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Atmospheric aerosol particles have a profound impact on Earth's climate by scattering and absorbing solar and terrestrial radiation and by impacting the properties of clouds. Research aircraft such as the Deutsches Zentrum für Luft- und Raumfahrt e.V. (DLR) Falcon are widely used to study aerosol particles in the troposphere and lower stratosphere. However, transporting a representative sample to the instrumentation inside the aircraft remains a challenge due to high airspeeds and changing ambient conditions. In particular, for high-quality coarse-mode aerosol measurements, knowledge about losses or enhancements in the aerosol sampling system is crucial. In this study, the sampling efficiency of the aerosol inlet aboard the Falcon research aircraft is characterized for the first time with state-of-the art in situ measurements including sizing instruments operated behind the Falcon aerosol inlet and mounted at the aircraft wing not affected by the aerosol inlet. Sampling efficiencies were derived for different true airspeed ranges by comparing the in-cabin and "full"-size-range particle number size distributions during 174 flight sequences with a major contribution of mineral dust particles during the "Absorbing aerosol layers in a changing climate: aging, lifetime and dynamics" project (A-LIFE). Additionally, experimentally derived Stokes numbers were used to calculate the cutoff diameter of the aerosol sampling system for different particle densities as a function of true airspeed. As expected, the results show that the velocity of the research aircraft has a major impact on the sampling of coarse-mode aerosol particles with in-cabin instruments. For true airspeeds up to about 190 ms-1 , aerosol particles larger than about 1 µm are depleted in the sampling system of the Falcon during the A-LIFE project. In contrast, for true airspeeds higher than 190 ms-1 , an enhancement of particles up to a diameter of 4 µm is observed. For even larger particles, the enhancement effect at the inlet is still present, but inertial and gravitational particle losses in the transport system get more and more pronounced, which leads to a decreasing overall sampling efficiency. In summary, aerosol particles are either depleted or enhanced in the Falcon aerosol inlet, whereas transport in sampling lines always leads to a loss of particles. Here, we have considered both effects and determined the cutoff diameter for the A-LIFE transport system (i.e., the sampling lines only), the cutoff diameter of the Falcon aerosol inlet (i.e., the effect of the inlet only), and the combined effect of the inlet and sampling lines. [ABSTRACT FROM AUTHOR]

Atmospheric aerosol particles have a profound impact on Earth's climate by scattering and absorbing solar and terrestrial radiation and by impacting the properties of clouds. Research aircraft such as the Deutsches Zentrum für Luft-und Raumfahrt e.V. (DLR) Falcon are widely used to study aerosol particles in the troposphere and lower stratosphere. However, transporting representative sample to the instrumentation inside the aircraft remains a challenge due to high airspeeds and changing ambient conditions. In particular, for high-quality coarse mode aerosol measurements, knowledge about losses or enhancements in the aerosol sampling system is crucial. In this study, we present a detailed characterization of the Falcon aerosol sampling system. Aerosol number size distributions were measured during the A-LIFE field campaign simultaneously with in-cabin and out-cabin/wing-mounted instrumentation. Sampling efficiencies were derived for different true airspeed ranges by comparing the in-cabin and the out-cabin particle number size distributions during flight sequences with a major contribution of mineral dust particles in the coarse mode size range. Additionally, experimentally derived Stokes numbers were used to calculate the cut-off diameter of the A-LIFE aerosol sampling system for different particle densities as a function of true airspeed. The results show that the velocity of the research aircraft has a major impact on the sampling of coarse mode aerosol particles with in-cabin instruments. For true airspeeds up to about 190 m s-1, aerosol particles larger than about 1 µm are depleted in the sampling system of the Falcon during the A-LIFE project. In contrast, for true airspeeds higher than 190 m 1, an enhancement of particles up to a diameter of 4 µm is observed. For even larger particles, the enhancement effect at the inlet is still present, but inertial and gravitational particle losses in the transport system get more and more pronounced which leads to a decreasing overall sampling efficiency. In summary, aerosol particles can either be depleted or enhanced at an aerosol inlet, whereas transport in sampling lines always leads to a loss of particles. Therefore, it is important to consider both, inlet and transport efficiency, when quantifying the sampling efficiency of an aerosol sampling system. [ABSTRACT FROM AUTHOR]

