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In September 2021, volcanic aerosol (mainly freshly formed sulfate plumes) originating from the eruption of Cumbre Vieja on La Palma, Canary Islands, Spain, crossed Cabo Verde at altitudes below 2 km. On 24 September 2021, an extraordinary large aerosol optical depth (AOD) close to 1 (daily mean at 500 nm) was observed at Mindelo, Cabo Verde. This event provided favorable conditions to obtain lidar-derived profiles of extinction and backscatter coefficients, lidar ratio, and depolarization ratio at 355, 532 and 1064 nm in the sulfate aerosol plume. A novel feature of the lidar system operated at Mindelo is the availability of extinction, lidar ratio and depolarization measurements at 1064 nm in addition to the standard wavelengths of 355 and 532 nm. Having measurements of these parameters at all three wavelengths is a major advantage for the aerosol characterization and in aerosol typing efforts as the lidar ratio and the particle linear depolarization ratio are key parameters for this purpose. In this article, we present the key results of the lidar observations obtained on one specific day, namely on 24 September 2021 at 04:38–05:57 UTC, including the first ever measurements of the particle extinction coefficient, the lidar ratio and the depolarization ratio at 1064 nm for volcanic sulfate, and discuss the findings in terms of aerosol optical properties and mass concentrations by comparison with a reference observation (16 September 2021) representing the typical background conditions before the start of the eruptions. We found an unusual high particle extinction coefficient of 721 ± 51, 549 ± 38 and 178 ± 13 Mm−1, as well as an enhanced lidar ratio of 66.9 ± 10.1, 60.2 ± 9.2 and 30.8 ± 8.7 sr at 355, 532 and 1064 nm, respectively, in the sulfate-dominated planetary boundary layer (PBL). The particle linear depolarization ratio was ≤ 0.9 % at all respective wavelengths. It is the first time that lidar-derived intensive aerosol optical properties could be derived for volcanic sulfate at all three wavelengths, and thus it is a highly valuable data set for global aerosol characterization. The lidar analysis also revealed a sulfate-related AOD of about 0.35 ± 0.03 at 532 nm of the total PBL-related AOD of 0.43. The rest of the AOD contribution was caused by a lofted Saharan dust layer extending from 1.4 to 5 km and leading to a total AOD of 0.79 at 532 nm. Volcanic ash contribution to the observed aerosol plumes could be mostly excluded based on trajectory analysis and the observed optical properties. Peak mass concentration was 178.5 ± 44.6 µg m−3 in the volcanic-influenced and sulfate-dominated polluted PBL, showing the hazardous potential of such sulfate plumes to significantly worsen local air quality even at remote locations.

The number of intense wildfires may increase further in upcoming years as a consequence of climate change. It is therefore necessary to improve our knowledge about the role of smoke in the climate system, with emphasis on the impact of smoke particles on the evolution of clouds, precipitation, and cloud radiative properties. Presently, one key aspect of research is whether or not wildfire smoke particles can initiate cirrus formation. In this study, we present lidar observations over Limassol, Cyprus, from 27 October to 3 November 2020, when extended wildfire smoke fields crossed the Mediterranean Basin from Portugal to Cyprus. We found strong evidence that aged smoke (organic aerosol particles) originating from wildfires in North America triggered significant ice nucleation at temperatures from −47 to −53 ∘C and caused the formation of extended cirrus layers. The observations suggest that the ice crystals were nucleated just below the tropopause in the presence of smoke particles serving as ice-nucleating particles (INPs). The main part of the 2–3 km thick smoke layer was, however, in the lower stratosphere just above the tropopause. With actual radiosonde observations of temperature and relative humidity and lidar-derived smoke particle surface area concentrations used as starting values, gravity wave simulations show that the lofting of air by 100–200 m is sufficient to initiate significant ice nucleation on the smoke particles, leading to ice crystal number concentrations of 1–100 L−1.

The MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition was the largest Arctic field campaign ever conducted. MOSAiC offered the unique opportunity to monitor and characterize aerosols and clouds with high vertical resolution up to 30 km height at latitudes from 80 to 90∘ N over an entire year (October 2019 to September 2020). Without a clear knowledge of the complex aerosol layering, vertical structures, and dominant aerosol types and their impact on cloud formation, a full understanding of the meteorological processes in the Arctic, and thus advanced climate change research, is impossible. Widespread ground-based in situ observations in the Arctic are insufficient to provide these required aerosol and cloud data. In this article, a summary of our MOSAiC observations of tropospheric aerosol profiles with a state-of-the-art multiwavelength polarization Raman lidar aboard the icebreaker Polarstern is presented. Particle optical properties, i.e., light-extinction profiles and aerosol optical thickness (AOT), and estimates of cloud-relevant aerosol properties such as the number concentration of cloud condensation nuclei (CCN) and ice-nucleating particles (INPs) are discussed, separately for the lowest part of the troposphere (atmospheric boundary layer, ABL), within the lower free troposphere (around 2000 m height), and at the cirrus level close to the tropopause. In situ observations of the particle number concentration and INPs aboard Polarstern are included in the study. A strong decrease in the aerosol amount with height in winter and moderate vertical variations in summer were observed in terms of the particle extinction coefficient. The 532 nm light-extinction values dropped from >50 Mm−1 close to the surface to Mm−1 at 4–6 km height in the winter months. Lofted, aged wildfire smoke layers caused a re-increase in the aerosol concentration towards the tropopause. In summer (June to August 2020), much lower particle extinction coefficients, frequently as low as 1–5 Mm−1, were observed in the ABL. Aerosol removal, controlled by in-cloud and below-cloud scavenging processes (widely suppressed in winter and very efficient in summer) in the lowermost 1–2 km of the atmosphere, seems to be the main reason for the strong differences between winter and summer aerosol conditions. A complete annual cycle of the AOT in the central Arctic could be measured. This is a valuable addition to the summertime observations with the sun photometers of the Arctic Aerosol Robotic Network (AERONET). In line with the pronounced annual cycle in the aerosol optical properties, typical CCN number concentrations (0.2 % supersaturation level) ranged from 50–500 cm−3 in winter to 10–100 cm−3 in summer in the ABL. In the lower free troposphere (at 2000 m), however, the CCN level was roughly constant throughout the year, with values mostly from 30 to 100 cm−3. A strong contrast between winter and summer was also given in terms of ABL INPs which control ice production in low-level clouds. While soil dust (from surrounding continents) is probably the main INP type during the autumn, winter, and spring months, local sea spray aerosol (with a biogenic aerosol component) seems to dominate the ice nucleation in the ABL during the summer months (June–August). The strong winter vs. summer contrast in the INP number concentration by roughly 2–3 orders of magnitude in the lower troposphere is, however, mainly caused by the strong cloud temperature contrast. A unique event of the MOSAiC expedition was the occurrence of a long-lasting wildfire smoke layer in the upper troposphere and lower stratosphere. Our observations suggest that the smoke particles frequently triggered cirrus formation close to the tropopause from October 2019 to May 2020.

