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The purpose of this study is to understand the drivers of cloud droplet formation in orographic clouds. We used a combination of modeling, in situ, and remote sensing measurements at the high-altitude Helmos Hellenic Atmospheric Aerosol and Climate Change ((HAC)2) station, which is located at the top of Mt. Helmos (1314 m above sea level), Greece, during the Cloud–AerosoL InteractionS in the Helmos Background TropOsphere (CALISHTO) campaign in fall 2021 (https://calishto.panacea-ri.gr/, last access: 1 August 2024) to examine the origins of the aerosols (i.e., local aerosol from the planetary boundary layer (PBL) or long-range-transported aerosol from the free-tropospheric layer (FTL) contributing to the cloud condensation nuclei (CCN)), their characteristics (hygroscopicity, size distribution, and mixing state), and the vertical velocity distributions and resulting supersaturations. We found that the characteristics of the PBL aerosol were considerably different from FTL aerosol and use the aerosol particle number and equivalent mass concentration of the black carbon (eBC) in order to determine when (HAC)2 was within the FTL or PBL based on time series of the height of the PBL. During the (HAC)2 cloud events we sample a mixture of interstitial aerosol and droplet residues, which we characterize using a new approach that utilizes the in situ droplet measurements to determine time periods when the aerosol sample is purely interstitial. From the dataset we determine the properties (size distribution and hygroscopicity) of the pre-cloud, activated, and interstitial aerosol. The hygroscopicity of activated aerosol is found to be higher than that of the interstitial or pre-cloud aerosol. A series of closure studies with the droplet parameterization shows that cloud droplet concentration (Nd) and supersaturation can be predicted to within 25 % of observations when the aerosol size distributions correspond to pre-cloud conditions. The analysis of the characteristic supersaturation of each aerosol population indicates that droplet formation in clouds is aerosol-limited when formed in FTL air masses – hence droplet formation is driven by aerosol variations, while clouds formed in the PBL tend to be velocity-limited and droplet variations are driven by fluctuations in vertical velocity. Given that the cloud dynamics do not vary significantly between air masses, the variation in aerosol concentration and type is mostly responsible for these shifts in cloud microphysical state and sensitivity to aerosol. With these insights, the remote sensing of cloud droplets in such clouds can be used to infer either CCN spectra (when in the FTL) or vertical velocity (when in the PBL). In conclusion, we show that a coordinated measurement of aerosol and cloud properties, together with the novel analysis approaches presented here, allows for the determination of the drivers of droplet formation in orographic clouds and their sensitivity to aerosol and vertical velocity variations.

In May–June 2019, smoke plumes from wildfires in Alberta, Canada, were advected all the way to Europe. To analyze the evolution of the plumes and to estimate the amount of smoke aerosols transported to Europe, retrievals from the spaceborne lidar CALIOP (Cloud-Aerosol LIdar with Orthogonal Polarization) were used. The plumes were located with the help of a trajectory analysis, and the masses of smoke aerosols were retrieved from the CALIOP observations. The accuracy of the CALIOP mass retrievals was compared with the accuracy of ground-based lidars/ceilometer near the source in North America and after the long-range transport in Europe. Overall, CALIOP and the ground-based lidars/ceilometer produced comparable results. Over North America the CALIOP layer mean mass was 30 % smaller than the ground-based estimates, whereas over southern Europe that difference varied between 12 % and 43 %. Finally, the CALIOP mass retrievals were compared with simulated aerosol concentrations from two reanalysis models: MERRA-2 (Modern-Era Retrospective analysis for Research and Applications, Version 2) and CAMS (Copernicus Atmospheric Monitoring System). The simulated total column aerosol optical depths (AODs) and the total column mass concentration of smoke agreed quite well with CALIOP observations, but the comparison of the layer mass concentration of smoke showed significant discrepancies. The amount of smoke aerosols in the model simulations was consistently smaller than in the CALIOP retrievals. These results highlight the limitations of such models and more specifically their limitation to reproduce properly the smoke vertical distribution. They indicate that CALIOP is a useful tool monitoring smoke plumes over secluded areas, whereas reanalysis models have difficulties in representing the aerosol mass in these plumes. This study shows the advantages of spaceborne aerosol lidars, e.g., being of paramount importance to monitor smoke plumes, and reveals the urgent need of future lidar missions in space.

The European Aerosol Research Lidar Network (EARLINET), part of the Aerosols, Clouds and Trace gases Research Infrastructure (ACTRIS), organized an intensive observational campaign in May 2020, with the objective of monitoring the atmospheric state over Europe during the COVID-19 lockdown and relaxation period. Besides the standard operational processing of the lidar data in EARLINET, for seven EARLINET sites having collocated sun-photometric observations in the Aerosol Robotic Network (AERONET), a network exercise was held in order to derive profiles of the concentration and effective column size distributions of the aerosols in the atmosphere, by applying the GRASP/GARRLiC (from Generalized Aerosol Retrieval from Radiometer and Lidar Combined data – GARRLiC – part of the Generalized Retrieval of Atmosphere and Surface Properties – GRASP) inversion algorithm. The objective of this network exercise was to explore the possibility of identifying the anthropogenic component and of monitoring its spatial and temporal characteristics in the COVID-19 lockdown and relaxation period. While the number of cases is far from being statistically significant so as to provide a conclusive description of the atmospheric aerosols over Europe during this period, this network exercise was fundamental to deriving a common methodology for applying GRASP/GARRLiC to a network of instruments with different characteristics. The limits of the approach are discussed, in particular the missing information close to the ground in the lidar measurements due to the instrument geometry and the sensitivity of the GRASP/GARRLiC retrieval to the settings used, especially for cases with low aerosol optical depth (AOD) like the ones we show here. We found that this sensitivity is well-characterized in the GRASP/GARRLiC products, since it is included in their retrieval uncertainties.

Active remote sensors equipped with the capability to detect polarization, a shape-relevant parameter, are essential to aerosol particle identification in the vertical domain. Most commonly, the linear particle depolarization ratio has been available at the shorter wavelengths of 355 and/or 532 nm. Recently, linear particle depolarization ratios at longer wavelengths (910, 1064, and 1565 nm) have emerged in lidar aerosol research. In this study, a synergy of three lidars, namely a PollyXT lidar, a Vaisala CL61 ceilometer, and a HALO Photonics StreamLine Pro Doppler lidar, as well as in situ aerosol and pollen observations have been utilized to investigate the spectral dependence of birch and pine pollen particles. We found that, regardless of the pollen type, the linear particle depolarization ratio was subject to the amount of pollen and its relative contribution to the aerosol mixture in the air. More specifically, during birch pollination, characteristic linear particle depolarization ratios of 5 ± 2 % (355 nm), 28 ± 6 % (532 nm), 23 ± 6 % (910 nm), and 33 ± 4 % (1565 nm) were retrieved at the pollen layer. Regarding the pine-dominant period, characteristic linear particle depolarization ratios of 6 ± 2 %, 43 ± 11 %, 22 ± 6 %, and 26 ± 3 % were determined at wavelengths of 355, 532, 910, and 1565 nm, respectively. For birch, the linear particle depolarization ratio at 1565 nm was the highest, followed by the 532 and 910 nm wavelengths, respectively. A sharp decrease at 355 nm was evident for birch pollen. For pine pollen, a maximum at the 532 nm wavelength was observed. There was no significant change in the linear particle depolarization ratio at 910 nm for the pollen types considered in this study. Given the low concentration of pollen in the air, the inclusion of the longer wavelengths (910 and 1565 nm) for the detection of birch and pine can be beneficial due to their sensitivity to trace large aerosol particles.

This paper presents a collection of lidar-derived aerosol intensive optical properties for several aerosol types, namely the particle linear depolarization ratio, the extinction-to-backscatter ratio (lidar ratio) and the Ångström exponent. The data collection, named DeLiAn, is based on globally distributed, long-term, ground-based, multiwavelength, Raman and polarization lidar measurements, conducted mainly with lidars that have been developed at the Leibniz Institute for Tropospheric Research. The intensive optical properties are presented at two wavelengths, 355 and 532 nm, for 13 aerosol categories. The categories cover the basic aerosol types (i.e., marine, pollution, continental European background, volcanic ash, smoke, mineral dust), as well as the most frequently observed mixtures they form. This extensive collection also incorporates more peculiar aerosol categories, including dried marine aerosol that, compared to marine aerosol, exhibits a significantly enhanced depolarization ratio (up to 15 %). Besides Saharan dust, additional mineral dust types related to their source region were identified due to their lower lidar ratios (Central Asian and Middle Eastern dust). In addition, extreme wildfire events (such as in north America and Australia) emitted smoke into the stratosphere showing significantly different optical properties, i.e., high depolarization values (up to 25 %), compared to tropospheric smoke. The data collection reflects and underlines the variety of aerosol mixtures in the atmosphere and can be used for the development of aerosol-typing schemes. The paper contains the most up-to-date and comprehensive overview of optical properties from aerosol lidar measurements and, therefore, provides a solid basis for future aerosol retrievals in the frame of both spaceborne and ground-based lidars. Furthermore, DeLiAn can assist the efforts for the harmonization of satellite records of aerosol properties performed at different wavelengths.

