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

We present particle optical properties of stratospheric smoke layers observed with multiwavelength polarization Raman lidar over Punta Arenas (53.2^∘ S, 70.9^∘ W), Chile, at the southernmost tip of South America in January 2020. The smoke originated from the record-breaking bushfires in Australia. The stratospheric aerosol optical thickness reached values up to 0.85 at 532 nm in mid-January 2020. The main goal of this rapid communication letter is to provide first stratospheric measurements of smoke extinction-to-backscatter ratios (lidar ratios) and particle linear depolarization ratios at 355 and 532 nm wavelengths. These aerosol parameters are important input parameters in the analysis of spaceborne CALIPSO and Aeolus lidar observations of the Australian smoke spreading over large parts of the Southern Hemisphere in January and February 2020 up to heights of around 30 km. Lidar and depolarization ratios, simultaneously measured at 355 and 532 nm, are of key importance regarding the homogenization of the overall Aeolus (355 nm wavelength) and CALIPSO (532 nm wavelength) lidar data sets documenting the spread of the smoke and the decay of the stratospheric perturbation, which will be observable over the entire year of 2020. We found typical values and spectral dependencies of the lidar ratio and linear depolarization ratio for aged stratospheric smoke. At 355 nm, the lidar ratio and depolarization ratio ranged from 53 to 97 sr (mean 71 sr) and 0.2 to 0.26 (mean 0.23), respectively. At 532 nm, the lidar ratios were higher (75–112 sr, mean 97 sr) and the depolarization ratios were lower with values of 0.14–0.22 (mean 0.18). The determined depolarization ratios for aged Australian smoke are in very good agreement with respective ones for aged Canadian smoke, observed with lidar in stratospheric smoke layers over central Europe in the summer of 2017. The much higher 532 nm lidar ratios, however, indicate stronger absorption by the Australian smoke particles.

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.

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 $-\mathrm{15}{}^{\circ }\mathrm{C}$ 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 $-\mathrm{15}{}^{\circ }\mathrm{C}$ . 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 $-\mathrm{8}{}^{\circ }\mathrm{C}$ . These differences are potentially caused by the contrast in the ice-nucleating particle (INP) reservoir between the different sites.

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 µm ² cm⁻³.

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 N_d) at a height of 50–100 m above the cloud base together with aerosol information (aerosol extinction coefficients, cloud condensation nuclei concentration N_CCN) 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 N_d and N_CCN (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 α_par or N_CCN) measured at heights about 500 m below the cloud base (and thus for dry aerosol conditions).