radiative effect in both the long and short wavelength regimes in the polar winter. We perform radiative transfer calculations with the uvspec model from the libRadtran software package in a one-dimensional column between the surface and the top of the atmosphere (TOA), using the IWC profiles as well as the state of the atmospheric column at the time of measurement, as given by weather forecast products, as input. In parameter studies, we vary the surface albedo and solar zenith angle in ranges typical of the Arctic region. We find the strongest (positive) radiative forcing up to about 48Wm-2 for cirrus over bright snow, whereas the forcing is mostly weaker and even ambiguous, with a rather symmetric range of values down to -35Wm-2 , over the open ocean in winter and spring. The IWC structure over several kilometres in the vertical affects the irradiance at the TOA via the distribution of optical thickness. We show the extent to which IWC profiles with a coarser vertical resolution can reflect this effect. Further, a highly variable heating rate profile within the cloud is found which drives dynamical processes and contributes to the thermal stratification at the tropopause. Our case studies highlight the importance of a detailed resolution of cirrus clouds and the consideration of surface albedo for estimations of the radiative energy budget in the Arctic. [ABSTRACT FROM AUTHOR]

Linear contrails and contrail cirrus induced by global aviation have long been known to contribute to climate change by warming the atmosphere. Besides increasing global cirrus cloudiness, aviation may also alter the properties of natural cirrus clouds by soot emissions which lead to more heterogeneous freezing. During the first COVID-19 lockdown in Europe, changes in the properties and occurrence of cirrus clouds were determined with the lidar measurements of CALIPSO, which are presumed to be caused by the corresponding reduction in civil aviation. In the 10 years before the COVID-19 outbreak, however, aviation grew strongly in terms of CO 2 emissions and flight densities in Europe. In this study, 10-year lidar measurements with CALIPSO are analysed to determine the seasonality and long-term trends in cirrus clouds as well as their correlations with the ambient temperatures and air traffic. The results show that there is a distinct seasonal cycle in the occurrence rates (ORs) and particle linear depolarization ratio (PLDR) of cirrus clouds. In addition, cirrus clouds appear within a broader altitude range in winter than in summer and they are characterized by larger OR and PLDR values in winter than in summer. The monthly medians of PLDR as well as their deseasonalized time series in the 10-year period before COVID-19 both show positive trends, which are statistically significant according to the Mann–Kendall (MK) significance test. However, the ORs of cirrus clouds show a negative trend, which might be connected with the background meteorological conditions. Since the cirrus PLDR strongly depends on the ambient temperatures, the contributions induced by temperature are further removed from the cirrus PLDR with a simple linear regression model. The derived residuals show significant positive trends according to the MK test. To compare the cirrus PLDR and air traffic (with the CO 2 emissions from aviation as a proxy), the deseasonalization of both datasets were previously conducted since the seasonal cycles in both are not consistent. The deseasonalized time series determined for the cirrus PLDR and CO 2 emissions from aviation both show increasing trends and their correlation coefficient is r=0.54 at the confidence level above 99.5 %. Finally, comparisons between the cirrus PLDR and aviation in every season were made and revealed a strong correlation in other seasons than in summer. [ABSTRACT FROM AUTHOR]

Atmospheric aerosols can act as ice-nucleating particles (INPs), thereby influencing the formation and the microphysical properties of cirrus clouds, resulting in distinct climate effects. In addition to mineral dust and soot particles, laboratory experiments suggest crystalline ammonium sulfate and glassy organic particles as effective INPs in the cirrus regime. However, the impact of these new particle types at the global scale is still highly uncertain. Here, we present and analyse a global climatology of INPs derived from model simulations performed with a global aerosol–climate model coupled to a two-moment cloud microphysical scheme and a parametrization for aerosol-induced ice formation in cirrus clouds. This global INP climatology comprises mineral dust and soot particles as well as crystalline ammonium sulfate and glassy organics, including a simplified formulation of the particle phase state for the latter. By coupling the different INP types to the microphysical cirrus cloud scheme, their ice nucleation potential under cirrus conditions is analysed, considering possible competition mechanisms between different INPs. The simulated INP concentrations in the range of about 1 to 100 L -1 agree well with in situ observations and other global model studies. We show that INP concentrations of glassy organics and crystalline ammonium sulfate are strongly related to the ambient conditions which often inhibit the glassy or crystalline phase respectively. Our model results suggest that glassy organic particles probably only have a minor influence, as INP concentrations are mostly low in the cirrus regime. On the other hand, crystalline ammonium sulfate often shows large INP concentrations, has the potential to influence ice nucleation in cirrus clouds, and should be taken into account in future model applications. [ABSTRACT FROM AUTHOR]