Aerosols and clouds affect atmospheric radiative processes and climate in many complex ways and still pose the largest uncertainty in current estimates of the Earth's changing energy budget. Airborne in situ sensors such as the Cloud, Aerosol, and Precipitation Spectrometer (CAPS) or other optical spectrometers and optical array probes provide detailed information about the horizontal and vertical distribution of aerosol and cloud properties. However, flow distortions occurring at the location where these instruments are mounted on the outside of an aircraft may directly produce artifacts in detected particle number concentration and also cause droplet deformation and/or breakup during the measurement process. Several studies have investigated flow-induced errors assuming that air is incompressible. However, for fast-flying aircraft, the impact of air compressibility is no longer negligible. In this study, we combine airborne data with numerical simulations to investigate the flow around wing-mounted instruments and the induced errors for different realistic flight conditions. A correction scheme for deriving particle number concentrations from in situ aerosol and cloud probes is proposed, and a new formula is provided for deriving the droplet volume from images taken by optical array probes. Shape distortions of liquid droplets can either be caused by errors in the speed with which the images are recorded or by aerodynamic forces acting at the droplet surface caused by changes of the airflow when it approaches the instrument. These forces can lead to the dynamic breakup of droplets causing artifacts in particle number concentration and size. An estimation of the critical breakup diameter as a function of flight conditions is provided. Experimental data show that the flow speed at the instrument location is smaller than the ambient flow speed. Our simulations confirm the observed difference and reveal a size-dependent impact on particle speed and concentration. This leads, on average, to a 25 % overestimation of the number concentration of particles with diameters larger than 10 µm diameter and causes distorted images of droplets and ice crystals if the flow values recorded at the instrument are used. With the proposed corrections, errors of particle number concentration and droplet volume, as well as image distortions, are significantly reduced by up to 1 order of magnitude. Although the presented correction scheme is derived for the DLR Falcon research aircraft (Saharan Aerosol Long-range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE) campaign) and validated for the DLR Falcon (Absorbing aerosol layers in a changing climate: aging, lifetime and dynamics mission conducted in 2017 (A-LIFE) campaign) and the NASA DC-8 (Atmospheric Tomography Mission (ATom) campaigns), the general conclusions hold for any fast-flying research aircraft. [ABSTRACT FROM AUTHOR]

Aerosols and clouds affect atmospheric radiative processes and climate in many complex ways and still pose the largest uncertainty in current estimates of the Earth's changing energy budget. Airborne in-situ sensors such as the Cloud, Aerosol, and Precipitation Spectrometer (CAPS) or other optical spectrometers and optical array probes provide detailed information about the horizontal and vertical distribution of aerosol and cloud properties. However, flow distortions occurring at the location where these instruments are mounted on the outside of an aircraft may directly produce artifacts in detected particle number concentration and also cause droplet deformation and/or break-up during the measurement process. Several studies have investigated flow-induced errors assuming that air is incompressible. However, for fast-flying aircraft, the impact of air compressibility is no longer negligible. In this study, we combine airborne data with numerical simulations to investigate the flow around wing-mounted instruments and the induced errors for different realistic flight conditions. A correction scheme for deriving particle number concentrations from in-situ aerosol and cloud probes is proposed, and a new formula is provided for deriving the droplet volume from images taken by optical array probes, reducing errors by up to one order of magnitude. Shape distortions of liquid droplets can either be caused by errors in the speed with which the images are recorded or by aerodynamic forces acting at the droplet surface caused by changes in the airflow around the instrument. These forces can lead to the dynamic breakup of droplets causing artifacts in particle number concentration and size. Furthermore, an estimation of the critical breakup diameter, as a function of flight conditions is provided. Experimental data show that flow speed at the instrument location is smaller than the ambient flow speed. Our simulations confirm the observed difference and reveal a size-dependent impact on particle speed and concentration. This leads, on average, to a 25 % overestimation of the number concentration of particles larger than ~10 μm} diameter and causes distorted images of droplets and ice crystals if the flow values recorded at the instrument are used. With the proposed correction scheme both errors are significantly reduced by a factor 10. Although the presented correction scheme is derived for the DLR Falcon research aircraft (SALTRACE campaign) and validated for the DLR Falcon (A-LIFE campaign) and the NASA DC-8 (ATom campaign), the general conclusions hold for any fast-flying research airplane. [ABSTRACT FROM AUTHOR]