We carried out a closure study of aerosol–cloud interactions during stratocumulus formation using a large eddy simulation model UCLALES–SALSA (University of California Los Angeles large eddy simulation model–sectional aerosol module for large applications) and observations from the 2020 cloud sampling campaign at Puijo SMEAR IV (Station for Measuring Ecosystem–Atmosphere Relations) in Kuopio, Finland. The unique observational setup combining in situ and cloud remote sensing measurements allowed a closer look into the aerosol size–composition dependence of droplet activation and droplet growth in turbulent boundary layer driven by surface forcing and radiative cooling. UCLALES–SALSA uses spectral bin microphysics for aerosols and hydrometeors, and incorporates a full description of their interactions into the turbulent-convective radiation-dynamical model of stratocumulus. Based on our results, the model successfully described the probability distribution of updraught velocities and consequently the size dependency of aerosol activation into cloud droplets, and further recreated the size distributions for both interstitial aerosol and cloud droplets. This is the first time such a detailed closure is achieved not only accounting for activation of cloud droplets in different updraughts, but also accounting for processes evaporating droplets and drizzle production through coagulation–coalescence. We studied two cases of cloud formation, one diurnal (24 September 2020) and one nocturnal (31 October 2020), with high and low aerosol loadings, respectively. Aerosol number concentrations differ more than 1 order of magnitude between cases and therefore, lead to cloud droplet number concentration (CDNC) values which range from less than 100 cm−3 up to 1000 cm−3. Different aerosol loadings affected supersaturation at the cloud base, and thus the size of aerosol particles activating to cloud droplets. Due to higher CDNC, the mean size of cloud droplets in the diurnal high aerosol case was lower. Thus, droplet evaporation in downdraughts affected more the observed CDNC at Puijo altitude compared to the low aerosol case. In addition, in the low aerosol case, the presence of large aerosol particles in the accumulation mode played a significant role in the droplet spectrum evolution as it promoted the drizzle formation through collision and coalescence processes. Also, during the event, the formation of ice particles was observed due to subzero temperature at the cloud top. Although the modelled number concentration of ice hydrometeors was too low to be directly measured, the retrieval of hydrometeor sedimentation velocities with cloud radar allowed us to assess the realism of modelled ice particles. The studied cases are presented in detail and can be further used by the cloud modellers to test and validate their models in a well-characterized modelling setup. We also provide recommendations on how increasing amount of information on aerosol properties could improve the understanding of processes affecting cloud droplet number and liquid water content in stratiform clouds.

Upon a new measurement technique, it is possible to sharpen the determination of microphysical properties of cloud droplets using high resolving power imaging. The shape, size, and position of each particle inside a well-defined, three-dimensional sample volume can be measured with holographic methods without assumptions of particle properties. In situ cloud measurements were carried out at the Puijo station in Kuopio, Finland, focusing on intercomparisons between cloud droplet analyzers over 2 months in September–November 2020. The novel holographic imaging instrument (ICEMET) was adapted to measure microphysical properties of liquid clouds, and these values were compared with parallel measurements of a cloud droplet spectrometer (FM-120) and particle measurements using a twin-inlet system. When the intercomparison was carried out during isoaxial sampling, our results showed good agreement in terms of variability between the instruments, with the averaged ratios between ICEMET and FM-120 being 0.6 ± 0.2, 1.0 ± 0.5, and 1.2 ± 0.2 for the total number concentration (Nd) of droplets, liquid water content (LWC), and median volume diameter (MVD), respectively. This agreement during isoaxial sampling was also confirmed by mutual correlation and Pearson correlation coefficients. The ICEMET-observed LWC was more reliable than FM-120 (without a swivel-head mount), which was verified by comparing the estimated LWC to measured values, whereas the twin-inlet DMPS system and FM-120 observations of Nd showed good agreement both in variability and amplitude. Field data revealed that ICEMET can detect small cloud droplets down to 5 µm via geometric magnification.

Lidar observations were analysed to characterize atmospheric pollen at four EARLINET (European Aerosol Research Lidar Network) stations (Hohenpeißenberg, Germany; Kuopio, Finland; Leipzig, Germany; and Warsaw, Poland) during the ACTRIS (Aerosol, Clouds and Trace Gases Research Infrastructure) COVID-19 campaign in May 2020. The reanalysis (fully quality-assured) lidar data products, after the centralized and automatic data processing with the Single Calculus Chain (SCC), were used in this study, focusing on particle backscatter coefficients at 355 and 532 nm and particle linear depolarization ratios (PDRs) at 532 nm. A novel method for the characterization of the pure pollen depolarization ratio was presented, based on the non-linear least square regression fitting using lidar-derived backscatter-related Ångström exponents (BAEs) and PDRs. Under the assumption that the BAE between 355 and 532 nm should be zero (±0.5) for pure pollen, the pollen depolarization ratios were estimated: for Kuopio and Warsaw stations, the pollen depolarization ratios at 532 nm were of 0.24 (0.19–0.28) during the birch-dominant pollen periods, whereas for Hohenpeißenberg and Leipzig stations, the pollen depolarization ratios of 0.21 (0.15–0.27) and 0.20 (0.15–0.25) were observed for periods of mixture of birch and grass pollen. The method was also applied for the aerosol classification, using two case examples from the campaign periods; the different pollen types (or pollen mixtures) were identified at Warsaw station, and dust and pollen were classified at Hohenpeißenberg station.

We studied ice-nucleating abilities of particulate emissions from a modern heavy-duty diesel engine using three different types of fuel. The polydisperse particle emissions were sampled during engine operation and introduced to a continuous-flow diffusion chamber (CFDC) instrument at a constant relative humidity RHwater=110 %, while the temperature was ramped between −43 and −32 ∘C (T scan). The tested fuels were EN 590 compliant low-sulfur fossil diesel, hydrotreated vegetable oil (HVO), and rapeseed methyl ester (RME); all were tested without blending. Sampling was carried out at different stages in the engine exhaust aftertreatment system, with and without simulated atmospheric processing using an oxidation flow reactor. In addition to ice nucleation experiments, we used supportive instrumentation to characterize the emitted particles for their physicochemical properties and presented six parameters. We found that the studied emissions contained no significant concentrations of ice-nucleating particles likely to be of atmospheric relevance. The substitution of fossil diesel with renewable fuels, using different emission aftertreatment systems such as a diesel oxidation catalyst, and photochemical aging of total exhaust had only minor effect on their ice-nucleating abilities.

Aerosol particles play an important role in the microphysics of clouds and hence in their likelihood to precipitate. In the changing climate already-dry areas such as the United Arab Emirates (UAE) are predicted to become even drier. Comprehensive observations of the daily and seasonal variation in aerosol particle properties in such locations are required, reducing the uncertainty in such predictions. We analyse observations from a 1-year measurement campaign at a background location in the United Arab Emirates to investigate the properties of aerosol particles in this region, study the impact of boundary layer mixing on background aerosol particle properties measured at the surface, and study the temporal evolution of the aerosol particle cloud formation potential in the region. We used in situ aerosol particle measurements to characterise the aerosol particle composition, size, number, and cloud condensation nuclei (CCN) properties; in situ SO2 measurements as an anthropogenic signature; and a long-range scanning Doppler lidar to provide vertical profiles of the horizontal wind and turbulent properties to monitor the evolution of the boundary layer. Anthropogenic sulfate dominated the aerosol particle mass composition in this location. There was a clear diurnal cycle in the surface wind direction, which had a strong impact on aerosol particle total number concentration, SO2 concentration, and black carbon mass concentration. Local sources were the predominant source of black carbon as concentrations clearly depended on the presence of turbulent mixing, with much higher values during calm nights. The measured concentrations of SO2, instead, were highly dependent on the surface wind direction as well as on the depth of the boundary layer when entrainment from the advected elevated layers occurred. The wind direction at the surface or of the elevated layer suggests that the oil refineries and the cities of Dubai and Abu Dhabi and other coastal conurbations were the remote sources of SO2. We observed new-aerosol-particle formation events almost every day (on 4 d out of 5 on average). Calm nights had the highest CCN number concentrations and lowest κ values and activation fractions. We did not observe any clear dependence of CCN number concentration and κ parameter on the height of the daytime boundary layer, whereas the activation fraction did show a slight increase with increasing boundary layer height due to the change in the shape of the aerosol particle size distribution where the relative portion of larger aerosol particles increased with increasing boundary layer height. We believe that this indicates that size is more important than chemistry for aerosol particle CCN activation at this site. The combination of instrumentation used in this campaign enabled us to identify periods when anthropogenic pollution from remote sources that had been transported in elevated layers was present and had been mixed down to the surface in the growing boundary layer.

A quantitative comparison study for Raman lidar and ceilometer observations, and for model simulations of mass concentration estimates of smoke particles is presented. Layers of biomass burning aerosol particles were observed in the lower troposphere, at 2 to 5 km height on 4 to 6 June 2019, over Kuopio, Finland. These long-range-transported smoke particles originated from a Canadian wildfire event. The most pronounced smoke plume detected on 5 June was intensively investigated. Optical properties were retrieved from the multi-wavelength Raman polarization lidar PollyXT. Particle linear depolarization ratios (PDRs) of this plume were measured to be 0.08±0.02 at 355 nm and 0.05±0.01 at 532 nm, suggesting the presence of partly coated soot particles or particles that have mixed with a small amount of dust or other non-spherical aerosol type. The layer-mean PDR at 355 nm (532 nm) decreased during the day from ∼ 0.11 (0.06) in the morning to ∼ 0.05 (0.04) in the evening; this decrease with time could be linked to the particle aging and related changes in the smoke particle shape properties. Lidar ratios were derived as 47±5 sr at 355 nm and 71±5 sr at 532 nm. A complete ceilometer data processing for a Vaisala CL51 ceilometer is presented from a sensor-provided attenuated backscatter coefficient to particle mass concentration (including the water vapor correction for high latitude for the first time). Aerosol backscatter coefficients (BSCs) were measured at four wavelengths (355, 532, 1064 nm from PollyXT and 910 nm from CL51). Two methods, based on a combined lidar and sun-photometer approach, are applied for mass concentration estimations from both PollyXT and the ceilometer CL51 observations. In the first method, no. 1, we used converted BSCs at 532 nm (from measured BSCs) by corresponding measured backscatter-related Ångström exponents, whereas in the second method, no. 2, we used measured BSCs at each wavelength independently. A difference of ∼ 12 % or ∼ 36 % was found between PollyXT and CL51 estimated mass concentrations using method no. 1 or no. 2, showing the potential of mass concentration estimates from a ceilometer. Ceilometer estimations have an uncertainty of ∼ 50 % in the mass retrieval, but the potential of the data lies in the great spatial coverage of these instruments. The mass retrievals were compared with the Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) meteorological and aerosol reanalysis. The inclusion of dust (as indicated by MERRA-2 data) in the retrieved mass concentration is negligible considering the uncertainties, which also shows that ceilometer observations for mass retrievals can be used even without exact knowledge of the composition of the smoke-dominated aerosol plume in the troposphere.

