Marine aerosol properties over the Southern Ocean in relation to the wintertime meteorological conditions

Given the vast expanse of oceans on our planet, marine aerosols (and sea salt in particular) play an important role in the climate system via multitude of direct and indirect effects. The efficacy of their net impact, however, depends strongly on the local meteorological conditions that influence their physical, optical and chemical properties. Understanding the coupling between aerosol properties and meteorological conditions is therefore important. It has been historically difficult to statistically quantify this coupling over larger oceanic areas due to the lack of suitable observations, leading to large uncertainties in the representation of aerosol processes in climate models. Perhaps no other region shows higher uncertainties in the representation of marine aerosols and their effects than the Southern Ocean. During winter the Southern Ocean boundary layer is dominated by sea salt emissions. Here, using 10 years of austral winter period (June, July and August, 2007–2016) space-based aerosol profiling by CALIOP-CALIPSO in combination with meteorological reanalysis data, we investigated the sensitivity of marine aerosol properties over the Southern Ocean (40–65∘ S) to various meteorological parameters, such as vertical relative humidity (RH), surface wind speed and sea surface temperature (SST) in terms of joint histograms. The sensitivity study is done for the climatological conditions and for the enhanced cyclonic and anticyclonic conditions in order to understand the impact of large-scale atmospheric circulation on the aerosol properties. We find a clear demarcation in the 532 nm aerosol backscatter and extinction at RH around 60 %, irrespective of the state of the atmosphere. The backscatter and extinction increase at higher relative humidity as a function of surface wind speed. This is mainly because of the water uptake by the wind-driven sea salt aerosols at high RH near the ocean surface resulting in an increase in size, which is confirmed by the decreased depolarization for the wet aerosols. An increase in aerosol backscatter and extinction is observed during the anticyclonic conditions compared to cyclonic conditions for the higher wind speeds and relative humidity, mainly due to aerosols being confined to the boundary layer, and their proximity to the ocean surface facilitates the growth of the particles. We further find a very weak dependency of aerosol backscatter on SSTs at lower wind speeds. However, when the winds are stronger than about 12 m s−1, the backscattering coefficient generally increases with SST. When aerosol properties are investigated in terms of aerosol verticality and in relation to meteorological parameters, it is seen that the aerosol backscatter values in the free troposphere (pressure <850 hPa) are much lower than in the boundary layer, irrespective of the RH and the three weather states. This indicates that the local emissions from the ocean surface make the dominant contribution to aerosol loads over the Southern Ocean. A clear separation of particulate depolarization is observed in the free and lower troposphere, more prominent in the climatological mean and the cyclonic states. For RH > 60 %, low depolarization values are noticeable in the lower troposphere, which is an indication of the dominance of water-coated and mostly spherical sea salt particles. For RH < 60 %, there are instances when the aerosol depolarization increases in the boundary layer; this is more prominent in the mean and anticyclonic cases, which can be associated with the presence of drier aerosol particles. Based on the joint histograms investigated here, we provide third-degree polynomials to obtain aerosol extinction and backscatter as a function of wind speed and relative humidity. Additionally, backscattering coefficient is also expressed jointly in terms of wind speed and sea surface temperature. Furthermore, depolarization is expressed as a function of relative humidity. These fitting functions would be useful to test and improve the parameterizations of sea salt aerosols in the climate models. We also note some limitations of our study. For example, interpreting the verticality of aerosol properties (especially depolarization) in relation to the meteorological conditions in the free and upper troposphere (pressure <850 hPa) was challenging. Furthermore, we do not see any direct evidence of sudden crystallization (efflorescence), deliquescence or hysteresis effects of the aerosols. Observing such effects will likely require a targeted investigation of individual cases considering tracer transport, rather than the statistical sensitivity study that entails temporally and geographically averaged large data sets.

Aerosol backscatter probe for rocket and balloon research

The article briefly describes an optical probe for direct measurements and studies of the vertical distribution of the aerosol component of the atmosphere. The operation principle is based on the measurement of backscattering from a sequence of powerful probing pulses. The analyzed air volume is located at a close (0.5 m) distance from the radiation source. LEDs at 470 nm and 940 nm are used as radiation sources. The probe can be easily integrated with all types of standard aerological radiosondes, meteorological rockets, and having its own navigation module and telemetry system it can also be used in autonomous launches. The results of measurements carried out at the Dolgoprudny aerological station in November 2020, which recorded low values of the aerosol backscattering coefficients in the stratosphere, are presented.

