Abstract. Atmospheric aerosol particles are the precondition for the formation of cloud droplets and therefore have large influence on the microphysical and radiative properties of clouds. In this work, four different methods to derive or measure number concentrations of cloud condensation nuclei (CCN) were analyzed and compared for present-day aerosol conditions: (i) a model parameterization based on simulated particle concentrations, (ii) the same parameterization based on gravimetrical particle measurements, (iii) direct CCN measurements with a CCN counter, and (iv) lidar-derived and in situ measured vertical CCN profiles. In order to allow for sensitivity studies of the anthropogenic impact, a scenario to estimate the maximum CCN concentration under peak aerosol conditions of the mid-1980s in Europe was developed as well. In general, the simulations are in good agreement with the observations. At ground level, average values between 0.7 and 1.5×109 CCN m−3 at a supersaturation of 0.2 % were found with the different methods under present-day conditions. The discrimination of the chemical species revealed an almost equal contribution of ammonium sulfate and ammonium nitrate to the total number of CCN for present-day conditions. This was not the case for the peak aerosol scenario, in which it was assumed that no ammonium nitrate was formed while large amounts of sulfate were present, consuming all available ammonia during ammonium sulfate formation. The CCN number concentration at five different supersaturation values has been compared to the measurements. The discrepancies between model and in situ observations were lowest for the lowest (0.1 %) and highest supersaturations (0.7 %). For supersaturations between 0.3 % and 0.5 %, the model overestimated the potentially activated particle fraction by around 30 %. By comparing the simulation with observed profiles, the vertical distribution of the CCN concentration was found to be overestimated by up to a factor of 2 in the boundary layer. The analysis of the modern (year 2013) and the peak aerosol scenario (expected to be representative of the mid-1980s over Europe) resulted in a scaling factor, which was defined as the quotient of the average vertical profile of the peak aerosol and present-day CCN concentration. This factor was found to be around 2 close to the ground, increasing to around 3.5 between 2 and 5 km and approaching 1 (i.e., no difference between present-day and peak aerosol conditions) with further increasing height.
Abstract. 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.
Abstract. Triple-wavelength lidar observations of the depolarization ratio and the backscatter coefficient of marine aerosol as a function of relative humidity (RH) are presented with a 5 min time resolution. The measurements were performed at Barbados (13° N, 59° W) during the Saharan Aerosol Long-range Transport and Aerosol-Cloud interaction Experiment (SALTRACE) winter campaign in February 2014. The phase transition from spherical sea salt particles to cubic-like sea salt crystals was observed with a polarization lidar. The radiosonde and water-vapor Raman lidar observations show a drop in RH below 50 % in the marine aerosol layer simultaneously with a strong increase in particle linear depolarization ratio, which reaches values up to 0.12 ± 0.08 (at 355 nm), 0.15 ± 0.03 (at 532 nm), and 0.10 ± 0.01 (at 1064 nm). The lidar ratio (extinction-to-backscatter ratio) increased from 19 and 23 sr for spherical sea salt particles to 27 and 25 sr (at 355 and 532 nm, respectively) for cubic-like particle ensembles. Furthermore the scattering enhancement due to hygroscopic growth of the marine aerosol particles under atmospheric conditions was measured. Extinction enhancement factors from 40 to 80 % RH of 1.94 ± 0.94 at 355 nm, 3.70 ± 1.14 at 532 nm, and 5.37 ± 1.66 at 1064 nm were found. The enhanced depolarization ratios and lidar ratios were compared to modeling studies of cubic sea salt particles.
Abstract. In August 2018, the first Doppler wind lidar in space called Atmospheric Laser Doppler Instrument (ALADIN) was launched on board the satellite Aeolus by the European Space Agency (ESA). Aeolus measures profiles of one horizontal wind component (i.e., mainly the west–east direction) in the troposphere and lower stratosphere on a global basis. Furthermore, profiles of aerosol and cloud properties can be retrieved via the high spectral resolution lidar (HSRL) technique. The Aeolus mission is supposed to improve the quality of weather forecasts and the understanding of atmospheric processes. We used the opportunity to perform a unique validation of the wind products of Aeolus by utilizing the RV Polarstern cruise PS116 from Bremerhaven to Cape Town in November/December 2018. Due to concerted course modifications, six direct intersections with the Aeolus ground track could be achieved in the Atlantic Ocean west of the African continent. For the validation of the Aeolus wind products, we launched additional radiosondes and used the EARLINET/ACTRIS lidar PollyXT for atmospheric scene analysis. The six analyzed cases prove that Aeolus is able to measure horizontal wind speeds in the nearly west–east direction. Good agreements with the radiosonde observations could be achieved for both Aeolus wind products – the winds observed in clean atmospheric regions called Rayleigh winds and the winds obtained in cloud layers called Mie winds (according to the responsible scattering regime). Systematic and statistical errors of the Rayleigh winds were less than 1.5 and 3.3 m s−1, respectively, when compared to radiosonde values averaged to the vertical resolution of Aeolus. For the Mie winds, a systematic and random error of about 1 m s−1 was obtained from the six comparisons in different climate zones. However, it is also shown that the coarse vertical resolution of 2 km in the upper troposphere, which was set in this early mission phase 2 months after launch, led to an underestimation of the maximum wind speed in the jet stream regions. In summary, promising first results of the first wind lidar space mission are shown and prove the concept of Aeolus for global wind observations.