Lidar observations during the pollen season 2019 at the European Aerosol Research Lidar Network (EARLINET) station in Kuopio, Finland, were analyzed in order to optically characterize atmospheric pollen. Pollen concentration and type information were obtained by a Hirst-type volumetric air sampler. Previous studies showed the detectability of non-spherical pollen using depolarization ratio measurements. We present lidar depolarization ratio measurements at three wavelengths of atmospheric pollen in ambient conditions. In addition to the depolarization ratio detected with the multiwavelength Raman polarization lidar PollyXT at 355 and 532 nm, depolarization measurements of a co-located Halo Doppler lidar at 1565 nm were utilized. During a 4 d period of high birch (Betula) and spruce (Picea abies) pollen concentrations, unusually high depolarization ratios were observed within the boundary layer. Detected layers were investigated regarding the share of spruce pollen to the total pollen number concentration. Daily mean linear particle depolarization ratios of the pollen layers on the day with the highest spruce pollen share are 0.10 ± 0.02, 0.38 ± 0.23 and 0.29 ± 0.10 at 355, 532 and 1565 nm, respectively, whereas on days with lower spruce pollen share, depolarization ratios are lower with less wavelength dependence. This spectral dependence of the depolarization ratios could be indicative of big, non-spherical spruce pollen. The depolarization ratio of pollen particles was investigated by applying a newly developed method and assuming a backscatter-related Ångström exponent of zero. Depolarization ratios of 0.44 and 0.16 at 532 and 355 nm for the birch and spruce pollen mixture were determined.

The depolarization ratio is a valuable parameter for lidar-based aerosol categorization. Usually, the aerosol particle depolarization ratio is determined at relatively short wavelengths of 355 nm and/or 532 nm, but some multi-wavelength studies including longer wavelengths indicate strong spectral dependency. Here, we investigate the capabilities of Halo Photonics StreamLine Doppler lidars to retrieve the particle linear depolarization ratio at the 1565 nm wavelength. We utilize collocated measurements with another lidar system, PollyXT at Limassol, Cyprus, and at Kuopio, Finland, to compare the depolarization ratio observed by the two systems. For mineral-dust-dominated cases we find typically a slightly lower depolarization ratio at 1565 nm than at 355 and 532 nm. However, for dust mixed with other aerosol we find a higher depolarization ratio at 1565 nm. For polluted marine aerosol we find a marginally lower depolarization ratio at 1565 nm compared to 355 and 532 nm. For mixed spruce and birch pollen we find a slightly higher depolarization ratio at 1565 nm compared to 532 nm. Overall, we conclude that Halo Doppler lidars can provide a particle linear depolarization ratio at the 1565 nm wavelength at least in the lowest 2–3 km above ground.

Long-term statistics of atmospheric aerosol and especially cloud scavenging were studied at the Puijo measurement station in Kuopio, Finland, during October 2010–November 2014. Aerosol size distributions, scattering coefficients at three different wavelengths (450, 550, and 700 nm), and absorption coefficient at wavelength 637 nm were measured with a special inlet system to sample interstitial and total aerosol in clouds. On average, accumulation mode particle concentration was found to be correlated with temperature with the lowest average concentrations of 200 cm−3 around 0 ∘C increasing to 800 cm−3 at 20 ∘C. The scavenging efficiencies of both scattering and absorbing material were observed to have a slightly positive temperature correlation in in-cloud measurements. At 0 ∘C, the scavenging efficiencies of scattering and absorbing material were 0.85 and 0.55 with slopes of 0.005 and 0.003 ∘C−1, respectively. Scavenging efficiencies were also studied as a function of the diameter at which half of the particles are activated into cloud droplets. This analysis indicated that there is a higher fraction of absorbing material, typically black carbon, in smaller sizes so that at least 20 %–30 % of interstitial particles within clouds consist of absorbing material. In addition, the PM1 inlet revealed that approximately 20 % of absorbing material was observed to reside in particles with ambient diameter larger than ∼ 1 µm at relative humidity below 90 %. Similarly, 40 % of scattering material was seen to be in particles larger than 1 µm. Altogether, this dataset provides information on the size-dependent aerosol composition and in-cloud scavenging of different types of aerosol. The dataset can be useful in evaluating how well the size-dependent aerosol composition is simulated in global aerosol models and how well these models capture the in-cloud scavenging of different types of aerosol in stratus clouds.

We introduce an automated aerosol type classification method, called Source Classification Analysis (SCAN). SCAN is based on predefined and characterized aerosol source regions, the time that the air parcel spends above each geographical region, and a number of additional criteria. The output of SCAN is compared with two independent aerosol classification methods, which use the intensive optical parameters from lidar data: (1) the Mahalanobis distance automatic aerosol type classification (MD) and (2) a neural network aerosol typing algorithm (NATALI). In this paper, data from the European Aerosol Research Lidar Network (EARLINET) have been used. A total of 97 free tropospheric aerosol layers from four typical EARLINET stations (i.e., Bucharest, Kuopio, Leipzig, and Potenza) in the period 2014–2018 were classified based on a 3β+2α+1δ lidar configuration. We found that SCAN, as a method independent of optical properties, is not affected by overlapping optical values of different aerosol types. Furthermore, SCAN has no limitations concerning its ability to classify different aerosol mixtures. Additionally, it is a valuable tool to classify aerosol layers based on even single (elastic) lidar signals in the case of lidar stations that cannot provide a full data set (3β+2α+1δ) of aerosol optical properties; therefore, it can work independently of the capabilities of a lidar system. Finally, our results show that NATALI has a lower percentage of unclassified layers (4 %), while MD has a higher percentage of unclassified layers (50 %) and a lower percentage of cases classified as aerosol mixtures (5 %).

We present a novel algorithm for characterizing the optical properties of pure pollen particles, based on the depolarization ratio values obtained in lidar measurements. The algorithm was first tested and validated through a simulator and then applied to the lidar observations during a 4-month pollen campaign from May to August 2016 at the European Aerosol Research Lidar Network (EARLINET) station in Kuopio (62∘44′ N, 27∘33′ E), in Eastern Finland. With a Burkard sampler, 20 types of pollen were observed and identified from concurrent measurements, with birch (Betula), pine (Pinus), spruce (Picea), and nettle (Urtica) pollen being the most abundant, contributing more than 90 % of the total pollen load, regarding number concentrations. Mean values of lidar-derived optical properties in the pollen layer were retrieved for four intense pollination periods (IPPs). Lidar ratios at both 355 and 532 nm ranged from 55 to 70 sr for all pollen types, without significant wavelength dependence. An enhanced depolarization ratio was found when there were pollen grains in the atmosphere, and an even higher depolarization ratio (with mean values of 0.25 or 0.14) was observed with the presence of the more non-spherical spruce or pine pollen. Under the assumption that the backscatter-related Ångström exponent between 355 and 532 nm should be zero for pure pollen, the depolarization ratio of pure pollen particles at 532 nm was assessed, resulting in 0.24±0.01 and 0.36±0.01 for birch and pine pollen, respectively. Pollen optical properties at 1064 and 355 nm were also estimated. The backscatter-related Ångström exponent between 532 and 1064 nm was assessed to be ∼0.8 (∼0.5) for pure birch (pine) pollen; thus the longer wavelength would be a better choice to trace pollen in the air. Pollen depolarization ratios of 0.17 and 0.30 at 355 nm were found for birch and pine pollen, respectively. The depolarization values show a wavelength dependence for pollen. This can be the key parameter for pollen detection and characterization.

Continuous, semi-long-term, ground-based in situ cloud measurements were conducted during the Pallas Cloud Experiment (PaCE) in 2013. The measurements were carried out in Finnish sub-Arctic region at Sammaltunturi station (67∘58′ N, 24∘07′ E; 560 m a.s.l.), part of Pallas Atmosphere – Ecosystem Supersite and Global Atmosphere Watch (GAW) program. The main motivation of the campaign was to conduct in situ cloud measurements with three different cloud spectrometer probes and perform an evaluation of their ground-based setups. Therefore, we mutually compared the performance of the cloud and aerosol spectrometer (CAS), the cloud droplet probe (CDP) and the forward-scattering spectrometer probe (FSSP-100) (DMT; Boulder, CO, USA). We investigated how different meteorological parameters affect each instrument's ground-based setup operation and quantified possible biases and discrepancies of different microphysical cloud properties. Based on the obtained results we suggested limitations for further use of the instrument setups in campaigns where the focus is on investigating aerosol–cloud interactions. Measurements in this study were made by instruments owned by the Finnish Meteorological Institute and results concern their operation in sub-Arctic conditions with frequently occurring supercooled clouds. The measured parameter from each instrument was the size distribution, and additionally we derived the number concentration, the effective diameter, the median volume diameter and the liquid water content. A complete intercomparison between the CAS probe and the FSSP-100 ground setups and additionally between the FSSP-100 and the CDP probe ground setups was made and presented. Unfortunately, there was not a sufficient amount of common data to compare all three probes together due to operational problems of the CDP ground setup in sub-zero conditions. The CAS probe that was fixed to one direction lost a significant number of cloud droplets when the wind direction was out of wind iso-axial conditions in comparison with the FSSP-100 and the CDP, which were both placed on a rotating platform. We revealed that CAS and FSSP-100 had good agreement in deriving sizing parameters (effective diameter and median volume diameter from 5 to 35 µm) even though CAS was losing a significant amount of cloud droplets. The most sensitive derived parameter was liquid water content, which was strongly connected to the wind direction and temperature.

