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This study presents results of direct observations of aerosol chemical composition in clouds. A high-resolution time-of-flight aerosol mass spectrometer was used to make measurements of cloud interstitial particles (INT) and mixed cloud interstitial and droplet residual particles (TOT). The differences between these two are the cloud droplet residuals (RES). Positive matrix factorization analysis of high-resolution mass spectral data sets and theoretical calculations were performed to yield distributions of chemical composition of the INT and RES particles. We observed that less oxidized hydrocarbon-like organic aerosols (HOA) were mainly distributed into the INT particles, whereas more oxidized low-volatile oxygenated OA (LVOOA) mainly in the RES particles. Nitrates existed as organic nitrate and in chemical form of NH(4)NO(3). Organic nitrates accounted for 45% of total nitrates in the INT particles, in clear contrast to 26% in the RES particles. Meanwhile, sulfates coexist in forms of acidic NH(4)HSO(4) and neutralized (NH(4))(2)SO(4). Acidic sulfate made up 64.8% of total sulfates in the INT particles, much higher than 10.7% in the RES particles. The results indicate a possible joint effect of activation ability of aerosol particles, cloud processing, and particle size effects on cloud formation.

Remote sensing has been a key resource for developing extensive and detailed datasets for studying and constraining aerosol-cloud-climate interactions. However, aerosol-cloud collocation challenges, algorithm limitations, as well as difficulties in unraveling dynamic from aerosol-related effects on cloud microphysics, have long challenged precise retrievals of cloud droplet number concentrations. By combining a series of remote sensing techniques and in situ measurements at ground level, we developed a semiautomated approach that can address several retrieval issues for a robust estimation of cloud droplet number for non-precipitating Planetary Boundary Layer (PBL) clouds. The approach is based on satellite retrievals of the PBL cloud droplet number (Ndsat) using the geostationary meteorological satellite data of the Optimal Cloud Analysis (OCA) product, which is obtained by the Spinning Enhanced Visible and InfraRed Imager (SEVIRI) of the European Organization for the Exploitation of Meteorological Satellites (EUMETSAT). The parameters of the retrieval are optimized through closure with droplet number obtained from a combination of ground-based remote sensing data and in situ observations at ground level. More specifically, the remote sensing data are used to retrieve cloud-scale vertical velocity, and the in situ aerosol measurements at ground level were used constrain as input to a state-of-the-art droplet activation parameterization to predict the respective Cloud Condensation Nuclei (CCN) spectra, cloud maximum supersaturation and droplet number concentration (Nd), accounting for the effects of vertical velocity distribution and lateral entrainment. Closure studies between collocated Nd and Nd sat are then used to evaluate exising droplet spectral width parameters used for the retrieval of droplet number, and determine the optimal values for retrieval. This methodology, used to study aerosol-cloud interactions for non-precipitating clouds formed over the Athens Metropolitan Area (AMA), Greece, during the springtime period from March to May 2020, shows that droplet closure can be achieved to within ±33.4%, comparable to the level of closure obtained in many in situ studies. Given this, the ease of applying this approach with satellite data obtained from SEVIRI with high temporal (15 min) and spatial resolution (3.6 km Ã--4.6 km), opens the possibility of continuous and reliable Ndsat, giving rise to high value datasets for aerosol-cloud-climate interaction studies. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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 space-borne lidar CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) were used. The plumes were located with the help of a trajectory analysis, and the mass 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 (AOD) 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 space-borne aerosol lidars, e.g. being of paramount importance to monitor smoke plumes, and reveals the urgent need of future lidar missions in space. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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 polarisation 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 significant 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 currently most 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 harmonization of satellite records of aerosol properties performed at different wavelengths. [ABSTRACT FROM AUTHOR]