In this study, which is the third part of the HaloCam series after , we present a novel technique to retrieve quantitative information about ice crystal optical and microphysical properties using ground-based imaging observations of halo displays. Comparing HaloCam's calibrated RGB images of 22 and 46 ∘ halo observations against a lookup table of simulated radiances, this technique allows the retrieval of the sizes and shapes of randomly oriented crystals as well as the fraction of smooth and rough ice crystals for cirrus clouds. We analyzed 4400 HaloCam images between September 2015 and November 2016 showing a visible 22 ∘ halo. The optical properties of hexagonal 8-element aggregates of columns with a mean ice crystal effective radius of about 20 µ m and a mixture of 37 % smooth and 63 % rough crystals on average best match the HaloCam observations. Implemented on different sites, HaloCam in combination with the machine-learning-based halo detection algorithm HaloForest can provide a consistent dataset for climatological studies of ice crystal properties representing typical cirrus clouds. Representative ice crystal optical properties are required for remote sensing of cirrus clouds as well as climate modeling. Since ground-based passive imaging observations provide information about the forward scattering part of the ice crystal optical properties, the results of this work ideally complement the results of satellite-based and airborne studies. [ABSTRACT FROM AUTHOR]

Large amounts of dust aerosols are lifted to the upper troposphere every year and play a major role in cirrus formation by acting as efficient ice nuclei. However, the relative importance of heterogeneous nucleation and spontaneous homogenous nucleation in dust-related cirrus clouds is still not well evaluated globally. Here, based on spaceborne observations, we propose a method to identify two ice-nucleating regimes of dust-related cirrus clouds, i.e., (1) the sole presence of heterogeneous nucleation and (2) competition between heterogeneous and homogeneous nucleation, by characterizing the relationship between dust ice-nucleating particle concentrations (INPCs) calculated from the Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) using the POlarization LIdar PHOtometer Networking (POLIPHON) method and in-cloud ice crystal number concentration (ICNC) from the DARDAR (lidar–radar) dataset. Two typical cirrus cases over central China are shown as a demonstration. In the first case, the upper part (near the cloud top) of a series of cirrus clouds successfully realized the INPC–ICNC closure, meaning that solely heterogeneous nucleation takes place, while the lower part of cirrus clouds showed the possible competition between heterogeneous and homogeneous nucleation. In the second case, the ICNCs in the cirrus cloud dramatically exceeded the dust INPCs in the vicinity by more than an order of magnitude, revealing that besides dust-induced heterogeneous nucleation, homogeneous nucleation also participated in ice formation and produced additional ice crystals. The proposed identification method is anticipated to apply in the evaluation of the influence of upper-troposphere dust on global cirrus formation and the investigation of the potential positive role of cirrus cloud thinning in the offset of climate warming. [ABSTRACT FROM AUTHOR]

As the near-surface atmosphere over the Antarctic Plateau is cold and pristine, its physico-chemical conditions resemble to a certain extent those of the high troposphere where cirrus clouds form. In this paper, we carry out an observational analysis of two shallow fog clouds forming in situ at cirrus temperatures – that is, temperatures lower than 235 K – at Dome C, inner Antarctic Plateau. The combination of lidar profiles with temperature and humidity measurements from advanced thermo-hygrometers along a 45 m mast makes it possible to characterise the formation and development of the fog. High supersaturations with respect to ice are observed before the initiation of fog, and the values attained suggest that the nucleation process at play is the homogeneous freezing of solution aerosol droplets. This is the first time that in situ observations show that this nucleation pathway can be at the origin of an ice fog. Once nucleation occurs, the relative humidity gradually decreases down to subsaturated values with respect to ice in a few hours, owing to vapour deposition onto ice crystals and turbulent mixing. The development of fog is tightly coupled with the dynamics of the boundary layer which, in the first study case, experiences a weak diurnal cycle, while in the second case, it transits from a very stable to a weakly stable dynamical regime. Overall, this paper highlights the potential of the site of Dome C for carrying out observational studies of very cold cloud microphysical processes in natural conditions and using in situ ground-based instruments. [ABSTRACT FROM AUTHOR]