A record-breaking stratospheric ozone loss was observed over the Arctic and Antarctica in 2020. Strong ozone depletion occurred over Antarctica in 2021 as well. The ozone holes developed in smoke-polluted air. In this article, the impact of Siberian and Australian wildfire smoke (dominated by organic aerosol) on the extraordinarily strong ozone reduction is discussed. The study is based on aerosol lidar observations in the North Pole region (October 2019–May 2020) and over Punta Arenas in southern Chile at 53.2∘ S (January 2020–November 2021) as well as on respective NDACC (Network for the Detection of Atmospheric Composition Change) ozone profile observations in the Arctic (Ny-Ålesund) and Antarctica (Neumayer and South Pole stations) in 2020 and 2021. We present a conceptual approach on how the smoke may have influenced the formation of polar stratospheric clouds (PSCs), which are of key importance in the ozone-depleting processes. The main results are as follows: (a) the direct impact of wildfire smoke below the PSC height range (at 10–12 km) on ozone reduction seems to be similar to well-known volcanic sulfate aerosol effects. At heights of 10–12 km, smoke particle surface area (SA) concentrations of 5–7 µm2 cm−3 (Antarctica, spring 2021) and 6–10 µm2 cm−3 (Arctic, spring 2020) were correlated with an ozone reduction in terms of ozone partial pressure of 0.4–1.2 mPa (about 30 % further ozone reduction over Antarctica) and of 2–3.5 mPa (Arctic, 20 %–30 % reduction with respect to the long-term springtime mean). (b) Within the PSC height range, we found indications that smoke was able to slightly increase the PSC particle number and surface area concentration. In particular, a smoke-related additional ozone loss of 1–2 mPa (10 %–20 % contribution to the total ozone loss over Antarctica) was observed in the 14–23 km PSC height range in September–October 2020 and 2021. Smoke particle number concentrations ranged from 10 to 100 cm−3 and were about a factor of 10 (in 2020) and 5 (in 2021) above the stratospheric aerosol background level. Satellite observations indicated an additional mean column ozone loss (deviation from the long-term mean) of 26–30 Dobson units (9 %–10 %, September 2020, 2021) and 52–57 Dobson units (17 %–20 %, October 2020, 2021) in the smoke-polluted latitudinal Antarctic belt from 70–80∘ S.

Understanding the evolution of the ice phase within mixed-phase clouds (MPCs) is necessary to reduce uncertainties related to the cloud radiative feedback in climate projections and precipitation initiation. Both primary ice formation via ice-nucleating particles (INPs) and secondary ice production (SIP) within MPCs are unconstrained, not least because of the lack of atmospheric observations. In the past decades, advanced remote sensing methods have emerged which provide high-resolution data of aerosol and cloud properties and could be key in understanding microphysical processes on a global scale. In this study, we retrieved INP concentrations and ice multiplication factors (IMFs) in wintertime orographic clouds using active remote sensing and in situ observations obtained during the RACLETS campaign in the Swiss Alps. INP concentrations in air masses dominated by Saharan dust and continental aerosol were retrieved from a polarization Raman lidar and validated with aerosol and INP in situ observations on a mountaintop. A calibration factor of 0.0204 for the global INP parameterization by DeMott et al. (2010) is derived by comparing in situ aerosol and INP measurements, improving the INP concentration retrieval for continental aerosols. Based on combined lidar and radar measurements, the ice crystal number concentration and ice water content were retrieved and validated with balloon-borne in situ observations, which agreed with the balloon-borne in situ observations within an order of magnitude. For seven cloud cases the ice multiplication factors (IMFs), defined as the quotient of the ice crystal number concentration to the INP concentration, were calculated. The median IMF was around 80, and SIP was active (defined as IMFs > 1) nearly 85 % of the time. SIP was found to be active at all observed temperatures (−30 to −5 ∘C), with the highest IMFs between −20 and −5 ∘C. The introduced methodology could be extended to larger datasets to better understand the impact of SIP not only over the Alps but also at other locations and for other cloud types.