One year of ground-based night-time Raman lidar observations has been analysed under the Optimization of Aerosol Seeding In rain enhancement Strategies (OASIS) project, in order to characterize the aerosol particle properties over a rural site in the United Arab Emirates. In total, 1130 aerosol particle layers were detected during the 1-year measurement campaign which took place between March 2018 and February 2019. Several subsequent aerosol layers could be observed simultaneously in the atmosphere up to 11 km. The observations indicate that the measurement site is a receptor of frequent dust events, but predominantly the dust is mixed with aerosols of anthropogenic and/or marine origin. The mean aerosol optical depth over the measurement site ranged at 0.37 ± 0.12 and 0.21 ± 0.11 for 355 and 532 nm, respectively. Moreover, mean lidar ratios of 43 ± 11 sr at a wavelength of 355 nm and 39 ± 10 sr at 532 nm were found. The average linear particle depolarization ratio measured over the course of the campaign was 15 ± 6 % and 19 ± 7 % at the 355 and 532 nm wavelengths, respectively. Since the region is both a source and a receptor of mineral dust, we have also explored the properties of Arabian mineral dust of the greater area of the United Arab of Emirates and the Arabian Peninsula. The observed Arabian dust particle properties were 45 ± 5 (42 ± 5) sr at 355 (532) nm for the lidar ratio, 25 ± 2 % (31 ± 2 %) for the linear particle depolarization ratio at 355 (532) nm, and 0.3 ± 0.2 (0.2 ± 0.2) for the extinction-related Ångström exponent (backscatter-related Ångström exponent) between 355 and 532 nm. This study is the first to report comprehensive optical properties of the Arabian dust particles based on 1-year long observations, using to their fullest the capabilities of a multi-wavelength Raman lidar instrument. The results suggest that the mineral dust properties over the Middle East and western Asia, including the observation site, are comparable to those of African mineral dust with regard to the particle depolarization ratios, but not for lidar ratios. The smaller lidar ratio values in this study compared to the reference studies are attributed to the difference in the geochemical characteristics of the soil originating in the study region compared to northern Africa.

Measurements of geometrical and optical properties of cirrus clouds, performed with a multi-wavelength PollyXT Raman lidar during the period 2008 to 2016, are analysed. The measurements were performed with the same instrument, during sequential periods, in three places at different latitudes, Gwal Pahari (28.43∘ N, 77.15∘ E; 243 m a.s.l.) in India, Elandsfontein (26.25∘ S, 29.43∘ E; 1745 m a.s.l.) in South Africa and Kuopio (62.74∘ N, 27.54∘ E; 190 m a.s.l.) in Finland. The lidar dataset was processed by an automatic cirrus cloud masking algorithm, developed in the frame of this work. In the following, we present a statistical analysis of the lidar-retrieved geometrical characteristics (cloud boundaries, geometrical thickness) and optical properties of cirrus clouds (cloud optical depth, lidar ratio, ice crystal depolarisation ratio) measured over the three areas that correspond to subtropical and subarctic regions as well as their seasonal variability. The effect of multiple scattering from ice particles to the derived optical products is also considered and corrected in this study. Our results show that cirrus layers, which have a noticeable monthly variability, were observed between 6.5 and 13 km, with temperatures ranging from −72 to −27 ∘C. The observed differences on cirrus clouds' geometrical and optical properties over the three regions are discussed in terms of latitudinal and temperature dependence. The latitudinal dependence of the geometrical properties is consistent with satellite observations, following the pattern observed with CloudSat, with decreasing values towards the poles. The geometrical boundaries have their highest values in the subtropical regions, and overall, our results seem to demonstrate that subarctic cirrus clouds are colder, lower and optically thinner than subtropical cirrus clouds. The dependence of cirrus cloud geometrical thickness and optical properties on mid-cirrus temperatures shows a quite similar tendency for the three sites but less variability for the subarctic dataset. Cirrus clouds are geometrically and optically thicker at temperatures between −45 and −35 ∘C, and a second peak is observed at lower temperatures ∼-70 ∘C for the subarctic site. Lidar ratio values also exhibit a pattern, showing higher values moving toward the poles, with higher mean values observed over the subarctic site. The dependency of the mid-cirrus temperatures on the lidar ratio values and the particle depolarisation values is further examined. Our study shows that the highest values of the cirrus lidar ratio correspond to higher values of cirrus depolarisation and warmer cirrus. The kind of information presented here can be rather useful in the cirrus parameterisations required as input to radiative transfer models and can be a complementary tool for satellite products that cannot provide cloud vertical structure. In addition, ground-based statistics of the cirrus properties could be useful in the validation and improvement of the corresponding derived products from satellite retrievals.

This research was part of the Salutary Umeå Study of Aerosols in Biomass Cookstove Emissions (SUSTAINE) laboratory experiment campaign. We studied ice-nucleating abilities of particulate emissions from solid-fuel-burning cookstoves, using a portable ice nuclei counter, Spectrometer Ice Nuclei (SPIN). These emissions were generated from two traditional cookstove types commonly used for household cooking in sub-Saharan Africa and two advanced gasifier stoves under research to promote sustainable development alternatives. The solid fuels studied included biomass from two different African tree species, Swedish softwood and agricultural residue products relevant to the region. Measurements were performed with a modified version of the standard water boiling test on polydisperse samples from flue gas during burning and size-selected accumulation mode soot particles from a 15 m3 aerosol-storage chamber. The studied soot particle sizes in nanometers were 250, 260, 300, 350, 400, 450 and 500. From this chamber, the particles were introduced to water-supersaturated freezing conditions (−32 to −43 ∘C) in the SPIN. Accumulation mode soot particles generally produced an ice-activated fraction of 10−3 in temperatures 1–1.5 ∘C higher than that required for homogeneous freezing at fixed RHw=115 %. In five special experiments, the combustion performance of one cookstove was intentionally modified. Two of these exhibited a significant increase in the ice-nucleating ability of the particles, resulting in a 10−3 ice activation at temperatures up to 5.9 ∘C higher than homogeneous freezing and the observed increased ice-nucleating ability. We investigated six different physico-chemical properties of the emission particles but found no clear correlation between them and increasing ice-nucleating ability. We conclude that the freshly emitted combustion aerosols form ice via immersion and condensation freezing at temperatures only moderately above homogeneous freezing conditions.

A new method, called ElEx (elastic extinction), is proposed for the estimation of extinction coefficient lidar profiles using only the information provided by the elastic and polarization channels of a lidar system. The method is applicable to lidar measurements both during daytime and nighttime under well-defined aerosol mixtures. ElEx uses the particle backscatter profiles at 532 nm and the vertically resolved particle linear depolarization ratio measurements at the same wavelength. The particle linear depolarization ratio and the lidar ratio values of pure aerosol types are also taken from literature. The total extinction profile is then estimated and compared well with Raman retrievals. In this study, ElEx was applied in an aerosol mixture of marine and dust particles at Finokalia station during the CHARADMExp campaign. Any difference between ElEx and Raman extinction profiles indicates that the nondust component could be probably attributed to polluted marine or polluted continental aerosols. Comparison with sun photometer aerosol optical depth observations is performed as well during daytime. Differences in the total aerosol optical depth are varying between 1.2 % and 72 %, and these differences are attributed to the limited ability of the lidar to correctly represent the aerosol optical properties in the near range due to the overlap problem.

We present the results of birch pollen characterization using lidar and in situ measurements based on a 11 d pollination period from 5 to 15 May 2016 at the European Aerosol Research Lidar Network (EARLINET) station in Vehmasmäki (Kuopio; 62∘44′ N, 27∘33′ E), Finland. The ground-based multiwavelength Raman polarization lidar PollyXT performed continuous measurements at this rural forest site and has been combined with a Hirst-type volumetric air sampler, which measured the pollen type and concentration at roof level (4 m). The period was separated into two parts due to different atmospheric conditions and detected pollen types. During the first period, high concentrations of birch pollen were measured with a maximum 2 h average pollen concentration of 3700 grains m−3. Other pollen types represented less than 3 % of the total pollen count. In observed pollen layers, the mean particle depolarization ratio at 532 nm was 10±6 % during the intense birch pollination period. Mean lidar ratios were found to be 45±7 and 55±16 sr at 355 and 532 nm, respectively. During the second period, birch pollen was still dominant, but a significant contribution of spruce pollen was observed as well. Spruce pollen grains are highly nonspherical, leading to a larger mean depolarization ratio of 26±7 % for the birch–spruce pollen mixture. Furthermore, higher lidar ratios were observed during this period with mean values of 60±3 and 62±10 sr at 355 and 532 nm, respectively. The presented study shows the potential of the particle depolarization ratio to track pollen grains in the atmosphere.