Satellite observations have revealed an enhanced aerosol layer near the tropopause over Asia during the summer monsoon, called the "Asian Tropopause Aerosol Layer" (ATAL). In this work, aerosol particles in the ATAL were collected with a balloon-borne impactor near the tropopause region over India, using extended-duration balloon flights, in summer 2017 and winter 2018. The chemical composition of these particles was further investigated by quantitative analysis using offline ion chromatography. Nitrate (NO 3-) and nitrite (NO 2-) were found to be the dominant ions in the collected aerosols with values ranging between 87 and 343 ng m -3 at STP (standard temperature and pressure) during the summer campaign. In contrast, sulfate (SO 42-) levels were found to be above the detection limit (>10 ng m -3 at STP) only in winter. In addition, we determined the origin of the air masses sampled during the flights using the analysis of back trajectories as well as a convective proxy from cloud-top temperature fields derived from a geostationary satellite. The results obtained from this analysis were put into the context of large-scale transport and aerosol distribution using GEOS-Chem chemical transport model simulations. The first flight in summer 2017 which sampled an air mass within the Asian monsoon anticyclone (AMA), influenced by convection over Western China, was associated with particle size diameters from 0.05 to 0.15 µ m. In contrast, the second flight sampled air masses at the edge of the AMA associated with a larger particle size radius (>2 µ m) with a higher NO 2- concentration. The sampled air masses in winter 2018 were likely affected by smoke from the Pacific Northwest fire event in Canada, which occurred 7 months before our campaign, associated with concentration enhancements of SO 42- and Ca 2+. Overall, our results suggest that nitrogen-containing particles represent a large fraction of cloud-free and in-cloud aerosols populating the ATAL, which is partially in agreement with the results from aircraft measurements during the StratoClim (Stratospheric and upper tropospheric processes for better climate predictions) campaign. The exact nature of those particles is still unknown, but their coincidences with subvisible cirrus clouds and their sizes suggest nitric acid trihydrate (NAT) as a possible candidate, as NAT has already been observed in the tropical upper troposphere and lower stratosphere in other studies. Furthermore, GEOS-Chem model simulations indicate that lightning NO x emissions could have significantly impacted the production of nitrate aerosols sampled during the summer of 2017. [ABSTRACT FROM AUTHOR]

Cirrus cloud thinning (CCT) is a relatively new radiation management proposal to counteract anthropogenic climate warming by targeting Earth's terrestrial radiation balance. The efficacy of this method was presented in several general circulation model (GCM) studies that showed widely varied radiative responses, originating in part from the differences in the representation of cirrus ice microphysics between the different GCMs. The recent implementation of a new, more physically based ice microphysics scheme (Predicted Particle Properties, P3) that abandons ice hydrometeor size class separation into the ECHAM-HAM GCM, coupled to a new approach for calculating cloud fractions that increases the relative humidity (RH) thresholds for cirrus cloud formation, motivated a reassessment of CCT efficacy. In this study, we first compared CCT sensitivity between the new cloud fraction approach and the original ECHAM-HAM cloud fraction approach. Consistent with previous approaches using ECHAM-HAM, with the P3 scheme and the higher RH thresholds for cirrus cloud formation, we do not find a significant cooling response in any of our simulations. The most notable response from our extreme case is the reduction in the maximum global-mean net top-of-atmosphere (TOA) radiative anomalies from overseeding by about 50 %, from 9.9 W m -2 with the original cloud fraction approach down to 4.9 W m -2 using the new cloud fraction RH thresholds that allow partial grid-box coverage of cirrus clouds above ice saturation, unlike the original approach. Even with this reduction with the updated cloud fraction approach, the TOA anomalies from overseeding far exceed those reported in previous studies. We attribute the large positive TOA anomalies to seeding particles overtaking both homogeneous nucleation and heterogeneous nucleation on mineral dust particles within cirrus clouds to produce more numerous and smaller ice crystals. This effect is amplified by longer ice residence times in clouds due to the slower removal of ice via sedimentation in the P3 scheme. In an effort to avoid this overtaking effect of seeding particles, we increased the default critical ice saturation ratio (Si,seed) for ice nucleation on seeding particles from the default value of 1.05 to 1.35 in a second sensitivity test. With the higher Si,seed we drastically reduce overseeding, which suggests that Si,seed is a key factor to consider for future CCT studies. However, the global-mean TOA anomalies contain high uncertainty. In response, we examined the TOA anomalies regionally and found that specific regions only show a small potential for targeted CCT, which is partially enhanced by using the larger Si,seed. Finally, in a seasonal analysis of TOA responses to CCT, we find that our results do not confirm the previous finding that high-latitude wintertime seeding is a feasible strategy to enhance CCT efficacy, as seeding in our model enhances the already positive cirrus longwave cloud radiative effect for most of our simulations. Our results also show feedbacks on lower-lying mixed-phase and liquid clouds through the reduction in ice crystal sedimentation that reduces cloud droplet depletion and results in stronger cloud albedo effects. However, this is outweighed by stronger longwave trapping from cirrus clouds with more numerous and smaller ice crystals. Therefore, we conclude that CCT is unlikely to act as a feasible climate intervention strategy on a global scale. [ABSTRACT FROM AUTHOR]