Abstract. Triple-wavelength polarization lidar measurements in Saharan dust layers were performed at Barbados (13.1° N, 59.6° W), 5000–8000 km west of the Saharan dust sources, in the framework of the Saharan Aerosol Long-range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE-1, June–July 2013, SALTRACE-3, June–July 2014). Three case studies are discussed. High quality was achieved by comparing the dust linear depolarization ratio profiles measured at 355, 532, and 1064 nm with respective dual-wavelength (355, 532 nm) depolarization ratio profiles measured with a reference lidar. A unique case of long-range transported dust over more than 12 000 km is presented. Saharan dust plumes crossing Barbados were measured with an airborne triple-wavelength polarization lidar over Missouri in the midwestern United States 7 days later. Similar dust optical properties and depolarization features were observed over both sites indicating almost unchanged dust properties within this 1 week of travel from the Caribbean to the United States. The main results of the triple-wavelength polarization lidar observations in the Caribbean in the summer seasons of 2013 and 2014 are summarized. On average, the particle linear depolarization ratios for aged Saharan dust were found to be 0.252 ± 0.030 at 355 nm, 0.280 ± 0.020 at 532 nm, and 0.225 ± 0.022 at 1064 nm after approximately 1 week of transport over the tropical Atlantic. Based on published simulation studies we present an attempt to explain the spectral features of the depolarization ratio of irregularly shaped mineral dust particles, and conclude that most of the irregularly shaped coarse-mode dust particles (particles with diameters > 1 µm) have sizes around 1.5–2 µm. The SALTRACE results are also set into the context of the SAMUM-1 (Morocco, 2006) and SAMUM-2 (Cabo Verde, 2008) depolarization ratio studies. Again, only minor changes in the dust depolarization characteristics were observed on the way from the Saharan dust sources towards the Caribbean.
Abstract. The CALIPSO Level 3 (CL3) product is the most recent data set produced by the observations of the Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument onboard the Cloud–Aerosol Lidar and Pathfinder Satellite Observations (CALIPSO) space platform. The European Aerosol Research Lidar Network (EARLINET), based mainly on multi-wavelength Raman lidar systems, is the most appropriate ground-based reference for CALIPSO calibration/validation studies on a continental scale. In this work, CALIPSO data are compared against EARLINET monthly averaged profiles obtained by measurements performed during CALIPSO overpasses. In order to mitigate uncertainties due to spatial and temporal differences, we reproduce a modified version of CL3 data starting from CALIPSO Level 2 (CL2) data. The spatial resolution is finer and nearly 2° × 2° (latitude × longitude) and only simultaneous measurements are used for ease of comparison. The CALIPSO monthly mean profiles following this approach are called CALIPSO Level 3*, CL3*. We find good agreement on the aerosol extinction coefficient, yet in most of the cases a small CALIPSO underestimation is observed with an average bias of 0.02 km−1 up to 4 km and 0.003 km−1 higher above. In contrast to CL3 standard product, the CL3* data set offers the possibility to assess the CALIPSO performance also in terms of the particle backscatter coefficient keeping the same quality assurance criteria applied to extinction profiles. The mean relative difference in the comparison improved from 25 % for extinction to 18 % for backscatter, showing better performances of CALIPSO backscatter retrievals. Additionally, the aerosol typing comparison yielded a robust identification of dust and polluted dust. Moreover, the CALIPSO aerosol-type-dependent lidar ratio selection is assessed by means of EARLINET observations, so as to investigate the performance of the extinction retrievals. The aerosol types of dust, polluted dust, and clean continental showed noticeable discrepancy. Finally, the potential improvements of the lidar ratio assignment have been examined by adjusting it according to EARLINET-derived values.