The Mineral Aerosol Profiling from Infrared Radiances (MAPIR) algorithm retrieves vertical dust concentration profiles from cloud-free Infrared Atmospheric Sounding Interferometer (IASI) thermal infrared (TIR) radiances using Rodgers' optimal estimation method (OEM). We describe the new version 4.1 and evaluation results. Main differences with respect to previous versions are the Levenberg–Marquardt modification of the OEM, the use of the logarithm of the concentration in the retrieval and the use of Radiative Transfer for TOVS (RTTOV) for in-line radiative transfer calculations. The dust aerosol concentrations are retrieved in seven 1 km thick layers centered at 0.5 to 6.5 km. A global data set of the daily dust distribution was generated with MAPIR v4.1 covering September 2007 to June 2018, with further extensions planned every 6 months. The post-retrieval quality filters reject about 16 % of the retrievals, a huge improvement with respect to the previous versions in which up to 40 % of the retrievals were of bad quality. The median difference between the observed and fitted spectra of the good-quality retrievals is 0.32 K, with lower values over oceans. The information content of the retrieved profiles shows a dependence on the total aerosol load due to the assumption of a lognormal state vector. The median degrees of freedom in dusty scenes (min 10 µm AOD of 0.5) is 1.4. An evaluation of the aerosol optical depth (AOD) obtained from the integrated MAPIR v4.1 profiles was performed against 72 AErosol RObotic NETwork (AERONET) stations. The MAPIR AOD correlates well with the ground-based data, with a mean correlation coefficient of 0.66 and values as high as 0.88. Overall, there is a mean AOD (550 nm) positive bias of only 0.04 with respect to AERONET, which is an extremely good result. The previous versions of MAPIR were known to largely overestimate AOD (about 0.28 for v3). A second evaluation exercise was performed comparing the mean aerosol layer altitude from MAPIR with the mean dust altitude from Cloud–Aerosol LIdar with Orthogonal Polarization (CALIOP). A small underestimation was found, with a mean difference of about 350 m (standard deviation of about 1 km) with respect to the CALIOP cumulative extinction altitude, which is again considered very good as the vertical resolution of MAPIR is 1 km. In the comparisons against AERONET and CALIOP, a dependence of MAPIR on the quality of the temperature profiles used in the retrieval is observed. Finally, a qualitative comparison of dust aerosol concentration profiles was done against lidar measurements from two ground-based stations (M'Bour and Al Dhaid) and from the Cloud–Aerosol Transport System (CATS) instrument on board the International Space Station (ISS). MAPIR v4.1 showed the ability to detect dust plumes at the same time and with a similar extent as the lidar instruments. This new MAPIR version shows a great improvement of the accuracy of the aerosol profile retrievals with respect to previous versions, especially so for the integrated AOD. It now offers a unique 3-D dust data set, which can be used to gain more insight into the transport and emission processes of mineral dust aerosols.

In this work, the height of the planetary boundary layer (PBLH) is investigated over Gwal Pahari (Gual Pahari), New Delhi, for almost a year. To this end, ground-based measurements from a multiwavelength Raman lidar were used. The modified wavelet covariance transform (WCT) method was utilized for PBLH retrievals. Results were compared to data from Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) and the Weather Research and Forecasting (WRF) model. In order to examine the difficulties of PBLH detection from lidar, we analyzed three cases of PBLH diurnal evolution under different meteorological and aerosol load conditions. In the presence of multiple aerosol layers, the employed algorithm exhibited high efficiency (r=0.9) in the attribution of PBLH, whereas weak aerosol gradients induced high variability in the PBLH. A sensitivity analysis corroborated the stability of the utilized methodology. The comparison with CALIPSO observations yielded satisfying results (r=0.8), with CALIPSO slightly overestimating the PBLH. Due to the relatively warmer and drier winter and, correspondingly, colder and rainier pre-monsoon season, the seasonal PBLH cycle during the measurement period was slightly weaker than the cycle expected from long-term climate records.

The formation rates of 3 nm particles were estimated at SMEAR IV, Puijo (Finland), where the continuous measurements extend only down to 7 nm in diameter. We extrapolated the formation rates at 7 nm (J7) down to 3 nm (J3) based on an approximate solution to the aerosol general dynamic equation, assuming a constant condensational growth rate, a power-law size-dependent scavenging rate, and negligible self-coagulation rate for the nucleation mode particles. To evaluate our method, we first applied it to new particle formation (NPF) events in Hyytiälä (Finland), which extend down to 3 nm, and, therefore, J3 and J7 can be determined directly from the measured size distribution evolution. The Hyytiälä results show that the estimated daily mean J3 values slightly overestimate the observed mean J3, but a promising 91 % of the estimated J3 values are within a factor of 2 from the measured ones. However, when considering detailed daily time evolution, the agreement is not as good due to fluctuations in data as well as uncertainties in estimated growth rates, which are required in order to calculate the time lag between formation of 3 and 7 nm particles. At Puijo, the mean J7 for clear NPF days during April 2007–December 2015 was 0.44 cm−3 s−1, while the extrapolated mean J3 was 0.61 cm−3 s−1.

We present tropospheric water vapor profiles measured with a Raman lidar during three field campaigns held in Finland. Co-located radio soundings are available throughout the period for the calibration of the lidar signals. We investigate the possibility of calibrating the lidar water vapor profiles in the absence of co-existing on-site soundings using water vapor profiles from the combined Advanced InfraRed Sounder (AIRS) and the Advanced Microwave Sounding Unit (AMSU) satellite product; the Aire Limitée Adaptation dynamique Développement INternational and High Resolution Limited Area Model (ALADIN/HIRLAM) numerical weather prediction (NWP) system, and the nearest radio sounding station located 100 km away from the lidar site (only for the permanent location of the lidar). The uncertainties of the calibration factor derived from the soundings, the satellite and the model data are −1); during summer it is wet (5.54±1.02 g kg−1); and at other times, the air is in an intermediate state. These are averaged values over the lowest 2 km in the atmosphere. Above that height a quick decrease in water vapor mixing ratios is observed, except during summer months where favorable atmospheric conditions enable higher mixing ratio values at higher altitudes. Lastly, the seasonal change in disagreement between the lidar and the model has been studied. The analysis showed that, on average, the model underestimates water vapor mixing ratios at high altitudes during spring and summer.

Long-term in situ measurements of aerosol–cloud interactions are usually performed in measurement stations residing on hills, mountains, or high towers. In such conditions, the surface topography of the surrounding area can affect the measured cloud droplet distributions by increasing turbulence or causing orographic flows and thus the observations might not be representative for a larger scale. The objective of this work is to analyse, how the local topography affects the observations at Puijo measurement station, which is located in the 75 m high Puijo tower, which itself stands on a 150 m high hill. The analysis of the measurement data shows that the observed cloud droplet number concentration mainly depends on the cloud condensation nuclei (CCN) concentration. However, when the wind direction aligns with the direction of the steepest slope of the hill, a clear topography effect is observed. This finding was further analysed by simulating 3-D flow fields around the station and by performing trajectory ensemble modelling of aerosol- and wind-dependent cloud droplet formation. The results showed that in typical conditions, with geostrophic winds of about 10 m s−1, the hill can cause updrafts of up to 1 m s−1 in the air parcels arriving at the station. This is enough to produce in-cloud supersaturations (SSs) higher than typically found at the cloud base of ∼ 0.2 %), and thus additional cloud droplets may form inside the cloud. In the observations, this is seen in the form of a bimodal cloud droplet size distribution. The effect is strongest with high winds across the steepest slope of the hill and with low liquid water contents, and its relative importance quickly decreases as these conditions are relaxed. We therefore conclude that, after careful screening for wind speed and liquid water content, the observations at Puijo measurement station can be considered representative for clouds in a boreal environment.

Organic aerosols (OA) derived from small-scale wood combustion emissions are not well represented by current emissions inventories and models, although they contribute substantially to the atmospheric particulate matter (PM) levels. In this work, a 29 m3 smog chamber in the ILMARI facility of the University of Eastern Finland was utilized to investigate the formation of secondary organic aerosol (SOA) from a small-scale modern masonry heater commonly used in northern Europe. Emissions were oxidatively aged in the smog chamber for a variety of dark (i.e., O3 and NO3) and UV (i.e., OH) conditions, with OH concentration levels of (0.5–5) × 106 molecules cm−3, achieving equivalent atmospheric aging of up to 18 h. An aerosol mass spectrometer characterized the direct OA emissions and the SOA formed from the combustion of three wood species (birch, beech and spruce) using two ignition processes (fast ignition with a VOC-to-NOx ratio of 3 and slow ignition with a ratio of 5).Dark and UV aging increased the SOA mass fraction with average SOA productions 2.0 times the initial OA mass loadings. SOA enhancement was found to be higher for the slow ignition compared with fast ignition conditions. Positive matrix factorization (PMF) was used to separate SOA, primary organic aerosol (POA) and their subgroups from the total OA mass spectra. PMF analysis identified two POA and three SOA factors that correlated with the three major oxidizers: ozone, the nitrate radical and the OH radical. Organonitrates (ONs) were observed to be emitted directly from the wood combustion and additionally formed during oxidation via NO3 radicals (dark aging), suggesting small-scale wood combustion may be a significant ON source. POA was oxidized after the ozone addition, forming aged POA, and after 7 h of aging more than 75 % of the original POA was transformed. This process may involve evaporation and homogeneous gas-phase oxidation as well as heterogeneous oxidation of particulate organic matter. The results generally prove that logwood burning emissions are the subject of intensive chemical processing in the atmosphere, and the timescale for these transformations is relatively short, i.e., hours.

The relationship between aerosol hygroscopicity and cloud droplet activation was studied at the Puijo measurement station in Kuopio, Finland, during the autumn 2014. The hygroscopic growth of 80, 120 and 150 nm particles was measured at 90 % relative humidity with a hygroscopic tandem differential mobility analyzer. Typically, the growth factor (GF) distributions appeared bimodal with clearly distinguishable peaks around 1.0–1.1 and 1.4–1.6. However, the relative contribution of the two modes appeared highly variable reflecting the probable presence of fresh anthropogenic particle emissions. The hygroscopicity-dependent activation properties were estimated in a case study comprising four separate cloud events with varying characteristics. At 120 and 150 nm, the activation efficiencies within the low- and high-GF modes varied between 0–34 and 57–83 %, respectively, indicating that the less hygroscopic particles remained mostly non-activated, whereas the more hygroscopic mode was predominantly scavenged into cloud droplets. By modifying the measured GF distributions, it was estimated how the cloud droplet concentrations would change if all the particles belonged to the more hygroscopic group. According to κ-Köhler simulations, the cloud droplet concentrations increased up to 70 % when the possible feedback effects on effective peak supersaturation (between 0.16 and 0.29 %) were assumed negligible. This is an indirect but clear illustration of the sensitivity of cloud formation to aerosol chemical composition.