Capabilities of an Automatic Lidar Ceilometer to Retrieve Aerosol Characteristics within the Planetary Boundary Layer

Continuous observation and quantitative retrieval of aerosol backscatter coefficients are important in the study of air quality and climate in metropolitan areas such as New York City. Ceilometers are ideal for this application, but aerosol backscatter coefficient retrievals from ceilometers are challenging and require proper calibration. In this study, we calibrate the ceilometer (Lufft CHM15k, 1064 nm) system constant with the molecular backscatter coefficient and evaluate the calibrated profiles with other independent methods, including the water-phase cloud method and comparison with the NASA Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) attenuated backscatter coefficient profile. Multiple-day calibration results show a stable system constant with a relative uncertainty of about 7%. We also evaluate the overlap correction for the CHM15k ceilometer (provided by Lufft) with a Vaisala CL-31 ceilometer, and the results show good consistency between two ceilometers’ range-corrected signal (RCS) profiles above 200 m. Next, we implement a forward iterative method to retrieve aerosol backscatter coefficients from continuous ceilometer measurements. In the retrieval, the lidar ratio is constrained by the co-located NASA AERONET radiometer aerosol optical depth (AOD) retrieval and agrees with the AERONET lidar-ratio products, derived from aerosol microphysical parameters. The aerosol backscatter coefficient retrievals are validated with co-located elastic-Raman lidar retrievals and indicate a good correlation (R2≥0.95) in the planetary boundary layer (PBL). Furthermore, a case study shows that the ceilometer retrieved aerosol extinction coefficient profiles can be used to estimate the AOD of the PBL and the aloft plumes. Finally, simulations of the uncertainty of aerosol backscatter coefficient retrieval show that a calibration error of 10% results in 10–20% of relative error in the aerosol backscatter coefficient retrievals, while relative error caused by a lidar-ratio error of 10% is less than 4% in the PBL.

Marine aerosol properties over the Southern Ocean in relation to the wintertime meteorological conditions

Given the vast expanse of oceans on our planet, marine aerosols, and sea salt in particular, play an important role in the climate system via multitude of direct and indirect effects. The efficacy of their net impact however depends strongly on the local meteorological conditions that influence their physical, optical and chemical properties. Understanding the coupling between aerosol properties and meteorological conditions is therefore important. It has been historically difficult to statistically quantify this coupling over larger oceanic areas due to the lack of suitable observations, leading to large uncertainties in the representation of aerosol processes in climate models. Perhaps no other region shows higher uncertainties in the representation of marine aerosols and their effects than the Southern Ocean. During winter the Southern Ocean boundary layer is dominated by sea salt emissions. Here, using 10 years of austral winter period (June, July and August, 2007–2016) space based aerosol profiling by CALIOP-CALIPSO in combination with meteorological reanalysis data, we investigated the sensitivity of marine aerosol properties over the Southern Ocean (40S–65S) to various meteorological parameters, such as vertical relative humidity (RH), surface wind speed, and sea surface temperature (SST) in terms of joint histograms. The sensitivity study is done for the climatological conditions as well as for the enhanced cyclonic and anticyclonic conditions in order to understand the impact of large-scale atmospheric circulation on the aerosol properties. We find a clear demarcation in the 532 nm aerosol backscatter and extinction at RH around 60 %, irrespective of the state of the atmosphere. The backscatter and extinction increase at higher relative humidity as a function of surface wind speed. This is mainly because of the water uptake by the wind driven sea salt aerosols at high RH near the ocean surface resulting in an increase in size, which is confirmed by the decreased depolarization for the wet aerosols. An increase in aerosol backscatter and extinction is observed during the anticyclonic conditions compared to cyclonic conditions for the higher wind speeds and relative humidity, mainly due to aerosols being confined to the boundary layer and their proximity to the ocean surface facilitates the growth of the particles. We further find a very weak dependency of aerosol backscatter on SSTs at lower wind speeds. But when the winds are stronger than about 12 m/s, the backscattering coefficient generally increases with SST. When aerosol properties are investigated in terms of aerosol verticality and in relation to meteorological parameters, it is seen that the aerosol backscatter values in the free troposphere (pressure < 850 hPa) are much lower than in the boundary layer, irrespective of the RH and the three weather states. This indicates that the local emissions from the ocean surface make the dominant contribution to aerosol loads over the Southern Ocean. A clear separation of particulate depolarization is observed in the free and lower troposphere, more prominent in the climatological mean and the cyclonic states. For RH > 60 %, low depolarization values are noticeable in the lower troposphere, which is an indication of the dominance of water-coated, mostly spherical sea salt particles. For RH < 60 %, there are instances when the aerosol depolarization increases in the boundary layer, more prominently in the mean and anticyclonic cases which can be associated with the presence of drier aerosol particles. We also note some limitations of our study. For example, interpreting the verticality of aerosol properties (especially depolarization) in relation to the meteorological conditions in the free and upper troposphere (pressure < 850 hPa) was challenging. Furthermore, we do not see any direct evidence of sudden crystallization (efflorescence), deliquescence, or hysteresis effects of the aerosols. Observing such effects will likely require a targeted investigation of individual cases considering tracer transport, rather than the statistical sensitivity study that entails temporally and geographically averaged large data sets.