Record-breaking wildfires raged in southeastern Australia in late December 2019 and early January 2020. Rather strong pyrocumulonimbus (pyroCb) convection developed over the fire areas and lofted enormous amounts of biomass burning smoke into the tropopause region and caused the strongest wildfire-related stratospheric aerosol perturbation ever observed around the globe. We discuss the geometrical, optical, and microphysical properties of the stratospheric smoke layers and the decay of this major stratospheric perturbation. A multiwavelength polarization Raman lidar at Punta Arenas (53.2∘ S, 70.9∘ W), southern Chile, and an elastic backscatter Raman lidar at Río Grande (53.8∘ S, 67.7∘ W) in southern Argentina, were operated to monitor the major record-breaking event until the end of 2021. These lidar measurements can be regarded as representative for mid to high latitudes in the Southern Hemisphere. A unique dynamical feature, an anticyclonic, smoke-filled vortex with 1000 km horizontal width and 5 km vertical extent, which ascended by about 500 m d−1, was observed over the full last week of January 2020. The key results of the long-term study are as follows. The smoke layers extended, on average, from 9 to 24 km in height. The smoke partly ascended to more than 30 km height as a result of self-lofting processes. Clear signs of a smoke impact on the record-breaking ozone hole over Antarctica in September–November 2020 were found. A slow decay of the stratospheric perturbation detected by means of the 532 nm aerosol optical thickness (AOT) yielded an e-folding decay time of 19–20 months. The maximum smoke AOT was around 1.0 over Punta Arenas in January 2020 and thus 2 to 3 orders of magnitude above the stratospheric aerosol background of 0.005. After 2 months with strongly varying smoke conditions, the 532 nm AOT decreased to 0.03-0.06 from March–December 2020 and to 0.015–0.03 throughout 2021. The particle extinction coefficients at 532 nm were in the range of 10–75 Mm−1 in January 2020 and, later on, mostly between 1 and 5 Mm−1. Combined lidar–photometer retrievals revealed typical smoke extinction-to-backscatter ratios of 69 ± 19 sr (at 355 nm), 91 ± 17 sr (at 532 nm), and 120 ± 22 sr (at 1064 nm). An ozone reduction of 20 %–25 % in the 15–22 km height range was observed over Antarctica and New Zealand ozonesonde stations in the smoke-polluted air, with particle surface area concentrations of 1–5 µm2 cm−3.

Two layers of Saharan dust observed over Leipzig, Germany, in February and March 2021 were used to provide the first-ever lidar measurements of the dust lidar ratio (extinction-to-backscatter ratio) and linear depolarization ratio at all three classical lidar wavelengths (355, 532 and 1064 nm). The pure-dust conditions during the first event exhibit lidar ratios of 47 ± 8, 50 ± 5 and 69 ± 14 sr and particle linear depolarization ratios of 0.242 ± 0.024, 0.299 ± 0.018 and 0.206 ± 0.010 at wavelengths of 355, 532 and 1064 nm, respectively. The second, slightly polluted-dust case shows a similar spectral behavior of the lidar and depolarization ratio with values of the lidar ratio of 49 ± 4, 46 ± 5 and 57 ± 9 sr and the depolarization ratio of 0.174 ± 0.041, 0.298 ± 0.016 and 0.242 ± 0.007 at 355, 532 and 1064 nm, respectively. The results were compared with Aerosol Robotic Network (AERONET) version 3 (v3) inversion solutions and the Generalized Retrieval of Aerosol and Surface Properties (GRASP) at six and seven wavelengths. Both retrieval schemes make use of a spheroid shape model for mineral dust. The spectral slope of the lidar ratio from 532 to 1064 nm could be well reproduced by the AERONET and GRASP retrieval schemes. Higher lidar ratios in the UV were retrieved by AERONET and GRASP. The enhancement was probably caused by the influence of fine-mode pollution particles in the boundary layer which are included in the columnar photometer measurements. Significant differences between the measured and retrieved wavelength dependence of the particle linear depolarization ratio were found. The potential sources for these uncertainties are discussed.

Multi-year ground-based remote-sensing datasets were acquired with the Leipzig Aerosol and Cloud Remote Observations System (LACROS) at three sites. A highly polluted central European site (Leipzig, Germany), a polluted and strongly dust-influenced eastern Mediterranean site (Limassol, Cyprus), and a clean marine site in the southern midlatitudes (Punta Arenas, Chile) are used to contrast ice formation in shallow stratiform liquid clouds. These unique, long-term datasets in key regions of aerosol–cloud interaction provide a deeper insight into cloud microphysics. The influence of temperature, aerosol load, boundary layer coupling, and gravity wave motion on ice formation is investigated. With respect to previous studies of regional contrasts in the properties of mixed-phase clouds, our study contributes the following new aspects: (1) sampling aerosol optical parameters as a function of temperature, the average backscatter coefficient at supercooled conditions is within a factor of 3 at all three sites. (2) Ice formation was found to be more frequent for cloud layers with cloud top temperatures above -15∘C than indicated by prior lidar-only studies at all sites. A virtual lidar detection threshold of ice water content (IWC) needs to be considered in order to bring radar–lidar-based studies in agreement with lidar-only studies. (3) At similar temperatures, cloud layers which are coupled to the aerosol-laden boundary layer show more intense ice formation than decoupled clouds. (4) Liquid layers formed by gravity waves were found to bias the phase occurrence statistics below -15∘C. By applying a novel gravity wave detection approach using vertical velocity observations within the liquid-dominated cloud top, wave clouds can be classified and excluded from the statistics. After considering boundary layer and gravity wave influences, Punta Arenas shows lower fractions of ice-containing clouds by 0.1 to 0.4 absolute difference at temperatures between −24 and -8∘C. These differences are potentially caused by the contrast in the ice-nucleating particle (INP) reservoir between the different sites.