Optical and microphysical properties of different aerosol types over South Africa measured with a multi-wavelength polarization Raman lidar are presented. This study could assist in bridging existing gaps relating to aerosol properties over South Africa, since limited long-term data of this type are available for this region. The observations were performed under the framework of the EUCAARI campaign in Elandsfontein. The multi-wavelength PollyXT Raman lidar system was used to determine vertical profiles of the aerosol optical properties, i.e. extinction and backscatter coefficients, Ångström exponents, lidar ratio and depolarization ratio. The mean microphysical aerosol properties, i.e. effective radius and single-scattering albedo, were retrieved with an advanced inversion algorithm. Clear differences were observed for the intensive optical properties of atmospheric layers of biomass burning and urban/industrial aerosols. Our results reveal a wide range of optical and microphysical parameters for biomass burning aerosols. This indicates probable mixing of biomass burning aerosols with desert dust particles, as well as the possible continuous influence of urban/industrial aerosol load in the region. The lidar ratio at 355 nm, the lidar ratio at 532 nm, the linear particle depolarization ratio at 355 nm and the extinction-related Ångström exponent from 355 to 532 nm were 52 ± 7 sr, 41 ± 13 sr, 0.9 ± 0.4 % and 2.3 ± 0.5, respectively, for urban/industrial aerosols, while these values were 92 ± 10 sr, 75 ± 14 sr, 3.2 ± 1.3 % and 1.7 ± 0.3, respectively, for biomass burning aerosol layers. Biomass burning particles are larger and slightly less absorbing compared to urban/industrial aerosols. The particle effective radius were found to be 0.10 ± 0.03, 0.17 ± 0.04 and 0.13 ± 0.03 µm for urban/industrial, biomass burning, and mixed aerosols, respectively, while the single-scattering albedo at 532 nm was 0.87 ± 0.06, 0.90 ± 0.06, and 0.88 ± 0.07 (at 532 nm), respectively, for these three types of aerosols. Our results were within the same range of previously reported values.

The atmospheric science community demands autonomous and quality-assured vertically resolved measurements of aerosol and cloud properties. For this purpose, a portable lidar called Polly was developed at TROPOS in 2003. The lidar system was continuously improved with gained experience from the EARLINET community, involvement in worldwide field campaigns, and international institute collaborations within the last 10 years. Here we present recent changes of the setup of the portable multiwavelength Raman and polarization lidar PollyXT and discuss the improved capabilities of the system by means of a case study. The latest system developments include an additional near-range receiver unit for Raman measurements of the backscatter and extinction coefficient down to 120 m above ground, a water-vapor channel, and channels for simultaneous measurements of the particle linear depolarization ratio at 355 and 532 nm. Quality improvements were achieved by systematically following the EARLINET guidelines and the international PollyNET quality assurance developments. A modified ship radar ensures measurements in agreement with air-traffic safety regulations and allows for 24∕7 monitoring of the atmospheric state with PollyXT.

A global vertically resolved aerosol data set covering more than 10 years of observations at more than 20 measurement sites distributed from 63° N to 52° S and 72° W to 124° E has been achieved within the Raman and polarization lidar network PollyNET. This network consists of portable, remote-controlled multiwavelength-polarization-Raman lidars (Polly) for automated and continuous 24/7 observations of clouds and aerosols. PollyNET is an independent, voluntary, and scientific network. All Polly lidars feature a standardized instrument design with different capabilities ranging from single wavelength to multiwavelength systems, and now apply unified calibration, quality control, and data analysis. The observations are processed in near-real time without manual intervention, and are presented online at http://polly.tropos.de/. The paper gives an overview of the observations on four continents and two research vessels obtained with eight Polly systems. The specific aerosol types at these locations (mineral dust, smoke, dust-smoke and other dusty mixtures, urban haze, and volcanic ash) are identified by their Ångström exponent, lidar ratio, and depolarization ratio. The vertical aerosol distribution at the PollyNET locations is discussed on the basis of more than 55 000 automatically retrieved 30 min particle backscatter coefficient profiles at 532 nm as this operating wavelength is available for all Polly lidar systems. A seasonal analysis of measurements at selected sites revealed typical and extraordinary aerosol conditions as well as seasonal differences. These studies show the potential of PollyNET to support the establishment of a global aerosol climatology that covers the entire troposphere.

Ambient aerosol particles can take up water and thus change their optical properties depending on the hygroscopicity and the relative humidity (RH) of the surrounding air. Knowledge of the hygroscopicity effect is of crucial importance for radiative forcing calculations and is also needed for the comparison or validation of remote sensing or model results with in situ measurements. Specifically, particle light scattering depends on RH and can be described by the scattering enhancement factor f(RH), which is defined as the particle light scattering coefficient at defined RH divided by its dry value (RH Here, we present results of an intensive field campaign carried out in summer 2013 at the SMEAR II station at Hyytiälä, Finland. Ground-based and airborne measurements of aerosol optical, chemical and microphysical properties were conducted. The f(RH) measured at ground level by a humidified nephelometer is found to be generally lower (e.g. 1.63±0.22 at RH = 85 % and λ = 525 nm) than observed at other European sites. One reason is the high organic mass fraction of the aerosol encountered at Hyytiälä to which f(RH) is clearly anti-correlated (R2≈0.8). A simplified parametrization of f(RH) based on the measured chemical mass fraction can therefore be derived for this aerosol type. A trajectory analysis revealed that elevated values of f(RH) and the corresponding elevated inorganic mass fraction are partially caused by transported hygroscopic sea spray particles. An optical closure study shows the consistency of the ground-based in situ measurements. Our measurements allow to determine the ambient particle light extinction coefficient using the measured f(RH). By combining the ground-based measurements with intensive aircraft measurements of the particle number size distribution and ambient RH, columnar values of the particle extinction coefficient are determined and compared to columnar measurements of a co-located AERONET sun photometer. The water uptake is found to be of minor importance for the column-averaged properties due to the low particle hygroscopicity and the low RH during the daytime of the summer months. The in situ derived aerosol optical depths (AOD) clearly correlate with directly measured values of the sun photometer but are substantially lower compared to the directly measured values (factor of ~ 2–3). The comparison degrades for longer wavelengths. The disagreement between in situ derived and directly measured AOD is hypothesized to originate from losses of coarse and fine mode particles through dry deposition within the canopy and losses in the in situ sampling lines. In addition, elevated aerosol layers (above 3 km) from long-range transport were observed using an aerosol lidar at Kuopio, Finland, about 200 km east-north-east of Hyytiälä. These elevated layers further explain parts of the disagreement.

A 29 m3 Teflon chamber, designed for studies on the aging of combustion aerosols, at the University of Eastern Finland is described and characterized. The chamber is part of a research facility, called Ilmari, where small-scale combustion devices, a dynamometer for vehicle exhaust studies, dilution systems, the chamber, and cell and animal exposure devices are located side by side under the same roof. The small surface-to-volume ratio of the chamber enables reasonably long experiment times, with particle wall loss rate constants of 0.088, 0.080, 0.045, and 0.040 h−1 for polydisperse, 50, 100, and 200 nm monodisperse aerosols, respectively. The NO2 photolysis rate can be adjusted from 0 to 0.62 min−1. The irradiance spectrum is centered at either 350 or 365 nm, and the maximum irradiance, produced by up to 160 blacklight lamps, is 29.7 W m−2, which corresponds to the ultraviolet (UV) irradiance in Central Finland at noon on a sunny day in the midsummer. The temperature inside the chamber is uniform and can be kept at 25±1 °C. The chamber is kept in an overpressure with a moving top frame, which reduces sample dilution and entrance of contamination during an experiment. The functionality of the chamber was tested with oxidation experiments of toluene, resulting in secondary organic aerosol (SOA) yields of 12–42%, depending on the initial conditions, such as NOx concentration and UV irradiation. The highest gaseous oxidation product yields of 12.4–19.5% and 5.8–19.5% were detected with ions corresponding to methyl glyoxal (m/z 73.029) and 4-oxo-2-pentenal (m/z 99.044), respectively. Overall, reasonable yields of SOA and gaseous reaction products, comparable to those obtained in other laboratories, were obtained.

Raman lidar data obtained over a 1 year period has been analysed in relation to aerosol layers in the free troposphere over the Highveld in South Africa. In total, 375 layers were observed above the boundary layer during the period 30 January 2010 to 31 January 2011. The seasonal behaviour of aerosol layer geometrical characteristics, as well as intensive and extensive optical properties were studied. The highest centre heights of free-tropospheric layers were observed during the South African spring (2520 ± 970 m a.g.l., also elsewhere). The geometrical layer depth was found to be maximum during spring, while it did not show any significant difference for the rest of the seasons. The variability of the analysed intensive and extensive optical properties was high during all seasons. Layers were observed at a mean centre height of 2100 ± 1000 m with an average lidar ratio of 67 ± 25 sr (mean value with 1 standard deviation) at 355 nm and a mean extinction-related Ångström exponent of 1.9 ± 0.8 between 355 and 532 nm during the period under study. Except for the intensive biomass burning period from August to October, the lidar ratios and Ångström exponents are within the range of previous observations for urban/industrial aerosols. During Southern Hemispheric spring, the biomass burning activity is clearly reflected in the optical properties of the observed free-tropospheric layers. Specifically, lidar ratios at 355 nm were 89 ± 21, 57 ± 20, 59 ± 22 and 65 ± 23 sr during spring (September–November), summer (December–February), autumn (March–May) and winter (June–August), respectively. The extinction-related Ångström exponents between 355 and 532 nm measured during spring, summer, autumn and winter were 1.8 ± 0.6, 2.4 ± 0.9, 1.8 ± 0.9 and 1.8 ± 0.6, respectively. The mean columnar aerosol optical depth (AOD) obtained from lidar measurements was found to be 0.46 ± 0.35 at 355 nm and 0.25 ± 0.2 at 532 nm. The contribution of free-tropospheric aerosols on the AOD had a wide range of values with a mean contribution of 46%.