In aerosol science, there is an increasing interest to perform mobile measurements to obtain number size distribution of ultrafine particles (UFP), using portable instruments based on unipolar charging and size segregation by electrical particle mobility. Applications of such measurements range from ambient and indoor aerosol studies to source identification in work environments. However, knowledge on the actual measurement uncertainties of these portable instruments under various conditions has been limited. This investigation presents results from an intercomparison workshop conducted at the World Calibration Center for Aerosol Physics (WCCAP) in Leipzig, Germany, in January 2020. Manufacturers and users were invited to have their portable instruments tested and compared against reference instrumentation for particle number size distributions (PNSD) and total particle number concentration (PNC). In particular, the performances and uncertainties of the NanoScan SMPS (Scanning Mobility Particle Sizer) Model 3910 (TSI Inc.) and the Mini Wide Range Aerosol Spectrometer (WRAS) Model 1371 (Grimm Aerosol Technik) were investigated extensively against the WCCAP Mobility Particle Size Spectrometers (MPSS) and Condensation Particle Counters (CPC). A total of 11 TSI NanoScan SMPS and 4 GRIMM Mini WRAS instruments were characterized for ambient aerosols as well as lab-generated aerosols. The workshop results affirm that the portable instruments must be serviced and calibrated annually or prior field studies to provide measurements within the given uncertainties. It should be noted that users should carry out timely service, maintenance and calibration of portable instruments at their facilities. During initial inspection, non-serviced NanoScan SMPS instruments overestimated a dominant ultrafine aerosol mode by 120 % at around 80 nm. Maintenance and servicing improved the performance. Overall, the performance of NanoScan SMPS instruments improved for the ultrafine aerosol mode while the PNC in the fine aerosol mode still overestimated by up to 80 %. The latter effect seems to be systematically related to the unipolar charging of particles, and the reduced sensitivity of electrical particle mobility with increasing particle size above 200 nm. Due to shift in the second mode of bimodal distribution, particles are overcounted around 100 nm. With regard to the integral PNC, some of the NanoScan SMPS found to be in good agreement (i.e. within 20 %) compared to the reference CPC. In addition, a reasonably good unit-to-unit agreement within ±20 % was found for NanoScan SMPS instruments. The Mini WRAS instruments, after proper cleaning and servicing, provided improved results within ±15 % deviation in PNC in the ultrafine aerosol mode. Overall, most of the GRIMM Mini WRAS instruments (operating with software version 10.0) agrees well with PNC (i.e. 10-50 %) when the ultrafine mode was dominant. Conversely, PNC of the fine aerosol mode was systematically underestimated by 60 % above 100 nm. Except for one instrument, the integral PNC of the GRIMM Mini WRAS spectrometers were within an uncertainty range of ±20 % compared to the reference CPC. Additionally, it is important for users to note that the Mini WRAS performed significantly better when using software version 10.0 compared to version 8.2. The workshop results suggest that despite the above-mentioned uncertainties, these portable instruments are suited for mobile ultrafine particle measurements to detect relative differences in the PNSD such as source apportionment studies of ultrafine particles at work places or outdoors near sources. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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 Polly XT. 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 Polly XT and 910 nm from CL51). Two methods, based on a combined lidar and sun-photometer approach, are applied for mass concentration estimations from both Polly XT 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 Polly XT 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. [ABSTRACT FROM AUTHOR]

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 of this plume were measured to be 0.08 ± 0.02 at 355 nm and 0.05 ± 0.01 at 532 nm which were slightly higher than the values given in the literature. Nonspherical shaped aged smoke particles and/or the mixing with a small amount of fine dust particles could cause the observed increase in the particle linear depolarization ratios. 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 is presented, including the water vapor correction for high latitude for the first time, from sensor provided attenuated backscatter coefficient to particle mass concentration. A combined lidar and sun-photometer approach (based on AERONET products) is applied for mass concentration estimations. Mass concentrations were estimated from both PollyXT and the ceilometer CL51 observations, which were of the order of ~ 30 µg m-3 in the morning and decreased to ~ 20 µg m-3 in the night. A difference of ~ 30 % was found between PollyXT and CL51 estimated mass concentrations. The mass retrievals were discussed and compared with the Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) meteorological and aerosol reanalysis. The inclusion of dust in the retrieved mass concentration slightly improved the correspondence between the observations and the MERRA-2 simulations. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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 %). [ABSTRACT FROM AUTHOR]

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 PM 1 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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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, and 560 m a.s.l.), the part of Pallas Atmosphere – Ecosystem Supersite and Global Atmosphere Watch (GAW) programme. 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 operation and quantified possible biases and discrepancies of different microphysical cloud properties. Based on obtained results we suggested limitations for further use of the instruments in campaigns where focus is on investigating aerosol cloud interactions. Measurements in this study were made by Finnish Meteorological Institute owned instruments and results concern their operation in sub-Arctic conditions with frequently occurring super-cooled clouds. 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 and additionally between the FSSP-100 and the CDP probe was made and presented. Unfortunately, there was not 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 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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

In this study we estimate the particle extinction profiles at Finokalia, Crete, using only the information provided by the elastic and polarization channels of a PollyXT lidar system. Most of the time Finokalia site is affected by only two aerosol types, i.e. marine and dust particles. These two aerosol types, having different optical properties, permit the separation of aerosol mixture. The proposed method 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 taken from literature. The total extinction profile is then estimated and compared well with Raman retrievals. Any difference between the proposed methodology and Raman extinction profiles indicates that the non-dust component could be probably attributed to polluted marine or polluted continental aerosols. Comparison with sun-photometric aerosol optical depth observations is performed as well during daytime with reasonable differences between the two instruments. Differences in the total aerosol optical depth is attributed to the limited ability of the lidar to correctly represent the aerosol optical properties in the near range due to overlap problem. [ABSTRACT FROM AUTHOR]