During the 1-year MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition, the German icebreaker Polarstern drifted through Arctic Ocean ice from October 2019 to May 2020, mainly at latitudes between 85 and 88.5∘ N. A multiwavelength polarization Raman lidar was operated on board the research vessel and continuously monitored aerosol and cloud layers up to a height of 30 km. During our mission, we expected to observe a thin residual volcanic aerosol layer in the stratosphere, originating from the Raikoke volcanic eruption in June 2019, with an aerosol optical thickness (AOT) of 0.005–0.01 at 500 nm over the North Pole area during the winter season. However, the highlight of our measurements was the detection of a persistent, 10 km deep aerosol layer in the upper troposphere and lower stratosphere (UTLS), from about 7–8 to 17–18 km height, with clear and unambiguous wildfire smoke signatures up to 12 km and an order of magnitude higher AOT of around 0.1 in the autumn of 2019. Case studies are presented to explain the specific optical fingerprints of aged wildfire smoke in detail. The pronounced aerosol layer was present throughout the winter half-year until the strong polar vortex began to collapse in late April 2020. We hypothesize that the detected smoke originated from extraordinarily intense and long-lasting wildfires in central and eastern Siberia in July and August 2019 and may have reached the tropopause layer by the self-lifting process. In this article, we summarize the main findings of our 7-month smoke observations and characterize the aerosol in terms of geometrical, optical, and microphysical properties. The UTLS AOT at 532 nm ranged from 0.05–0.12 in October–November 2019 and 0.03–0.06 during the main winter season. The Raikoke aerosol fraction was estimated to always be lower than 15 %. We assume that the volcanic aerosol was above the smoke layer (above 13 km height). As an unambiguous sign of the dominance of smoke in the main aerosol layer from 7–13 km height, the particle extinction-to-backscatter ratio (lidar ratio) at 355 nm was found to be much lower than at 532 nm, with mean values of 55 and 85 sr, respectively. The 355–532 nm Ångström exponent of around 0.65 also clearly indicated the presence of smoke aerosol. For the first time, we show a distinct view of the aerosol layering features in the High Arctic from the surface up to 30 km height during the winter half-year. Finally, we provide a vertically resolved view on the late winter and early spring conditions regarding ozone depletion, smoke occurrence, and polar stratospheric cloud formation. The latter will largely stimulate research on a potential impact of the unexpected stratospheric aerosol perturbation on the record-breaking ozone depletion in the Arctic in spring 2020.

An advanced multiwavelength polarization Raman lidar was operated aboard the icebreaker Polarstern during the MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition to continuously monitor aerosol and cloud layers in the central Arctic up to 30 km height. The expedition lasted from September 2019 to October 2020 and measurements were mostly taken between 85 and 88.5∘ N. The lidar was integrated into a complex remote-sensing infrastructure aboard the Polarstern. In this article, novel lidar techniques, innovative concepts to study aerosol–cloud interaction in the Arctic, and unique MOSAiC findings will be presented. The highlight of the lidar measurements was the detection of a 10 km deep wildfire smoke layer over the North Pole region between 7–8 km and 17–18 km height with an aerosol optical thickness (AOT) at 532 nm of around 0.1 (in October–November 2019) and 0.05 from December to March. The dual-wavelength Raman lidar technique allowed us to unambiguously identify smoke as the dominating aerosol type in the aerosol layer in the upper troposphere and lower stratosphere (UTLS). An additional contribution to the 532 nm AOT by volcanic sulfate aerosol (Raikoke eruption) was estimated to always be lower than 15 %. The optical and microphysical properties of the UTLS smoke layer are presented in an accompanying paper (Ohneiser et al., 2021). This smoke event offered the unique opportunity to study the influence of organic aerosol particles (serving as ice-nucleating particles, INPs) on cirrus formation in the upper troposphere. An example of a closure study is presented to explain our concept of investigating aerosol–cloud interaction in this field. The smoke particles were obviously able to control the evolution of the cirrus system and caused low ice crystal number concentration. After the discussion of two typical Arctic haze events, we present a case study of the evolution of a long-lasting mixed-phase cloud layer embedded in Arctic haze in the free troposphere. The recently introduced dual-field-of-view polarization lidar technique was applied, for the first time, to mixed-phase cloud observations in order to determine the microphysical properties of the water droplets. The mixed-phase cloud closure experiment (based on combined lidar and radar observations) indicated that the observed aerosol levels controlled the number concentrations of nucleated droplets and ice crystals.