The Puijo aerosol–cloud observation station is a unique measurement site for its location in the mixed region between the boreal forestland and the municipality of Kuopio, Finland. A measurement campaign was carried out at the station during fall 2010. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-Tof-AMS) was deployed to characterize the atmospheric submicron aerosols. Positive matrix factorization (PMF) was applied to the unified high-resolution mass spectra organic species with NO+ and NO2+ ions to discover the intrinsic relationships between the organic and inorganic species and their daily cycles. On average, the submicron aerosols in this study were dominated by organic and sulfate species, composing 48.2 and 28.7% of total observed aerosol mass, respectively, with smaller contributions from ammonium (9.3%), nitrate (4.9%), chloride (0.8%) and BC (8.1%). The sources of these species included the primary emissions originating from the city area, secondary formation from both natural and anthropogenic emissions and regional transport. The PMF analysis succeeded in separating the mixed organic and inorganic spectra into three distinct organic and one inorganic factors. For organic factors, the semi-volatile oxygenated organic aerosol (SVOOA) and low-volatility oxygenated OA (LVOOA) accounted for 54.8 and 36.3% of total organic masses, respectively, while the hydrocarbon-like organic aerosol (HOA) accounted for 8.9% of total organics, with its main source from urban emissions. The inorganic factor is identified as NH4NO3, comprising 6.9% of the fitted aerosol mass by PMF. Based on the PMF results, the nitrate species were separated into organic and inorganic components, with the organic nitrates contributing one-third of the total nitrate mass. The results highlight both anthropogenic and biogenic emissions as important atmospheric aerosol sources in a forest–urban mixed region.

The aerosol direct radiative effect (ADRE) is defined as the change in the solar radiation flux, F, due to aerosol scattering and absorption. The difficulty in determining ADRE stems mainly from the need to estimate F without aerosols, F0, with either radiative transfer modeling and knowledge of the atmospheric state, or regression analysis of radiation data down to zero aerosol optical depth (AOD), if only F and AOD are observed. This paper examines the regression analysis method by using modeled surface data products provided by the Aerosol Robotic Network (AERONET). We extrapolated F0 by two functions: a straight linear line and an exponential nonlinear decay. The exponential decay regression is expected to give a better estimation of ADRE with a few percent larger extrapolated F0 than the linear regression. We found that, contrary to the expectation, in most cases the linear regression gives better results than the nonlinear. In such cases the extrapolated F0 represents an unrealistically low water vapor column (WVC), resulting in underestimation of attenuation caused by the water vapor, and hence too large F0 and overestimation of the magnitude of ADRE. The nonlinear ADRE is generally 40–50% larger in magnitude than the linear ADRE due to the extrapolated F0 difference. Since for a majority of locations, AOD and WVC have a positive correlation, the extrapolated F0 with the nonlinear regression fit represents an unrealistically low WVC, and hence too large F0. The systematic underestimation of F0 with the linear regression is compensated by the positive correlation between AOD and water vapor, providing the better result.

Interactions between aerosols and liquid water clouds were studied during autumns 2010–2011 at a semiurban measurement station on Puijo tower in Kuopio, Finland. Cloud interstitial and total aerosol size distributions, particle chemical composition and hygroscopicity and cloud droplet size distribution were measured, with a focus on comparing clean air masses with those affected by local sources. On average, the polluted air contained more particles than the clean air masses, and generally the concentrations decreased during cloud events. Cloud processing was found to take place, especially in the clean air masses, and to a lesser extent in the polluted air. Some, mostly minor, differences in the average particle chemical composition between the air masses were observed. The average size and number concentration of activating particles were quite similar for both air masses, producing average droplet populations with only minor distinctions. As a case study, a long cloud event was analyzed in detail, with a special focus on the emissions from local sources, including a paper mill and a heating plant. This revealed larger variations in particle and cloud properties than the analysis of the whole data set. Clear differences in the total (between 214 and 2200 cm−3) and accumulation mode particle concentrations (between 62 and 169 cm−3) were observed. Particle chemical composition, especially the concentrations of organics (between 0.42 and 1.28 μg m−3) and sulfate (between 0.16 and 4.43 μg m−3), varied considerably. This affected the hygroscopic growth factor: for example, for 100 nm particles the range was from 1.21 to 1.45 at 90% relative humidity. Particularly, large particles, high hygroscopicities and elevated amounts of inorganics were linked with the pollutant plumes. Moreover, the particle hygroscopicity distributions in the polluted air were clearly bimodal, indicating externally mixed aerosol. The variable conditions also had an impact on cloud droplet formation, with the droplet concentration varying between 138 and 240 cm−3 and mean diameter between 9.2 and 12.4 μm.

The Finnish Meteorological Institute, in collaboration with the University of Helsinki, has established a new ground-based remote-sensing network in Finland. The network consists of five topographically, ecologically and climatically different sites distributed from southern to northern Finland. The main goal of the network is to monitor air pollution and boundary layer properties in near real time, with a Doppler lidar and ceilometer at each site. In addition to these operational tasks, two sites are members of the Aerosols, Clouds and Trace gases Research InfraStructure Network (ACTRIS); a Ka band cloud radar at Sodankylä will provide cloud retrievals within CloudNet, and a multi-wavelength Raman lidar, PollyXT (POrtabLe Lidar sYstem eXTended), in Kuopio provides optical and microphysical aerosol properties through EARLINET (the European Aerosol Research Lidar Network). Three C-band weather radars are located in the Helsinki metropolitan area and are deployed for operational and research applications. We performed two inter-comparison campaigns to investigate the Doppler lidar performance, compare the backscatter signal and wind profiles, and to optimize the lidar sensitivity through adjusting the telescope focus length and data-integration time to ensure sufficient signal-to-noise ratio (SNR) in low-aerosol-content environments. In terms of statistical characterization, the wind-profile comparison showed good agreement between different lidars. Initially, there was a discrepancy in the SNR and attenuated backscatter coefficient profiles which arose from an incorrectly reported telescope focus setting from one instrument, together with the need to calibrate. After diagnosing the true telescope focus length, calculating a new attenuated backscatter coefficient profile with the new telescope function and taking into account calibration, the resulting attenuated backscatter profiles all showed good agreement with each other. It was thought that harsh Finnish winters could pose problems, but, due to the built-in heating systems, low ambient temperatures had no, or only a minor, impact on the lidar operation – including scanning-head motion. However, accumulation of snow and ice on the lens has been observed, which can lead to the formation of a water/ice layer thus attenuating the signal inconsistently. Thus, care must be taken to ensure continuous snow removal.

Atmospheric lidar measurements were carried out at Elandsfontein measurement station, on the eastern Highveld approximately 150 km east of Johannesburg in South Africa throughout 2010. The height of the planetary boundary layer (PBL) top was continuously measured using a Raman lidar, PollyXT (POrtabLe Lidar sYstem eXTended). High atmospheric variability together with a large surface temperature range and significant seasonal changes in precipitation were observed, which had an impact on the vertical mixing of particulate matter, and hence, on the PBL evolution. The results were compared to radiosondes, CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) space-borne lidar measurements and three atmospheric models that followed different approaches to determine the PBL top height. These models included two weather forecast models operated by ECMWF (European Centre for Medium-range Weather Forecasts) and SAWS (South African Weather Service), and one mesoscale prognostic meteorological and air pollution regulatory model TAPM (The Air Pollution Model). The ground-based lidar used in this study was operational for 4935 h during 2010 (49% of the time). The PBL top height was detected 86% of the total measurement time (42% of the total time). Large seasonal and diurnal variations were observed between the different methods utilised. High variation was found when lidar measurements were compared to radiosonde measurements. This could be partially due to the distance between the lidar measurements and the radiosondes, which were 120 km apart. Comparison of lidar measurements to the models indicated that the ECMWF model agreed the best with mean relative difference of 15.4%, while the second best correlation was with the SAWS model with corresponding difference of 20.1%. TAPM was found to have a tendency to underestimate the PBL top height. The wind speeds in the SAWS and TAPM models were strongly underestimated which probably led to underestimation of the vertical wind and turbulence and thus underestimation of the PBL top height. Comparison between ground-based and satellite lidar shows good agreement with a correlation coefficient of 0.88. On average, the daily maximum PBL top height in October (spring) and June (winter) was 2260 m and 1480 m, respectively. To our knowledge, this study is the first long-term study of PBL top heights and PBL growth rates in South Africa.

Concurrent measurement of aerosols, cloud condensation nuclei (CCN) and cloud droplet activation were carried out as a part of the third Pallas Cloud Experiment (PaCE-3) which took place at a ground based site located on northern Finland during the autumn of 2009. In this study, we investigate relationships between the aerosol properties, CCN and size resolved cloud droplet activation. During the investigated cloudy periods, the inferred number of cloud droplets (CDNC) varied typically between 50 and 150 cm−3 and displayed a linear correlation both with the number of particles having sizes over 100 nm and with the CCN concentrations at 0.4% supersaturation. Furthermore, the diameter corresponding to the 50% activation fraction, D50, was generally in the range of 80 to 120 nm. The measured CCN concentrations were compared with predictions of a numerical model which used the measured size distribution and size resolved hygroscopicity as input. Assuming that the droplet surface tension is equal to that of water, the measured and predicted CCN concentrations were generally within 30%. We also simulated size dependent cloud droplet activation with a previously developed air parcel model. By forcing the model to reproduce the experimental values of CDNC, adiabatic estimates for the updraft velocity and the maximum supersaturation reached in the clouds were derived. Performed sensitivity studies showed further that the observed variability in CDNC was driven mainly by changes in the particle size distribution while the variations in the updraft velocity and hygroscopicity contributed to a lesser extent. The results of the study corroborate conclusions of previous studies according to which the number of cloud droplets formed in clean air masses close to the Arctic is determined mainly by the number of available CCN.