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 v 4.1 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 v 4.1 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 v 3). 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 v 4.1 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. [ABSTRACT FROM AUTHOR]

The Mineral Aerosol Profiling from Infrared Radiances (MAPIR) algorithm retrieves vertical dust concentration profiles from cloud-free IASI thermal infrared (TIR) radiances using the Rodgers Optimal Estimation Method (OEM). We describe the new version 4.1 and validation 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 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 six months. The post-retrieval quality filters reject about 16 % of the retrievals, a huge improvement with respect to the previous versions where 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 dependency on the total aerosol load due to the assumption of a log-normal state vector. The median degrees of freedom in dusty scenes (min 10 µm AOD of 0.5) is 1.4. A validation of the aerosol optical depth (AOD) obtained from the integrated MAPIR v4.1 profiles was performed against 72 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 (500 nm) negative 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 validation exercise was performed comparing the mean aerosol layer altitude from MAPIR with the mean dust altitude from 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 dependency 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 CATS instrument onboard the 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 in the transport and emission processes of mineral dust aerosols. [ABSTRACT FROM AUTHOR]

Ground-based lidar measurements were performed at Gual Pahari measurement station, approximately 20km South of New Delhi, India, from March 2008 to March 2009. The height of the Planetary Boundary Layer (PBL) was retrieved with a portable Raman lidar system, utilizing the modified Wavelet Covariance Transform (WCT) method. The lidar derived PBL heights were compared to radiosonde data, Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite observations and two atmospheric models. The results were also analyzed on a seasonal basis. To examine the difficulties of PBL lidar detection under different meteorological and aerosol load conditions we focused on three case studies of PBL diurnal evolution. In the presence of a multiple aerosol layer structure, the WCT method exhibited high efficiency in PBL height determination. Good agreement with the European Center for Medium-range Weather Forecasts (ECMWF) and the Weather Research and Forecasting (WRF) estimations was found (r=0.69 and r=0.74, respectively) for a cumulus convection case. In the aforementioned cases, temperature, relative humidity and potential temperature radiosonde profiles were well compared to the respective WRF profiles. The Bulk Richardson Number scheme, which was applied to radiosonde profile data, was in good agreement with lidar data, especially during daytime (r=0.68). The overall comparison with CALIPSO satellite observations; namely, CALIOP Level 2 Aerosol Layer Product, was very satisfying (r=0.84), with CALIPSO Feature Detection Algorithms slightly overestimating PBL height. Lidar measurements revealed that the maximum PBL height was reached approximately three hours after the solar noon, whilst the daily evolution of the PBL was completed, on average, one hour earlier. The PBL diurnal cycle was also analyzed using ECMWF estimations, which produced a stronger cycle during the winter and pre-monsoon period. The seasonal analysis of lidar PBL heights yielded a less pronounced PBL cycle than the one expected from long term climate records. The lowest mean daytime PBL height (695m) appeared in winter, while the highest mean daytime PBL height (1326m) was found in the monsoon season as expected. PBL daily growth rates exhibited also a weak seasonal variability. [ABSTRACT FROM AUTHOR]

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< 2:8, 7.4 and 3.9%, respectively. We also include water vapor mixing ratio intercomparisons between the radio soundings and the various instruments/model for the period of the campaigns. A good agreement is observed for all comparisons with relative errors that do not exceed 50% up to 8 km altitude in most cases. A 4- year seasonal analysis of vertical water vapor is also presented for the Kuopio site in Finland. During winter months, the air in Kuopio is dry (1:15±0:40 gkg-1); during summer it is wet (5:54±1:02 gkg-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. [ABSTRACT FROM AUTHOR]

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 75m high Puijo tower, which itself stands on a 150m 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 10m s-1, the hill can cause updrafts of up to 1m 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. [ABSTRACT FROM AUTHOR]

We investigated size-resolved submicrometre aerosol particle number and volume concentration time series as well as aerosol dynamic parameters derived from Differential Mobility Particle Sizer (DMPS) measurements at five background stations in the Nordic boreal forest area. The stations in question were Aspvreten, Hyytiälä and Utö in southern Finland and Sweden, and Värriö and Pallas in the Finnish Lapland. The objective of our investigation was to identify and quantify annual and interannual variation observable in the time series. We found that the total number and mass concentrations were much lower at the Lapland stations than at the southern stations and that the total particle number was strongly correlated to particle formation event frequency. The annual total number concentration followed the annual distribution of particle formation events at the southern stations but much less clearly at the Lapland stations. The volume concentration was highest during summer, in line with higher condensation growth rates; this is in line with the assumption that a large part of the particle volume is produced by oxidized plant emissions. The decrease of sulphate emissions in Europe was not visible in our data set. Aerosol dynamic parameters such as condensation sink, condensation sink diameter and the power law exponent linking coagulation losses and condensation sink are presented to characterize the submicron Nordic background aerosol. [ABSTRACT FROM AUTHOR]