Heterogeneous chemical cycles of pyrogenic nitrogen and halides influence tropospheric ozone and affect the stratosphere during extreme Pyrocumulonimbus (PyroCB) events. We report field‐derived N2O5 uptake coefficients, γ(N2O5), and ClNO2 yields, φ(ClNO2), from two aircraft campaigns observing fresh smoke in the lower and mid troposphere and processed/aged smoke in the upper troposphere and lower stratosphere (UTLS). Derived φ(ClNO2) varied across the full 0–1 range but was typically <0.5 and smallest in a PyroCB (<0.05). Derived γ(N2O5) was low in agricultural smoke (0.2–3.6 × 10−3), extremely low in mid‐tropospheric wildfire smoke (0.1 × 10−3), but larger in PyroCB processed smoke (0.7–5.0 × 10−3). Aged biomass burning aerosol in the UTLS had a higher γ(N2O5) of 17 × 10−3 that increased with sulfate and liquid water, but that was 1–2 orders of magnitude lower than values for aqueous sulfuric aerosol used in stratospheric models. Plain Language Summary: The injection of reactive material into Earth's atmosphere from fires affects atmospheric composition at regional and hemispheric scales. Reported stratospheric ozone depletion during extreme events, such as the 2020 Australian wildfires, illustrates one example of fire impacts and the role of heterogeneous (gas‐particle) processes. We report field quantification of rates and product yields from airborne observations of smoke. Extremely slow heterogeneous reaction rates on young smoke increase with transport and aging, but upper atmospheric values are still a factor of 10 slower than parameterizations used in stratospheric models. Heterogeneous production of ClNO2, a major lower atmospheric chlorine activation pathway, may be active on biomass burning aerosol in the upper atmosphere. Key Points: ClNO2 formation is active on biomass burning (BB) particles but decreases with transport to the upper troposphere and lower stratosphere (UTLS)N2O5 uptake coefficients are low on young BB smoke and increase with transport through a PyroCB and UTLS agingN2O5 uptake coefficients on aged BB particles in the UTLS are significantly lower than those used in model parameterizations [ABSTRACT FROM AUTHOR]

The 2019 Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) field experiment obtained a diverse set of in situ and remotely sensed measurements before and during a pyrocumulonimbus (pyroCb) event over the Williams Flats fire in Washington State. This unique dataset confirms that pyroCb activity is an efficient vertical smoke transport pathway into the upper troposphere and lower stratosphere (UTLS). The magnitude of smoke plumes observed in the UTLS has increased significantly in recent years, following unprecedented wildfire and pyroCb activity observed worldwide. The FIREX-AQ pyroCb dataset is therefore extremely relevant to a broad community, providing the first measurements of fresh smoke exhaust in the upper troposphere, including from within active pyroCb cloud tops. High-resolution remote sensing reveals that three plume cores linked to localized fire fronts, burning primarily in dense forest fuels, contributed to four total pyroCb "pulses." Rapid changes in fire geometry and spatial extent dramatically influenced the magnitude, behavior, and duration of pyroCb activity. Cloud probe measurements and weather radar identify the presence of large ice particles within the pyroCb and hydrometers below cloud base, indicating precipitation development. The resulting feedbacks suggest that vertical smoke transport efficiency was reduced slightly when compared with intense pyroCb events reaching the lower stratosphere. Physical and optical aerosol property measurements in pyroCb exhaust are compared with previous assumptions. A large suite of aerosol and gas-phase chemistry measurements sets a foundation for future studies aimed at understanding the composition of smoke plumes lifted by pyroconvection into the UTLS and their role in the climate system. [ABSTRACT FROM AUTHOR]