We introduce a four-year (in 2006–2010) continuous data set of aerosol optical properties at Puijo in Kuopio, Finland. We study the annual and diurnal variation of the aerosol scattering and absorption coefficients, hemispheric backscattering fraction, scattering Ångström exponent, and single scattering albedo, whose median values over this period were 7.2 Mm−1 (at 550 nm), 1.0 Mm−1 (at 637 nm), 0.15, 1.93 (between 450 and 550 nm), and 0.85, respectively. The scattering coefficient peaked in the spring and autumn, being 2–4 times those in the summer and winter. An exception was the summer of 2010, when the scattering coefficient was elevated to ~300 Mm−1 by plumes from forest fires in Russia. The absorption coefficient peaked in the winter when soot-containing particles derived from biomass burning were present. The higher relative absorption coefficients resulted in lower single scattering albedo in winter. The optical properties varied also with wind direction and time of the day, indicating the effect of the local pollutant sources and the age of the particles. Peak values in the single scattering albedo were observed when the wind blew from a paper mill and from the sector without local pollutant sources. These observations were linked, respectively, to the sulphate-rich aerosol from the paper mill and the oxygenated organics in the aged aerosol, which both are known to increase the scattering characteristics of aerosols. Decreases in the single scattering albedo in the morning and afternoon, distinct in the summertime, were linked to the increased traffic density at these hours. The scattering and absorption coefficients of residential and long-range transported aerosol (two separate cloud events) were found to be decreased by clouds. The effect was stronger for the scattering than absorption, indicating preferential activation of the more hygroscopic aerosol with higher scattering characteristics.

One year of multi-wavelength (3 backscatter + 2 extinction + 1 depolarization) Raman lidar measurements at Gual Pahari, close to New Delhi, were analysed. The data was split into four seasons: spring (March–May), summer (June–August), autumn (September–November) and winter (December–February). The vertical profiles of backscatter, extinction, and lidar ratio and their variability during each season are presented. The measurements revealed that, on average, the aerosol layer was at its highest in spring (5.5 km). In summer, the vertically averaged (between 1–3 km) backscatter and extinction coefficients had the highest averages (3.3 Mm−1 sr−1 and 142 Mm−1 at 532 nm, respectively). Aerosol concentrations were slightly higher in summer compared to other seasons, and particles were larger in size. The autumn showed the highest lidar ratio and high extinction-related Ångström exponents (AEext), indicating the presence of smaller probably absorbing particles. The winter had the lowest backscatter and extinction coefficients, but AEext was the highest, suggesting still a large amount of small particles.

In this paper we introduce new in situ observations of atmospheric aerosols, especially chemical composition, physical and optical properties, on the eastern brink of the heavily polluted Highveld area in South Africa. During the observation period between 11 February 2009 and 31 January 2011, the mean particle number concentration (size range 10–840 nm) was 6310 cm3 and the estimated volume of sub-10 μm particles 9.3 μm3 m−3. The aerosol absorption and scattering coefficients at 637 nm were 8.3 Mm−1 and 49.5 Mm−1, respectively. The mean single-scattering albedo at 637 nm was 0.84 and the Ångström exponent of scattering was 1.5 over the wavelength range 450–635 nm. The mean O3, SO2, NOx and H2S-concentrations were 37.1, 11.5, 15.1 and 3.2 ppb, respectively. The observed range of concentrations was large and attributed to the seasonal variation of sources and regional meteorological effects, especially the anticyclonic re-circulation and strong winter-time inversions. In a global context, the levels of gases and particulates were typical for continental sites with strong anthropogenic influence, but clearly lower than the most polluted areas of south-eastern Asia. Of all pollutants observed at the site, ozone is the most likely to have adverse environmental effects, as the concentrations were high also during the growing season. The measurements presented here will help to close existing gaps in the ground-based global atmosphere observation system, since very little long-term data of this nature is available for southern Africa.

In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several new aerosol parameterizations and computations modules for chemical transport and global climate models were developed and evaluated. These achievements and related studies have substantially improved our understanding and reduced the uncertainties of aerosol radiative forcing and air quality-climate interactions. The EUCAARI results can be utilized in European and global environmental policy to assess the aerosol impacts and the corresponding abatement strategies.

Secondary new particle formation affects atmospheric aerosol and cloud droplet numbers and thereby, the aerosol effects on climate. In this paper, the frequency of nucleation events and the associated particle formation and growth rates, along with their seasonal variation, was analysed based on over ten years of aerosol measurements conducted at the Pallas GAW station in northern Finland. The long-term measurements also allowed a detailed examination of factors possibly favouring or suppressing particle formation. Effects of meteorological parameters and air mass properties as well as vapour sources and sinks for particle formation frequency and event parameters were inspected. In addition, the potential of secondary particle formation to increase the concentration of cloud condensation nuclei (CCN) sized particles was examined. Findings from these long-term measurements confirmed previous observations: event frequency peaked in spring and the highest growth rates were observed in summer, affiliated with increased biogenic activity. Events were almost exclusively observed in marine air masses on sunny cloud-free days. A low vapour sink by the background particle population as well as an elevated sulphuric acid concentration were found to favour particle formation. These were also conditions taking place most likely in marine air masses. Inter-annual trend showed a minimum in event frequency in 2003, when also the smallest annual median of growth rate was observed. This gives further evidence of the importance and sensitivity of particle formation for the condensing vapour concentrations at Pallas site. The particle formation was observed to increase CCN80 (>80 nm particle number) concentrations especially in summer and autumn seasons when the growth rates were the highest. When the growing mode exceeded the selected 80 nm limit, on average in those cases, 211 ± 114% increase of CCN80 concentrations was observed.

Particulate matter (PM) and equivalent black carbon (BCe) concentrations were measured at two locations in northern India during 2006–2010. The first measurement station was a background site in Mukteshwar, about 350 km northeast of New Delhi, in the foothills of the Indian Himalayas. The second measurement site was located in Gual Pahari, about 25 km south of New Delhi. Here we focused on resolving the effects of the Indian summer monsoon on the particulate matter and equivalent black carbon concentrations at two stations. The average monsoon time concentrations were decreased by 55–70 % compared to the pre-monsoon average concentrations at both stations, decreasing as a function of the total local rainfall during the monsoon season. In Mukteshwar during the monsoon, the 24 h PM2.5 concentrations were nearly always below the Indian National Air Quality Standard of 60 μg m−3. In Gual Pahari, 13 % of days exceeded this level during the monsoon season. However, the 24 h guideline of 25 μg m−3 given by the World Health Organization was more difficult to meet. In addition to loss processes, aerosol concentrations during the early monsoon were found to be affected by primary emissions, most likely from dust events from the Thar Desert. This resulted in elevated fractions of the coarse mode, PM2.5–10 at both stations. In Mukteshwar, additional dust contribution came from east of the station, from the Himalayan region. We also determined the characteristic transition times between the pre-monsoon, monsoon and post-monsoon. The onset and withdrawal transitions occurred faster in Mukteshwar than in Gual Pahari, both being typically less than 10 days. Transition periods in Gual Pahari took between 17 and 31 days. The shorter transition times in Mukteshwar were probably related to the more intense rains due to the mountain location, and the fact that the station was most of the time in the free troposphere.

Aerosol physical and optical properties were measured at two locations in northern India. The first measurement station was a background site in Mukteshwar, about 350 km northeast of New Delhi, in the foothills of the Indian Himalayas, with data from 2006 to 2009. The second measurement site was located in Gual Pahari, about 25 km south of New Delhi, with data from 2008 to 2009. At both stations, the average aerosol concentrations during the monsoon were decreased by 40–75 % compared to the pre-monsoon average concentrations. The decrease varied with the total local rainfall. In Mukteshwar, the monsoon season removed particles from all size classes, due to a combination of rain scavenging and activation to cloud and mountain fog droplets. The scavenging by rain is least effective for the size range of the accumulation mode particles. In Gual Pahari, this was the only major wet removal mechanism and, as a result, the accumulation mode particles were less effectively removed. Aerosol concentrations during the early monsoon were found to be affected by mineral dust which in Gual Pahari was observed as an increased particle volume at a diameter around 3–4 μm. The single scattering albedo varied from 0.73 to 0.93 during the monsoon season, being slightly lower in Gual Pahari than in Mukteshwar. This is due to the fact that Gual Pahari resided closer to high anthropogenic black carbon emissions. As the absorbing particles are typically in the accumulation mode, they were not effectively removed by rain scavenging. The aerosol columnar properties, which were measured in Gual Pahari, showed a somewhat different seasonal behaviour compared to the surface measurements, with the aerosol optical depth increasing to an annual maximum in the early monsoon season.

A fraction of the Himalayan aerosols originate from secondary sources, which are currently poorly quantified. To clarify the climatic importance of regional secondary particle formation in the Himalayas, data from 2005 to 2010 of continuous aerosol measurements at a high-altitude (2180 m) Indian Himalayan site, Mukteshwar, were analyzed. For this period, the days were classified, and the particle formation and growth rates were calculated for clear new particle formation (NPF) event days. The NPF events showed a pronounced seasonal cycle. The frequency of the events peaked in spring, when the ratio between event and non-event days was 53 %, whereas the events were truly sporadic on any other seasons. The annual mean particle formation and growth rates were 0.40 cm−3 s−1 and 2.43 nm h−1, respectively. The clear annual cycle was found to be mainly controlled by the seasonal evolution of the Planetary Boundary Layer (PBL) height together with local meteorological conditions. Spring NPF events were connected with increased PBL height, and therefore characterised as boundary layer events, while the rare events in other seasons represented lower free tropospheric particle formation. This provides insight on the vertical extent of NPF in the atmosphere.