The role of clouds in the surface radiation budget is particularly complex in the rapidly changing Arctic. However, despite their importance, long-term observations of Arctic clouds are relatively sparse. Here, we present observations of cold clouds based on 7 years (2011–2017) of ground-based lidar observations at the Arctic Lidar Observatory for Middle Atmosphere Research (ALOMAR) in Andenes in the Norwegian Arctic. In two case studies, we assess (1) the agreement between a co-located cirrus cloud observations from the ground-based lidar and the spaceborne lidar aboard the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite and (2) the ground-based lidar's capability to determine the cloud phase in mixed-phase clouds from depolarization measurements. We then compute multiyear statistics of cold clouds from both platforms with respect to their occurrence, cloud top and base height, cloud top temperature, and thermodynamic phase for the 2011–2017 period. We find that satellite- and ground-based observations agree well with respect to the coincident cirrus measurement and that the vertical phase distribution within a liquid-topped mixed-phase cloud could be identified from depolarization measurements. On average, 8 % of all satellite profiles were identified as single-layer cold clouds with no apparent seasonal differences. The average cloud top and base heights, combining the ground-based and satellite measurements, are 9.1 and 6.9 km, respectively, resulting in an average thickness of 2.2 km. Seasonal differences between the average top and base heights are on the order of 1–2 km and are largest when comparing fall (highest) and spring (lowest). However, seasonal variations are small compared with the observed day-to-day variability. Cloud top temperatures agree well between both platforms, with warmer cloud top temperatures in summer. The presented study demonstrates the capabilities of long-term cloud observations in the Norwegian Arctic from the ground-based lidar at Andenes. [ABSTRACT FROM AUTHOR]

The effective radiative forcing of anthropogenic aerosols (ERF aer) is an important measure of the anthropogenic aerosol effects simulated by a global climate model. Here we analyze ERF aer simulated by the E3SM version 1 (E3SMv1) atmospheric model using both century-long free-running atmosphere–land simulations and short nudged simulations. We relate the simulated ERF aer to characteristics of the aerosol composition and optical properties, and we evaluate the relationships between key aerosol and cloud properties. In terms of historical changes from the year 1870 to 2014, our results show that the global mean anthropogenic aerosol burden and optical depth increase during the simulation period as expected, but the regional averages show large differences in the temporal evolution. The largest regional differences are found in the emission-induced evolution of the burden and optical depth of the sulfate aerosol: a strong decreasing trend is seen in the Northern Hemisphere high-latitude region after around 1970, while a continued increase is simulated in the tropics. The relationships between key aerosol and cloud properties (relative changes between pre-industrial and present-day conditions) also show evident changes after 1970, diverging from the linear relationships exhibited for the period of 1870–1969. In addition to the regional differences in the simulated relationships, a reduced sensitivity in cloud droplet number and other cloud properties to aerosol perturbations is seen when the aerosol perturbation is large. Consequently, the global annual mean ERF aer magnitude does not increase after around 1970. The ERF aer in E3SMv1 is relatively large compared to the recently published multi-model estimates; the primary reason is the large indirect aerosol effect (i.e., through aerosol–cloud interactions). Compared to other models, E3SMv1 features large relative changes in the cloud droplet effective radius in response to aerosol perturbations. Large sensitivity is also seen in the liquid cloud optical depth, which is determined by changes in both the effective radius and liquid water path. Aerosol-induced changes in liquid and ice cloud properties in E3SMv1 are found to have a strong correlation, as the evolution of anthropogenic sulfate aerosols affects both the liquid cloud formation and the homogeneous ice nucleation in cirrus clouds (that causes a large effect on longwave ERF aer). As suggested by a previous study, the large ERF aer appears to be one of the reasons why the model cannot reproduce the observed global mean temperature evolution in the second half of the 20th century. Sensitivity simulations are performed to understand which parameterization and/or parameter changes have a large impact on the simulated ERF aer. The ERF aer estimates in E3SMv1 for the shortwave and longwave components are sensitive to the parameterization changes in both liquid and ice cloud processes. When the parameterization of ice cloud processes is modified, the top-of-model forcing changes in the shortwave and longwave components largely offset each other, so the net effect is negligible. This suggests that, to reduce the magnitude of the net ERF aer , it would be more effective to reduce the anthropogenic aerosol effect through liquid or mixed-phase clouds. [ABSTRACT FROM AUTHOR]

Contrail formation within natural cirrus introduces large perturbations in cirrus ice crystal number concentrations, leading to modifications in cirrus microphysical and optical properties. The number of contrail ice crystals formed in an aircraft plume depends on the atmospheric state as well as aircraft and fuel properties. Our aim is to study contrail formation within cirrus and, in particular, the impact of pre-existing cirrus on the contrail formation processes. We implement a parameterization for contrail ice nucleation and the survival of contrail ice crystals within the vortex phase within the high-resolution ICON-LEM at a horizontal resolution of 625 m over Germany and modify the parameterizations in order to consider the impact of the pre-existing cirrus. We then simulate contrail formation and analyze the change in ice nucleation and survival due to the presence of cirrus ice crystals. We have selected two different synoptic situations to sample a large range of cirrus cloud properties from those representative of average thick in situ formed cirrus and liquid origin cirrus that are connected to a frontal system down to very thin cirrus within a high-pressure system. We find that contrail formation within cirrus mostly leads to increases in cirrus ice crystal numbers by a few orders of magnitude. Pre-existing cirrus has a discernible impact on the contrail formation threshold temperature and on contrail ice crystal number concentrations only if the cirrus ice water content is high and ice supersaturation is low. The cirrus ice crystals sucked into and subsequently sublimated within the aircraft's engine and the ice crystals mixed into the aircraft plume experiencing sublimation and later deposition lead to an increase in the contrail formation threshold temperature most of the time. Often this increase is negligible, but in the above atmospheric conditions the increase in the contrail formation threshold can be large, reaching maximum values of 2 K. Consequently, significant increases in ice nucleation are very seldom, but in areas of high cirrus ice water content and ice crystal number concentrations, contrail ice nucleation rates can be significantly increased, in particular at lower flight levels. Cirrus ice crystals can also lead to a reduction in ice nucleation, but negative changes are significantly smaller and less common. After nucleation cirrus and contrail ice crystals compete for water vapor, while the combined contrail and cirrus ice water mass grows. Once the aircraft plume gets trapped within the wake vortices and descends the plume relative humidity decreases so that eventually both cirrus and contrail ice crystals sublimate. We find that the impact of cirrus ice crystals on the contrail ice crystal loss within the descending vortices is negligible. Only for nucleation rates several orders of magnitude lower than the soot number emission index can the impact be noticeable, but the relevance of this impact is limited. [ABSTRACT FROM AUTHOR]