Aerosol intercomparisons are inherently complex as they convolve instrument-dependent detection efficiencies vs. size (which often change with pressure, temperature, or humidity) and variations in the sampled aerosol population, in addition to differences in chemical detection principles (e.g., inorganic-only nitrate vs. inorganic plus organic nitrate for two instruments). The NASA Atmospheric Tomography Mission (ATom) spanned four separate aircraft deployments which sampled the remote marine troposphere from 86 ∘ S to 82 ∘ N over different seasons with a wide range of aerosol concentrations and compositions. Aerosols were quantified with a set of carefully characterized and calibrated instruments, some based on particle sizing and some on composition measurements. This study aims to provide a critical evaluation of inlet transmissions impacting aerosol intercomparisons, and of aerosol quantification during ATom, with a focus on the aerosol mass spectrometer (AMS). The volume determined from physical sizing instruments (aerosol microphysical properties, AMP, 2.7 nm to 4.8 µm optical diameter) is compared in detail with that derived from the chemical measurements of the AMS and the single particle soot photometer (SP2). Special attention was paid to characterize the upper end of the AMS size-dependent transmission with in-field calibrations, which we show to be critical for accurate comparisons across instruments with inevitably different size cuts. Observed differences between campaigns emphasize the importance of characterizing AMS transmission for each instrument and field study for meaningful interpretation of instrument comparisons. Good agreement (regression slope =0.949 and 1.083 for ATom-1 and ATom-2, respectively; SD =0.003) was found between the composition-based volume (including AMS-quantified sea salt) and that derived from AMP after applying the AMS inlet transmission. The AMS captured, on average, 95±15 % of the standard PM 1 volume (referred to as the URG Corp. standard cut 1 µm cyclone operated at its nominal efficiency). These results support the absence of significant unknown biases and the appropriateness of the accuracy estimates for AMS total mass and volume for the mostly aged air masses encountered in ATom. The particle size ranges (and their altitude dependence) that are sampled by the AMS and complementary composition instruments (such as soluble acidic gases and aerosol, SAGA, and particle analysis by laser mass spectrometry, PALMS) are investigated to inform their use in future studies. [ABSTRACT FROM AUTHOR]

Natural aerosols in pristine regions form the baseline used to evaluate the impact of anthropogenic aerosols on climate. Sea spray aerosol (SSA) is a major component of natural aerosols. Despite its importance, the abundance of SSA is poorly constrained. It is generally accepted that wind-driven wave breaking is the principle governing SSA production. This mechanism alone, however, is insufficient to explain the variability of SSA concentration at given wind speed. The role of other parameters, such as sea surface temperature (SST), remains controversial. Here, we show that higher SST promotes SSA mass generation at a wide range of wind speed levels over the remote Pacific and Atlantic Oceans, in addition to demonstrating the wind-driven SSA production mechanism. The results are from a global scale dataset of airborne SSA measurements at 150 to 200 m above the ocean surface during the NASA Atmospheric Tomography Mission. Statistical analysis suggests that accounting for SST greatly enhances the predictability of the observed SSA concentration compared to using wind speed alone. Our results support implementing SST into SSA source functions in global models to better understand the atmospheric burdens of SSA. [ABSTRACT FROM AUTHOR]