In the Arctic summer of 2017 (1 June to 16 July) measurements with the OCEANET-Atmosphere facility were performed during the Polarstern cruise PS106. OCEANET comprises amongst other instruments the multiwavelength polarization lidar PollyXT_OCEANET and for PS106 was complemented with a vertically pointed 35 GHz cloud radar. In the scope of the presented study, the influence of cloud height and surface coupling on the probability of clouds to contain and form ice is investigated. Polarimetric lidar data were used for the detection of the cloud base and the identification of the thermodynamic phase. Both radar and lidar were used to detect cloud top. Radiosonde data were used to derive the thermodynamic structure of the atmosphere and the clouds. The analyzed data set shows a significant impact of the surface-coupling state on the probability of ice formation. Surface-coupled clouds were identified by a quasi-constant potential temperature profile from the surface up to liquid layer base. Within the same minimum cloud temperature range, ice-containing clouds have been observed more frequently than surface-decoupled clouds by a factor of up to 6 (temperature intervals between −7.5 and −5 ∘C, 164 vs. 27 analyzed intervals of 30 min). The frequency of occurrence of surface-coupled ice-containing clouds was found to be 2–3 times higher (e.g., 82 % vs. 35 % between −7.5 and −5 ∘C). These findings provide evidence that above −10 ∘C heterogeneous ice formation in Arctic mixed-phase clouds occurs by a factor of 2–6 more often when the cloud layer is coupled to the surface. In turn, for minimum cloud temperatures below −15 ∘C, the frequency of ice-containing clouds for coupled and decoupled conditions approached the respective curve for the central European site of Leipzig, Germany (51∘ N, 12∘ E). This corroborates the hypothesis that the free-tropospheric ice nucleating particle (INP) reservoir over the Arctic is controlled by continental aerosol. Two sensitivity studies, also using the cloud radar for detection of ice particles and applying a modified coupling state detection, both confirmed the findings, albeit with a lower magnitude. Possible explanations for the observations are discussed by considering recent in situ measurements of INP in the Arctic, of which much higher concentrations were found in the surface-coupled atmosphere in close vicinity to the ice shore.

We present retrievals of tropospheric and stratospheric height profiles of particle mass, volume, surface area, and number concentrations in the case of wildfire smoke layers as well as estimates of smoke-related cloud condensation nuclei (CCN) and ice-nucleating particle (INP) concentrations from backscatter lidar measurements on the ground and in space. Conversion factors used to convert the optical measurements into microphysical properties play a central role in the data analysis, in addition to estimates of the smoke extinction-to-backscatter ratios required to obtain smoke extinction coefficients. The set of needed conversion parameters for wildfire smoke is derived from AERONET observations of major smoke events, e.g., in western Canada in August 2017, California in September 2020, and southeastern Australia in January–February 2020 as well as from AERONET long-term observations of smoke in the Amazon region, southern Africa, and Southeast Asia. The new smoke analysis scheme is applied to CALIPSO observations of tropospheric smoke plumes over the United States in September 2020 and to ground-based lidar observation in Punta Arenas, in southern Chile, in aged Australian smoke layers in the stratosphere in January 2020. These case studies show the potential of spaceborne and ground-based lidars to document large-scale and long-lasting wildfire smoke events in detail and thus to provide valuable information for climate, cloud, and air chemistry modeling efforts performed to investigate the role of wildfire smoke in the atmospheric system.

The seeder–feeder mechanism has been observed to enhance orographic precipitation in previous studies. However, the microphysical processes active in the seeder and feeder region are still being understood. In this paper, we investigate the seeder and feeder region of a mixed-phase cloud passing over the Swiss Alps, focusing on (1) fallstreaks of enhanced radar reflectivity originating from cloud top generating cells (seeder region) and (2) a persistent low-level feeder cloud produced by the boundary layer circulation (feeder region). Observations were obtained from a multi-dimensional set of instruments including ground-based remote sensing instrumentation (Ka-band polarimetric cloud radar, microwave radiometer, wind profiler), in situ instrumentation on a tethered balloon system, and ground-based aerosol and precipitation measurements. The cloud radar observations suggest that ice formation and growth were enhanced within cloud top generating cells, which is consistent with previous observational studies. However, uncertainties exist regarding the dominant ice formation mechanism within these cells. Here we propose different mechanisms that potentially enhance ice nucleation and growth in cloud top generating cells (convective overshooting, radiative cooling, droplet shattering) and attempt to estimate their potential contribution from an ice nucleating particle perspective. Once ice formation and growth within the seeder region exceeded a threshold value, the mixed-phase cloud became fully glaciated. Local flow effects on the lee side of the mountain barrier induced the formation of a persistent low-level feeder cloud over a small-scale topographic feature in the inner-Alpine valley. In situ measurements within the low-level feeder cloud observed the production of secondary ice particles likely due to the Hallett–Mossop process and ice particle fragmentation upon ice–ice collisions. Therefore, secondary ice production may have been partly responsible for the elevated ice crystal number concentrations that have been previously observed in feeder clouds at mountaintop observatories. Secondary ice production in feeder clouds can potentially enhance orographic precipitation.

Previous studies that investigated orographic precipitation have primarily focused on isolated mountain barriers. Here we investigate the influence of low-level blocking and shear-induced turbulence on the cloud microphysics and precipitation formation in a complex inner-Alpine valley. The analysis focuses on a mid-level cloud in a post-frontal environment and a low-level feeder cloud induced by an in-valley circulation. Observations were obtained from an extensive set of instruments including ground-based remote sensing instrumentation, in situ instrumentation on a tethered-balloon system and ground-based precipitation measurements. During this event, the boundary layer was characterized by a blocked low-level flow and enhanced turbulence in the region of strong vertical wind shear at the boundary between the blocked layer in the valley and the stronger cross-barrier flow aloft. Cloud radar observations indicated changes in the microphysical cloud properties within the turbulent shear layer including enhanced linear depolarization ratio (i.e., change in particle shape or density) and increased radar reflectivity (i.e., enhanced ice growth). Based on the ice particle habits observed at the surface, we suggest that riming, aggregation and needle growth occurred within the turbulent layer. Collisions of fragile ice crystals (e.g., dendrites, needles) and the Hallett–Mossop process might have contributed to secondary ice production. Additionally, in situ instrumentation on the tethered-balloon system observed the presence of a low-level feeder cloud above a small-scale topographic feature, which dissipated when the low-level flow turned from a blocked to an unblocked state. Our observations indicate that the low-level blocking (due to the downstream mountain barrier) created an in-valley circulation, which led to the production of local updrafts and the formation of a low-level feeder cloud. Although the feeder cloud did not enhance precipitation in this particular case (since the majority of the precipitation sublimated when falling through a subsaturated layer above), we propose that local flow effects such as low-level blocking can induce the formation of feeder clouds in mountain valleys and on the leeward slope of foothills upstream of the main mountain barrier, where they can act to enhance orographic precipitation through the seeder–feeder mechanism.