Knowledge of the spatiotemporal coverage of cirrus clouds is vital in quantifying the radiation budget of the Earth–atmosphere system. In this paper, we present the diurnal and vertical distributions of the occurrence of cirrus clouds during different seasons as well as the interannual variation in the occurrence of cirrus over Kattankulathur (12.82 ∘ N, 80.04 ∘ E) on the west coast of the Bay of Bengal. Long-term (2016–2018) continuous micropulse lidar (MPL) observations demonstrate laminar and descending cirrus clouds that occur either as single or multiple layers. The single-layer cirrus occurrence shows a diurnal pattern with frequent occurrence in the late evening (∼ 30 %–40 %), whereas multilayer cirrus clouds occur in the early morning (∼ 10 %–20 %). For the diurnal pattern in single-layer cirrus cloud occurrences, convective processes dominate during the pre-monsoon, southwest (SW) monsoon, and northeast (NE) monsoon seasons, while the freeze-drying process is favorable during the winter season. However, both convective and freeze-drying processes are dominant in the diurnal pattern of the multilayer cirrus occurrences. The occurrence reaches a maximum (∼ 40 %) during the SW and NE monsoon seasons, and it shows a minimum (∼ 25 %) during the winter season. The vertical distributions indicate that the maximum occurrence is confined within the tropical tropopause layer (TTL) during all seasons. Cirrus cloud rarely occurs above the tropopause; however, it frequently occurs below the TTL during all seasons. The vertical extent of the occurrence has a broader altitudinal coverage (∼ 8–17 km) during December–March and June–September, while the altitudinal coverage is narrower during April–May (∼ 10–17 km) and October–November (∼ 9–15 km). Cirrus cloud occurrence also exhibits interannual variations, with higher occurrence during 2016 compared with 2017 and 2018, in association with the El Niño–Southern Oscillation (ENSO). [ABSTRACT FROM AUTHOR]

In this paper, the effects of ice-supersaturated regions and thin, subvisual cirrus clouds on lapse rates are examined. For that, probability distribution and density functions of the lapse rate and the potential temperature gradients from 10 years of measurement data from the MOZAIC/IAGOS project and ERA5 reanalysis data were produced, and an analysis of an example case of an ice-supersaturated region with a large vertical extent is performed. For the study of the probability distribution and density functions, a distinction is made between ice-subsaturated and ice-supersaturated air masses (persistent contrails) and situations of particularly high ice supersaturation that allow the formation of optically thick and strongly warming contrails. The estimation of the lapse rates involves two adjacent standard pressure levels of the reanalysis surrounding MOZAIC's measurement/flight points. If the upper of these levels is in the stratosphere, the distribution function for subsaturated cases shows much lower lapse rates than those of supersaturated cases. If all levels are in the troposphere, the distributions become more similar, but the average lapse rates are still higher in supersaturated than in subsaturated cases, and the distributions peak at higher values and are narrower in ice-supersaturated regions (ISSRs) than elsewhere. This narrowing is particularly pronounced if there is substantial supersaturation. For the examination of an example case, ERA5 data and forecasts from ICON-EU (DWD) are compared. ERA5 data, in particular, show a large ice-supersaturated region below the tropopause, which was pushed up by uplifting air, while the data of ICON-EU indicate areas of saturation. The lapse rate in this ice-supersaturated region (ISSR), which is large, is associated with clouds and high relative humidity. Supersaturation and cloud formation result from uplifting of air layers. The temperature gradient within an uplifting layer steepens, for both dry and moist air. As soon as condensation or ice formation starts in the upper part of a lifting layer, the release of latent heat begins to decrease the lapse rate, but radiation starts to act in the opposite direction, keeping the lapse rate high. The highest lapse rates close to the stability limit can only be reached in potentially unstable situations. [ABSTRACT FROM AUTHOR]