Aerosol intercomparisons are inherently complex, as they convolve instrument-dependent detection efficiencies vs. size (which often change with pressure, temperature, or humidity) and variations on the sampled aerosol population, in addition to differences in chemical detection principles (e.g., including inorganic-only nitrate vs. inorganic plus organic nitrate for two instruments). The NASA Atmospheric Tomography Mission (ATom) spanned four separate aircraft deployments, which sampled the remote marine troposphere from 86° S to 82° N over different seasons with a wide range of aerosol concentrations and compositions. Aerosols were quantified with a set of carefully characterized and calibrated instruments, some based on particle sizing and some on composition measurements. This study aims to provide a critical evaluation of the size-related factors impacting aerosol intercomparisons, and of aerosol quantification during ATom, with a focus on the Aerosol Mass Spectrometer (AMS). The volume determined from physical sizing instruments is compared in detail with that derived from the chemical measurements of the AMS and the Single Particle Soot Photometer (SP2). Special attention was paid to characterize the upper end of the AMS size-dependent transmission with in-field calibrations, which we show to be critical for accurate comparisons across instruments with inevitably different size cuts. Observed differences between campaigns emphasize the importance of characterizing AMS transmission for each instrument and field study for meaningful interpretation of instrument comparisons. Good agreement was found between the composition-based volume (including AMS-quantified sea salt) and that derived from the size spectrometers. The very clean conditions during most of ATom resulted in substantial statistical noise (i.e., precision error), which we show to be substantially reduced by averaging at several-minute time intervals. The AMS captured, on average, 95 ± 15 % of the standard PM1 volume. These results support the absence of significant unknown biases and the appropriateness of the accuracy estimates for AMS total mass/volume for the mostly aged air masses encountered in ATom. The particle size ranges that contribute chemical composition information to the AMS and complementary composition instruments are investigated, to inform their use in future studies. [ABSTRACT FROM AUTHOR]

From 2016 to 2018 a DC-8 aircraft operated by the US National Aeronautics and Space Administration (NASA) made four series of flights, profiling the atmosphere from 180 m to ∼12 km above sea level (km a.s.l.) from the Arctic to the Antarctic over both the Pacific and Atlantic oceans. This program, the Atmospheric Tomography Mission (ATom), sought to sample the troposphere in a representative manner, making measurements of atmospheric composition in each season. This paper describes the aerosol microphysical measurements and derived quantities obtained during this mission. Dry size distributions from 2.7 nm to 4.8 µ m in diameter were measured in situ at 1 Hz using a battery of instruments: 10 condensation particle counters with different nucleation diameters, two ultra-high-sensitivity aerosol size spectrometers (UHSASs), one of which measured particles surviving heating to 300 ∘ C, and a laser aerosol spectrometer (LAS). The dry aerosol measurements were complemented by size distribution measurements from 0.5 to 930 µ m diameter at near-ambient conditions using a cloud, aerosol, and precipitation spectrometer (CAPS) mounted under the wing of the DC-8. Dry aerosol number, surface area, and volume, and optical scattering and asymmetry parameters at several wavelengths from the near-UV to the near-IR ranges were calculated from the measured dry size distributions (2.7 nm to 4.8 µ m). Dry aerosol mass was estimated by combining the size distribution data with particle density estimated from independent measurements of aerosol composition with a high-resolution aerosol mass spectrometer and a single-particle soot photometer. We describe the instrumentation and fully document the aircraft inlet and flow distribution system, the derivation of uncertainties, and the calculation of data products from combined size distributions. Comparisons between the instruments and direct measurements of some aerosol properties confirm that in-flight performance was consistent with calibrations and within stated uncertainties for the two deployments analyzed. The unique ATom dataset contains accurate, precise, high-resolution in situ measurements of dry aerosol size distributions, and integral parameters, and estimates and measurements of optical properties, for particles < 4.8 µ m in diameter that can be used to evaluate aerosol abundance and processes in global models. [ABSTRACT FROM AUTHOR]

The article focuses on the ML-CIRRUS experiment which deployed the High Altitude and Long Range Research Aircraft (HALO) along with satellites and models to acquire new data about nucleation, life cycle, predictability, and climate impact of natural cirrus and anthropogenic contrail cirrus. The experiment was conducted over Europe out of Oberpfaffenhofen in southern Germany in March and April 2014 which is a well suited to reach cirrus over all parts of Europe.