In a companion article (Jimenez et al., 2020), we introduced a new lidar method to derive microphysical properties of liquid-water clouds (cloud extinction coefficient, droplet effective radius, liquid-water content, cloud droplet number concentration Nd) at a height of 50–100 m above the cloud base together with aerosol information (aerosol extinction coefficients, cloud condensation nuclei concentration NCCN) below the cloud layer so that detailed studies of the influence of given aerosol conditions on the evolution of liquid-water cloud layers with high temporal resolution solely based on lidar observations have become possible now. The novel cloud retrieval technique makes use of lidar observations of the volume linear depolarization ratio at two different receiver field of views (FOVs). In this article, Part 2, the new dual-FOV polarization lidar technique is applied to cloud measurements in pristine marine conditions at Punta Arenas in southern Chile. A multiwavelength polarization Raman lidar, upgraded by integrating a second polarization-sensitive channel to permit depolarization ratio observations at two FOVs, was used for these measurements at the southernmost tip of South America. Two case studies are presented to demonstrate the potential of the new lidar technique. Successful aerosol–cloud-interaction (ACI) studies based on measurements with the upgraded aerosol–cloud lidar in combination with a Doppler lidar of the vertical wind component could be carried out with 1 min temporal resolution at these pristine conditions. In a stratocumulus layer at the top of the convective boundary layer, we found values of Nd and NCCN (for 0.2 % water supersaturation) ranging from 15–100 and 75–200 cm−3, respectively, during updraft periods. The studies of the aerosol impact on cloud properties yielded ACI values close to 1. The impact of aerosol water uptake on the ACI studies was analyzed with the result that the highest ACI values were obtained when considering aerosol proxies (light-extinction coefficient αpar or NCCN) measured at heights about 500 m below the cloud base (and thus for dry aerosol conditions).

In a series of two articles, a novel, robust, and practicable lidar approach is presented that allows us to derive microphysical properties of liquid-water clouds (cloud extinction coefficient, droplet effective radius, liquid-water content, cloud droplet number concentration) at a height of 50–100 m above the cloud base. The temporal resolution of the observations is on the order of 30–120 s. Together with the aerosol information (aerosol extinction coefficients, cloud condensation nucleus concentration) below the cloud layer, obtained with the same lidar, in-depth aerosol–cloud interaction studies can be performed. The theoretical background and the methodology of the new cloud lidar technique is outlined in this article (Part 1), and measurement applications are presented in a companion publication (Part 2) (Jimenez et al., 2020a). The novel cloud retrieval technique is based on lidar observations of the volume linear depolarization ratio at two different receiver fields of view (FOVs). Extensive simulations of lidar returns in the multiple scattering regime were conducted to investigate the capabilities of a dual-FOV polarization lidar to measure cloud properties and to quantify the information content in the measured depolarization features regarding the basic retrieval parameters (cloud extinction coefficient, droplet effective radius). Key simulation results and the overall data analysis scheme developed to obtain the aerosol and cloud products are presented.

For the first time, a dense data set of particle extinction-to-backscatter ratios (lidar ratios), linear depolarization ratios, and backscatter- and extinction-related Ångström exponents for a Central Asian site are presented. The observations were performed with a continuously running multiwavelength polarization Raman lidar at Dushanbe, Tajikistan, during an 18-month campaign (March 2015 to August 2016). The presented seasonally resolved observations fill an important gap in the database of aerosol optical properties used in aerosol typing efforts with spaceborne lidars and ground-based lidar networks. Lidar ratios and depolarization ratios are also basic input parameters in spaceborne lidar data analyses and in efforts to harmonize long-term observations with different space lidar systems operated at either 355 or 532 nm. As a general result, the found optical properties reflect the large range of occurring aerosol mixtures consisting of long-range-transported dust (from the Middle East and the Sahara), regional desert, soil, and salt dust, and anthropogenic pollution. The full range from highly polluted to pure dust situations could be observed. Typical dust depolarization ratios of 0.23–0.29 (355 nm) and 0.30–0.35 (532 nm) were observed. In contrast, comparably low lidar ratios were found. Dust lidar ratios at 532 nm accumulated around 35–40 sr and were even lower for regional background dust conditions (20–30 sr). Detailed correlation studies (e.g., lidar ratio vs. depolarization ratios, Ångström exponent vs. lidar ratio and vs. depolarization ratio) are presented to illuminate the complex relationships between the observed optical properties and to identify the contributions of anthropogenic haze, dust, and background aerosol to the overall aerosol mixtures found within the 18-month campaign. The observation of 532 nm lidar ratios ( sr) and depolarization ratios (around 15 %–20 %) in layers with very low particle extinction coefficient ( sr) suggests that direct emission and emission of resuspended salt dust (initially originated from numerous desiccating lakes and the Aralkum desert) have a sensitive impact on the aerosol background optical properties over Dushanbe.