Formation of atmospheric ice plays a crucial role in the microphysical evolution of mixed-phase and cirrus clouds and thus climate. How aerosol particles impact ice crystal formation by acting as ice-nucleating particles (INPs) is a subject of intense research activities. To improve understanding of atmospheric INPs, we examined daytime and nighttime particles collected during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign conducted in summer 2017. Collected particles, representative of a remote marine environment, were investigated for their propensity to serve as INPs in the immersion freezing (IMF) and deposition ice nucleation (DIN) modes. The particle population was characterized by chemical imaging techniques such as computer-controlled scanning electron microscopy with energy-dispersive X-ray analysis (CCSEM/EDX) and scanning transmission X-ray microscopy with near-edge X-ray absorption fine-structure spectroscopy (STXM/NEXAFS). Four major particle-type classes were identified where internally mixed inorganic–organic particles make up the majority of the analyzed particles. Following ice nucleation experiments, individual INPs were identified and characterized by SEM/EDX. The identified INP types belong to the major particle-type classes consisting of fresh sea salt with organics or processed sea salt containing dust and sulfur with organics. Ice nucleation experiments show IMF events at temperatures as low as 231 K , including the subsaturated regime. DIN events were observed at lower temperatures of 210 to 231 K. IMF and DIN observations were analyzed with regard to activated INP fraction, ice-nucleation active site (INAS) densities, and a water activity-based immersion freezing model (ABIFM) yielding heterogeneous ice nucleation rate coefficients. Observed IMF and DIN events of ice formation and corresponding derived freezing rates demonstrate that the marine boundary layer aerosol particles can serve as INPs under typical mixed-phase and cirrus cloud conditions. The derived IMF and DIN parameterizations allow for implementation in cloud and climate models to evaluate predictive effects of atmospheric ice crystal formation. [ABSTRACT FROM AUTHOR]

Soot particles are potential candidates for ice-nucleating particles in cirrus cloud formation, which is known to exert a net-warming effect on climate. Bare soot particles, generally hydrophobic and fractal ones, mainly exist near emission sources. Coated or internally mixed soot particles are more abundant in the atmosphere and have a higher probability of impacting cloud formation and climate. However, the ice nucleation ability of coated soot particles is not as well understood as that of freshly produced soot particles. In this laboratory study, two samples, a propane flame soot and a commercial carbon black, were used as atmospheric soot surrogates and coated with varying wt % of sulfuric acid (H 2 SO 4). The ratio of coating material mass to the mass of bare soot particles was controlled and progressively increased from less than 5 wt % to over 100 wt %. Both bare and coated soot particle ice nucleation activities were investigated with a continuous-flow diffusion chamber operated at mixed-phase and cirrus cloud conditions. The mobility diameter and mass distribution of size-selected soot particles with/without H 2 SO 4 coating were measured by a scanning mobility particle sizer and a centrifugal particle mass analyser running in parallel. The mixing state and morphology of soot particles were characterized by scanning electron microscopy and transmission electron microscopy. In addition, the evidence of the presence of H 2 SO 4 on a coated soot particle surface is shown by energy-dispersive X-ray spectroscopy. Our study demonstrates that H 2 SO 4 coatings suppress the ice nucleation activity of soot particles to varying degrees depending on the coating thickness, but in a non-linear fashion. Thin coatings causing pore filling in the soot aggregate inhibits pore condensation and freezing. Thick coatings promote particle ice activation via droplet homogeneous freezing. Overall, our findings reveal that H 2 SO 4 coatings will suppress soot particle ice nucleation abilities in the cirrus cloud regime, having implications for the fate of soot particles with respect to cloud formation in the upper troposphere. [ABSTRACT FROM AUTHOR]

Soot particles, acting as ice nucleating particles (INPs), can contribute to cirrus cloud formation, which has an important influence on climate. Aviation activities emitting soot particles into the upper troposphere can potentially impact ice nucleation (IN) in cirrus clouds. Pore condensation and freezing (PCF) is an important ice formation pathway for soot particles in the cirrus regime, which requires the soot INP to have specific morphological properties, i.e., mesopore structures. In this study, the morphology and pore size distribution of two kinds of soot samples were modified by a physical agitation method without any chemical modification by which more compacted soot sample aggregates could be produced compared to the unmodified sample. The IN activities of both fresh and compacted soot particles with different sizes, 60, 100, 200 and 400 nm, were systematically tested by the Horizontal Ice Nucleation Chamber (HINC) under mixed-phase and cirrus-cloud-relevant temperatures (T). Our results show that soot particles are unable to form ice crystals at T>235 K (homogeneous nucleation temperature, HNT), but IN is observed for compacted and larger-sized soot aggregates (>200 nm) well below the homogeneous freezing relative humidity (RH hom) for T< HNT, demonstrating PCF as the dominating mechanism for soot IN. We also observed that mechanically compacted soot particles can reach a higher particle activation fraction (AF) value for the same T and RH condition compared to the same aggregate size fresh soot particles. The results also reveal a clear size dependence for the IN activity of soot particles with the same degree of compaction, showing that compacted soot particles with large sizes (200 and 400 nm) are more active INPs and can convey the single importance of soot aggregate morphology for the IN ability. In order to understand the role of soot aggregate morphology for its IN activity, both fresh and compacted soot samples were characterized systematically using particle mass and size measurements, comparisons from TEM (transmission electron microscopy) images, soot porosity characteristics from argon (Ar) and nitrogen (N 2) physisorption measurements, as well as soot–water interaction results from DVS (dynamic vapor sorption) measurements. Considering the soot particle physical properties along with its IN activities, the enhanced IN abilities of compacted soot particles are attributed to decreasing mesopore width and increasing mesopore occurrence probability due to the compaction process. [ABSTRACT FROM AUTHOR]