Aerosols in the remote marine atmosphere are important components of the earth's chemistry-climate system. In these regions, cloud condensation nuclei (CCN) are often limited in abundance, and the radiative properties of clouds are particularly sensitive to changes in CCN concentrations. Aerosol particles affect tropospheric chemistry through heterogeneous processes and by serving as sources and sinks for compounds. Measurements of the remote tropospheric aerosol provide important constraints for the Eulerian global models that are used for analysis and prediction, and Lagrangian models that are used to evaluate sources and understanding of transport and chemical and physical processes. The Atmospheric Tomography Mission (ATom) was designed to improve understanding of chemistry and climate processes in the remote atmosphere over the oceans. Using the long-range NASA DC-8 research aircraft, ATom was composed of four sets of flights over the middle of the Pacific and Atlantic Oceans, from ~82°N to ~86°S. During these flights, the DC-8, repeatedly ascended and descended between ~0.15 and ~12 km in altitude. The four flight sets were completed in August-September 2016 (ATom-1), January-February 2017 (ATom-2), September-October 2017 (ATom-3), and April-May 2018 (ATom-4). The payload included fast-response aerosol size distributions, bulk and single-particle aerosol composition and aerosol optical properties, along with many reactive, tracer, and greenhouse gas-phase species.Initial results from analysis of the Atom aerosol observations will be summarized, including: evidence for the global-scale importance of new particle formation in the upper tropical troposphere for CCN abundance; the first global-scale measurements of free tropospheric sea-salt concentrations that provide strict limits on halogen abundance in the upper troposphere; the distribution of organic, biomass-burning, black carbon, and dust particle concentrations that constrain sources, transport, and removal; and aerosol composition measurements that show organic aerosol loss in the remote troposphere and that place constraints on aerosol pH, which influences a number of aerosol chemical processes. Access to the ATom dataset, future data products, and opportunities for further analysis will also be discussed. [ABSTRACT FROM AUTHOR]

Current estimates suggest that globally, about one third of cloud condensation nuclei (CCN) affecting low-level clouds originate from new particle formation (NPF) that takes place in the free troposphere. However, the exact mechanisms of how new particles form and grow to CCN sizes, and their relative importance are not yet well quantified. We investigate the formation of new particles and their growth to CCN-sizes in the remote marine atmosphere over the Pacific and Atlantic basins (~80 °N to ~86 °S). This is done using size distribution measurements (0.003-4.8 µm) from the airborne-based NASA Atmospheric Tomography global survey (ATom; 2016-2018), back trajectory data and two aerosol microphysics box models.Newly formed particles are ubiquitous at high altitudes throughout broad regions of the tropics and subtropics under low condensation sink conditions and are associated with upwelling in convective clouds. This pattern is observed over four seasons and both ocean basins. NPF was also found in the free troposphere over the Southern Ocean in February 2017, however it was not observed in August 2016, indicating seasonal differences.In this study we explore processes that govern NPF and growth in the tropical and subtropical free troposphere, and over the Southern Ocean, discuss similarities and differences in NPF in these regions, examine which nucleation scheme (e.g. binary, ternary, or charged) best explain the observations, evaluate whether observed sulfur precursors alone (SO2 and DMS) can explain the NPF, and discuss the growth of these new particles to CCN sizes. [ABSTRACT FROM AUTHOR]