We analyzed aerosol size distributions from the Finnish measuring stations at Hyytiälä, Värriö and Pallas and the Swedish station at Aspvreten over a period of several years. We identified occurrences of new particle formation bursts and obtained characteristics for the bursts from the size distribution data. In addition, we analyzed the directions from which air masses leading to new particle formation arrived. We found that new particle formation occurs over the whole area covered by the measurement stations. The Northern Atlantic is dominating as a source for air leading to new particle formation at all of the analyzed stations. The formation occurrence had a similar annual variation at all the stations, with peaks in springtime and autumn and minima in winter and summer. The ratio of event days to non-event days had a North-South dependence, with northern stations having lower event ratios. Particle growth rates ranged from 0.5 to 15 nm/h, with the mean growth rate being slightly higher at the southern stations. Southern stations also had a stronger particle source, on average 0.5 cm−3 s−1, compared to the northern stations (0.1 cm−3 s−1). Based on our analysis, it is evident that new particle formation occurs often in whole Nordic boreal forest area when air is transported from the North Atlantic, and that the same process or processes are very probably responsible for the formation over the whole area. [ABSTRACT FROM AUTHOR]

We report initial results from the Optimization of Aerosol Seeding In rain enhancement Strategies (OASIS) field campaign in the United Arab Emirates. Understanding the background aerosol properties is crucial when designing precipitation enhancement strategies. The 1-year OASIS field campaign aimed at characterising the vertical profile of aerosol and the boundary-layer dynamics. The measurement setup comprised in-situ aerosol measurements (DMPS, APS, aethalometer, CCN measurements, filter samples), multi-wavelength lidar (PollyXT), scanning Doppler lidar (Halo Photonics Streamline). Identifying turbulent mixing in the boundary layer enabled extending the information gleaned from the surface measurements into the vertical profile up to the top of the well-mixed layer. The boundary layer exhibited a consistent strong diurnal cycle, with calm conditions at night and a well-mixed convective boundary layer developing during the day to heights of at least 2 km and often reaching 4 km. The surface aerosol concentrations usually decrease during the morning, presumably as a result of dilution into the growing boundary layer, followed by new particle formation. Elevated aerosol layers were also common. A major feature was the presence of low level jets in the wind profile, providing a mechanism for rapid horizontal transport of aerosol, both local and remote. The low-level jets often occurred after sunset, presumably as a response to the collapse of the convective boundary layer. We also identified significant dust events through the combined analysis of boundary layer winds and surface aerosol concentrations, where a rapid increase in aerosol concentrations coincide with wind changes throughout the vertical profile. This indicates air mass changes suggesting long-range transport of aerosol, with possible mechanisms including sea breezes or large-scale synoptic flows. Such flows can potentially generate clouds and convection. [ABSTRACT FROM AUTHOR]

OASIS is a multidisciplinary project aiming at a comprehensive quantification of the role of atmospheric aerosols in efficient precipitation enhancement efforts in the United Arab Emirates (UAE). The projects specific scientific objectives are to: 1) undertake a comprehensive 1-year field campaign (Feb 2018 – Feb 2019) in the UAE employing a multitude of in-situ and lidar instruments to quantify the characteristics and the vertical profile of current background aerosol population as well as the key meteorological drivers of cloud formation in the study region, 2) identify optimal seeding strategies (in terms of e.g., time, location, amount of seeding) by using mesoscale meteorological simulations together with cloud-resolving model simulations with a highly advanced aerosol microphysics description, 3) quantify the characteristics of theoretically optimal ice nucleation seed aerosol by employing a suite of molecular-level simulation methods in order to support future experimental work aiming to develop more efficient ice nuclei, and 4) utilize novel statistical approaches to identify the major sources of uncertainty in prediction of rain enhancement success.This presentation summarizes the main results from the first two project years after the completion of the field campaign and a substantial fraction of the mesoscale, cloud-scale and molecular scale modelling work. Our findings highlight the close connection between the aerosol concentrations and the boundary layer dynamics in the UAE atmosphere, illuminate the optimal seeding strategies in both winter stratocumulus and summer convective cloud cases, and point to surface defects as potential sites for efficient ice nucleation. [ABSTRACT FROM AUTHOR]