Laboratory measurements at the AIDA cloud chamber and airborne in situ observations suggest that the homogeneous freezing thresholds at low temperatures are possibly higher than expected from the so-called "Koop line". This finding is of importance, because the ice onset relative humidity affects the cirrus cloud coverage and, at the very low temperatures of the tropical tropopause layer, together with the number of ice crystals also the transport of water vapor into the stratosphere. Both the appearance of cirrus clouds and the amount of stratospheric water feed back to the radiative budget of the atmosphere. In order to explore the enhanced ice onset humidities, we re-examine the entire homogeneous ice nucleation process, ice onset, and nucleated crystal numbers, by means of a two-moment microphysics scheme embedded in the trajectory-based model (CLaMS-Ice) as follows: the well-understood and described theoretical framework of homogeneous ice nucleation includes certain formulations of the water activity of the freezing aerosol particles and the saturation vapor pressure of water with respect to liquid water. However, different formulations are available for both parameters. Here, we present extensive sensitivity simulations testing the influence of three different formulations for the water activity and four for the water saturation on homogeneous ice nucleation. We found that the number of nucleated ice crystals is almost independent of these formulations but is instead sensitive to the size distribution of the freezing aerosol particles. The ice onset humidities, also depending on the particle size, are however significantly affected by the choices of the water activity and water saturation, in particular at cold temperatures ≲205 K. From the CLaMS-Ice sensitivity simulations, we here provide combinations of water saturation and water activity formulations suitable to reproduce the new, enhanced freezing line. [ABSTRACT FROM AUTHOR]

A global aerosol–climate model, including a two-moment cloud microphysical scheme and a parametrization for aerosol-induced ice formation in cirrus clouds, is applied in order to quantify the impact of aviation soot on natural cirrus clouds. Several sensitivity experiments are performed to assess the uncertainties in this effect related to (i) the assumptions on the ice nucleation abilities of aviation soot, (ii) the representation of vertical updrafts in the model, and (iii) the use of reanalysis data to relax the model dynamics (the so-called nudging technique). Based on the results of the model simulations, a radiative forcing from the aviation soot–cirrus effect in the range of -35 to 13 mW m -2 is quantified, depending on the assumed critical saturation ratio for ice nucleation and active fraction of aviation soot but with a confidence level below 95 % in several cases. Simple idealized experiments with prescribed vertical velocities further show that the uncertainties on this aspect of the model dynamics are critical for the investigated effect and could potentially add a factor of about 2 of further uncertainty to the model estimates of the resulting radiative forcing. The use of the nudging technique to relax model dynamics is proved essential in order to identify a statistically significant signal from the model internal variability, while simulations performed in free-running mode and with prescribed sea-surface temperatures and sea-ice concentrations are shown to be unable to provide robust estimates of the investigated effect. A comparison with analogous model studies on the aviation soot–cirrus effect show a very large model diversity, with a conspicuous lack of consensus across the various estimates, which points to the need for more in-depth analyses on the roots of such discrepancies. [ABSTRACT FROM AUTHOR]