For the first time, continuous, vertically resolved long-term aerosol measurements were conducted with a state-of-the-art multiwavelength lidar over a Central Asian site. Such observations are urgently required in efforts to predict future climate and environmental conditions and to support spaceborne remote sensing (ground truth activities). The lidar observations were performed in the framework of the Central Asian Dust Experiment (CADEX) at Dushanbe, Tajikistan, from March 2015 to August 2016. An AERONET (AErosol RObotic NETwork) sun photometer was operated at the lidar field site. During the 18-month campaign, mixtures of continental aerosol pollution and mineral dust were frequently detected from ground to cirrus height level. Regional sources of dust and pollution as well as long-range transport of mineral dust mainly from Middle Eastern and the Saharan deserts determine the aerosol conditions over Tajikistan. In this study, we summarize our findings and present seasonally resolved statistics regarding aerosol layering (main aerosol layer depth, lofted layer occurrence); optical properties (aerosol and dust optical thicknesses at 500–532 nm, vertically resolved light-extinction coefficient at 532 nm); profiles of dust and non-dust mass concentrations and dust fraction; and profiles of particle parameters relevant for liquid water, mixed-phase cloud, and cirrus formation such as cloud condensation nuclei (CCN) and ice-nucleating particle (INP) concentrations. The main aerosol layer over Dushanbe typically reaches 4–5 km height in spring to autumn. Frequently lofted dust-containing aerosol layers were observed at heights from 5 to 10 km, indicating a sensitive potential of dust to influence cloud ice formation. Typical dust mass fractions were of the order of 60 %–80 %. A considerable fraction is thus anthropogenic pollution and biomass burning smoke. The highest aerosol pollution levels (in the relatively shallow winter boundary layer) occur during the winter months. The seasonal mean 500 nm AOT (aerosol optical thickness) ranges from 0.15 in winter to 0.36 in summer during the CADEX period (March 2015 to August 2016); DOTs (dust optical thicknesses) were usually below 0.2; seasonally mean particle extinction coefficients were of the order of 100–500 Mm−1 in the main aerosol layer during the summer half year and about 100–150 Mm−1 in winter but were mainly caused by anthropogenic haze. Accordingly, the highest dust mass concentrations occurred in the summer season (200–600 µg m−3) and the lowest during the winter months (20–50 µg m−3) in the main aerosol layer. In winter, the aerosol pollution mass concentrations were 20–50 µg m−3, while during the summer half year (spring to autumn), the mass concentration caused by urban haze and biomass burning smoke decreases to 10–20 µg m−3 in the lower troposphere. The CCN concentration levels are always controlled by aerosol pollution. The INP concentrations were found to be high enough in the middle and upper troposphere to significantly influence ice formation in mixed-phase and ice clouds during spring and summer seasons.

The consequences of engineered silver nanoparticle (AgNP) exposure and cellular interaction with the immune system are poorly understood. The immunocytes of the Eisenia andrei earthworm are frequently applied in ecotoxicological studies and possess functional similarity to vertebrate macrophages. Hence, we characterized and compared the endocytosis mechanisms for the uptake of 75 nm AgNPs by earthworm coelomocytes, human THP-1 monocytes, and differentiated THP-1 (macrophage-like) cells. Our results indicate that microtubule-dependent, scavenger–receptor, and PI3K signaling-mediated macropinocytosis are utilized during AgNP engulfment by human THP-1 and differentiated THP-1 cells. However, earthworm coelomocytes employ actin-dependent phagocytosis during AgNPs uptake. In both human and earthworm immunocytes, AgNPs were located in the cytoplasm, within the endo-/lysosomes. We detected that the internalization of AgNPs is TLR/MyD88-dependent, also involving the bactericidal/permeability-increasing protein (BPI) in the case of human immunocytes. The exposure led to decreased mitochondrial respiration in human immunocytes; however, in coelomocytes, it enhanced respiratory parameters. Our findings provide more data about NP trafficking as nano-carriers in the nanomedicine field, as well as contribute to an understanding of the ecotoxicological consequences of nanoparticle exposure.

The multi-wavelength Raman lidar PollyXT has been regularly operated aboard the research vessel Polarstern on expeditions across the Atlantic Ocean from north to south and vice versa. The lidar measurements of the RV Polarstern cruises PS95 from Bremerhaven, Germany, to Cape Town, Republic of South Africa (November 2015), and PS98 from Punta Arenas, Chile, to Bremerhaven, Germany (April/May 2016), are presented and analysed in detail. The latest set-up of PollyXT allows improved coverage of the marine boundary layer (MBL) due to an additional near-range receiver.Three case studies provide an overview of the aerosol detected over the Atlantic Ocean. In the first case, marine conditions were observed near South Africa on the autumn cruise PS95. Values of optical properties (depolarisation ratios close to zero, lidar ratios of 23 sr at 355 and 532 nm) within the MBL indicate pure marine aerosol. A layer of dried marine aerosol, indicated by an increase of the particle depolarisation ratio to about 10 % at 355 nm (9 % at 532 nm) and thus confirming the non-sphericity of these particles, could be detected on top of the MBL. On the same cruise, an almost pure Saharan dust plume was observed near the Canary Islands, presented in the second case. The third case deals with several layers of Saharan dust partly mixed with biomass-burning smoke measured on PS98 near the Cabo Verde islands. While the MBL was partly mixed with dust in the pure Saharan dust case, an almost marine MBL was observed in the third case.A statistical analysis showed latitudinal differences in the optical properties within the MBL, caused by the down-mixing of dust in the tropics and anthropogenic influences in the northern latitudes, whereas the optical properties of the MBL in the Southern Hemisphere correlate with typical marine values. The particle depolarisation ratio of dried marine layers ranged between 4 and 9 % at 532 nm.Night measurements from PS95 and PS98 were used to illustrate the potential of aerosol classification using lidar ratio, particle depolarisation ratio at 355 and 532 nm, and Ångström exponent. Lidar ratio and particle depolarisation ratio have been found to be the main indicator for particle type, whereas the Ångström exponent is rather variable.