The tropical tropopause layer (TTL) is the transition layer between the troposphere and the stratosphere. Tropical cyclones may impact the TTL by perturbing the vertical distributions of cloud, temperature, and water vapor. This study combines several A-Train instruments, including radar from CloudSat, lidar from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite, and the Atmospheric Infrared Sounder (AIRS) on the Aqua satellite, to detect signatures of cyclone impacts on the distribution patterns of cloud, water vapor, temperature, and radiation by compositing these thermodynamic fields relative to the cyclone center location. Based on the CloudSat 2B-CLDCLASS-LIDAR product, this study finds that tropical cyclone events considerably increase the occurrence frequencies of TTL clouds, in the form of cirrus clouds above a clear troposphere. The amount of TTL cloud ice, however, is found to be mostly contributed by overshooting deep convection that penetrates the base of the TTL at 16 km. To overcome the lack of temperature and water vapor products in cloudy conditions, this study implements a synergistic method that retrieves temperature, water vapor, ice water content, and effective radius simultaneously by incorporating observations from AIRS, CloudSat, and CALIPSO. Using the synergistic method, we find a vertically oscillating pattern of temperature anomalies above tropical cyclones, with warming beneath the cloud top (around 16 km) and cooling above. Based on water vapor profiles retrieved by the synergistic method, we find that the layer integrated water vapor (LIWV) above 16 km is higher above tropical cyclones, especially above overshooting deep convective clouds, compared to climatological values. Moreover, we find that the longwave and net radiative cooling effect of clouds prevails within 1000 km of tropical cyclone centers. The radiative heating effects of clouds from the CloudSat 2B-FLXHR-LIDAR product are well differentiated by the collocated brightness temperature of an infrared window channel from the collocated AIRS L1B product. By performing instantaneous radiative heating rate calculations, we further find that TTL hydration is usually associated with radiative cooling of the TTL, which inhibits the diabatic ascent of moist air across isentropic surfaces to the stratosphere. Therefore, the radiative balance of the TTL under the impact of the cyclone does not favor the maintenance of moist anomalies in the TTL or transporting water vertically to the stratosphere. [ABSTRACT FROM AUTHOR]

By inducing linear contrails and contrail cirrus, air traffic has a main impact on the ice cloud coverage and occurrence. During the COVID-19 pandemic, civil air traffic over Europe was significantly reduced, in March and April 2020, to about 80 % compared to the year before. This unique situation allows us to study the effect of air traffic on cirrus clouds. This work investigates, based on satellite lidar measurements, if and how cirrus cloud properties and occurrence changed over Europe in the course of COVID-19. Cirrus cloud properties are analyzed for different years between 2014 and 2019, which showed similar meteorological conditions for the month of April as in 2020. The meteorological conditions for March, however, were warmer and drier in 2020 than the previous years. The average thickness of cirrus clouds was reduced to 1.18 km in March 2020 compared to a value of 1.40 km under normal conditions, which is stronger than expected from the aviation reduction due to the less favorable meteorology for ice cloud formation. While the April results in 2020 were only slightly reduced, with an average thickness of 70 m thinner than the composite mean of the previous 6 years. Comparing the different years shows that the cirrus cloud occurrence was reduced by about 17 %–30 %, with smaller cloud thicknesses found in 2020 for both months. In addition, the cirrus clouds measured in 2020 possess smaller values of the particle linear depolarization ratio (PLDR) than the previous years at a high significance level for both months, especially at colder temperatures (T<-50 ∘ C). The same analyses are extended to the observations over the USA and China. Besides the regional discrimination of cirrus clouds, we reach the final conclusion that cirrus clouds show significant changes in PLDR in both March and April over Europe, no changes in both months over China, and significant changes only in April over the USA. [ABSTRACT FROM AUTHOR]

An advanced multiwavelength polarization Raman lidar was operated aboard the icebreaker Polarstern during the MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition to continuously monitor aerosol and cloud layers in the central Arctic up to 30 km height. The expedition lasted from September 2019 to October 2020 and measurements were mostly taken between 85 and 88.5 ∘ N. The lidar was integrated into a complex remote-sensing infrastructure aboard the Polarstern. In this article, novel lidar techniques, innovative concepts to study aerosol–cloud interaction in the Arctic, and unique MOSAiC findings will be presented. The highlight of the lidar measurements was the detection of a 10 km deep wildfire smoke layer over the North Pole region between 7–8 km and 17–18 km height with an aerosol optical thickness (AOT) at 532 nm of around 0.1 (in October–November 2019) and 0.05 from December to March. The dual-wavelength Raman lidar technique allowed us to unambiguously identify smoke as the dominating aerosol type in the aerosol layer in the upper troposphere and lower stratosphere (UTLS). An additional contribution to the 532 nm AOT by volcanic sulfate aerosol (Raikoke eruption) was estimated to always be lower than 15 %. The optical and microphysical properties of the UTLS smoke layer are presented in an accompanying paper. This smoke event offered the unique opportunity to study the influence of organic aerosol particles (serving as ice-nucleating particles, INPs) on cirrus formation in the upper troposphere. An example of a closure study is presented to explain our concept of investigating aerosol–cloud interaction in this field. The smoke particles were obviously able to control the evolution of the cirrus system and caused low ice crystal number concentration. After the discussion of two typical Arctic haze events, we present a case study of the evolution of a long-lasting mixed-phase cloud layer embedded in Arctic haze in the free troposphere. The recently introduced dual-field-of-view polarization lidar technique was applied, for the first time, to mixed-phase cloud observations in order to determine the microphysical properties of the water droplets. The mixed-phase cloud closure experiment (based on combined lidar and radar observations) indicated that the observed aerosol levels controlled the number concentrations of nucleated droplets and ice crystals. [ABSTRACT FROM AUTHOR]