This study examines the adequacy of the existing Brewer network to supplement other networks from the ground and space to detect SO2 plumes of volcanic origin. It was found that large volcanic eruptions of the last decade in the Northern Hemisphere have a positive columnar SO2 signal seen by the Brewer instruments located under the plume. It is shown that a few days after the eruption the Brewer instrument is capable of detecting significant columnar SO2 increases, exceeding on average 2 DU relative to an unperturbed pre-volcanic 10-day baseline, with a mean close to 0 and σ = 0.46, as calculated from the 32 Brewer stations under study. Intercomparisons with independent measurements from the ground and space as well as theoretical calculations corroborate the capability of the Brewer network to detect volcanic plumes. For instance, the comparison with OMI (Ozone Monitoring Instrument) and GOME-2 (Global Ozone Monitoring Experiment-2) SO2 space-borne retrievals shows statistically significant agreement between the Brewer network data and the collocated satellite overpasses in the case of the Kasatochi eruption. Unfortunately, due to sparsity of satellite data, the significant positive departures seen in the Brewer and other ground networks following the Eyjafjallajökull, Bárðarbunga and Nabro eruptions could not be statistically confirmed by the data from satellite overpasses. A model exercise from the MACC (Monitoring Atmospheric Composition and Climate) project shows that the large increases in SO2 over Europe following the Bárðarbunga eruption in Iceland were not caused by local pollution sources or ship emissions but were clearly linked to the volcanic eruption. Sulfur dioxide positive departures in Europe following Bárðarbunga could be traced by other networks from the free troposphere down to the surface (AirBase (European air quality database) and EARLINET (European Aerosol Research Lidar Network)). We propose that by combining Brewer data with that from other networks and satellites, a useful tool aided by trajectory analyses and modelling could be created which can also be used to forecast high SO2 values both at ground level and in air flight corridors following future eruptions.

Dual frequency magnetic excitation of magnetic nanoparticles (MNP) enables enhanced biosensing applications. This was studied from an experimental and theoretical perspective: nonlinear sum-frequency components of MNP exposed to dual-frequency magnetic excitation were measured as a function of static magnetic offset field. The Langevin model in thermodynamic equilibrium was fitted to the experimental data to derive parameters of the lognormal core size distribution. These parameters were subsequently used as inputs for micromagnetic Monte-Carlo (MC)-simulations. From the hysteresis loops obtained from MC-simulations, sum-frequency components were numerically demodulated and compared with both experiment and Langevin model predictions. From the latter, we derived that approximately 90% of the frequency mixing magnetic response signal is generated by the largest 10% of MNP. We therefore suggest that small particles do not contribute to the frequency mixing signal, which is supported by MC-simulation results. Both theoretical approaches describe the experimental signal shapes well, but with notable differences between experiment and micromagnetic simulations. These deviations could result from Brownian relaxations which are, albeit experimentally inhibited, included in MC-simulation, or (yet unconsidered) cluster-effects of MNP, or inaccurately derived input for MC-simulations, because the largest particles dominate the experimental signal but concurrently do not fulfill the precondition of thermodynamic equilibrium required by Langevin theory.

The ambient aerosol particle extinction coefficient is measured with the Spectral Aerosol Extinction Monitoring System (SÆMS) along a 2.84 km horizontal path at 30–50 m height above ground in the urban environment of Leipzig (51.3° N, 12.4° E), Germany, since 2009. The dependence of the particle extinction coefficient (wavelength range from 300 to 1000 nm) on relative humidity up to almost 100 % was investigated. The main results are presented. For the wavelength of 550 nm, the mean extinction enhancement factor was found to be 1.75 ± 0.4 for an increase of relative humidity from 40 to 80 %. The respective 4-year mean extinction enhancement factor is 2.8 ± 0.6 for a relative-humidity increase from 40 to 95 %. A parameterization of the dependency of the urban particle extinction coefficient on relative humidity is presented. A mean hygroscopic exponent of 0.46 for the 2009–2012 period was determined. Based on a backward trajectory cluster analysis, the dependence of several aerosol optical properties for eight air flow regimes was investigated. Large differences were not found, indicating that local pollution sources widely control the aerosol conditions over the urban site. The comparison of the SÆMS extinction coefficient statistics with respective statistics from ambient AERONET sun photometer observations yields good agreement. Also, time series of the particle extinction coefficient computed from in situ-measured dry particle size distributions and humidity-corrected SÆMS extinction values (for 40 % relative humidity) were found in good overall consistency, which verifies the applicability of the developed humidity parameterization scheme. The analysis of the spectral dependence of particle extinction (Ångström exponent) revealed an increase of the 390–881 nm Ångström exponent from, on average, 0.3 (at 30 % relative humidity) to 1.3 (at 95 % relative humidity) for the 4-year period.