Ground-based lidar observations of vertical aersosol and water vapor profiles within the boundary layer over heterogeneous terrain

&lt;p&gt;Connecting the earth's surface with the free troposphere, the planetary boundary layer (PBL) comprises complex dynamics of turbulent behavior. This especially applies for areas with heterogeneous terrain. Relevant near-ground processes such as released energy fluxes and the emission of aerosols and trace gases directly interact with the atmosphere. Therefore, the PBL's physical state is determined both by the near-ground processes as well as entrainment of air parcels from higher layers. The mainly turbulence-driven transport of particles and properties throughout the PBL constrain a comprehensive understanding of the PBL's behavior. Hence, the energy balance closure problem as well as errors in precipitation forecast in long-term numerical weather predictions, amongst others, remain unresolved challenges. Here, ground-based lidar profiling is a well suitable method for observing the PBL, as data sampling allows for high temporal and vertical resolutions (Here: Sampling rate of 100\,Hz and 7.5\,m). During the CHEESEHEAD campaign, carried out in summer 2019, our newly developed ATMONSYS lidar performed measurements over complex terrain in northern Wisconsin. There, our lidar system was embedded in a dense network of multiple in-situ and remote sensing instruments. The central aim of this campaign was to further contribute to solve the energy balance closure problem. With the ATMONSYS lidar, vertical columns of aerosol backscatter coefficients, water vapor and temperature have been recorded. The presented work shows what the data is suitable for in terms of resolution and temporal extent in the first place. As a second point, focus is given on structure and variability of aerosol backscatter coefficient distributions and water vapor concentrations as well as their implications on the prevailing state of the PBL. Based on the presented findings, we discuss the potential and suitability of this experimental data for deriving transport processes within the PBL.&lt;/p&gt;

Measurement report: characteristics of clear-day convective boundary layer and associated entrainment zone as observed by a ground-based polarization lidar over Wuhan (30.5° N, 114.4° E)

Knowledge of the convective boundary layer (CBL) and associated entrainment zone (EZ) is important for understanding land–atmosphere interactions and assessing the living conditions in the biosphere. A tilted 532 nm polarization lidar (30∘ off zenith) has been used for the routine atmospheric measurements with 10 s time and 6.5 m height resolution over Wuhan (30.5∘ N, 114.4∘ E). From lidar-retrieved aerosol backscatter, instantaneous atmospheric boundary layer (ABL) depths are obtained using the logarithm gradient method and Harr wavelet transform method, while hourly mean ABL depths are obtained using the variance method. A new approach utilizing the full width at half maximum of the variance profile of aerosol backscatter ratio fluctuations is proposed to determine the entrainment zone thickness (EZT). Four typical clear-day observational cases in different seasons are presented. The CBL evolution is described and studied in four developing stages (formation, growth, quasi-stationary and decay); the instantaneous CBL depths exhibited different fluctuation magnitudes in the four stages and fluctuations at the growth stage were generally larger. The EZT is investigated for the same statistical time interval of 09:00–19:00 LT. It is found that the winter and late autumn cases had an overall smaller mean (mean) and standard deviation (SD) of EZT data compared to those of the late spring and early autumn cases. This statistical conclusion was also true for each of the four developing stages. In addition, compared to those of the late spring and early autumn cases, the winter and late autumn cases had larger percentages of EZT falling into the subranges of 0–50 m but smaller percentages of EZT falling into the subranges of > 150 m. It seems that both the EZT statistics (mean and SD) and percentage of larger EZT values provide measures of entrainment intensity. Common statistical characteristics also existed. All four cases showed moderate variations of the mean of the EZT from stage to stage. The growth stage always had the largest mean and SD of the EZT and the quasi-stationary stage usually the smallest SD of the EZT. For all four stages, most EZT values fell into the 50–150 m subrange; the overall percentage of the EZT falling into the 50–150 m subrange between 09:00 and 19:00 LT was > 67 % for all four cases. We believe that the lidar-derived characteristics of the clear-day CBL and associated EZ can contribute to improving our understanding of the structures and variations of the CBL as well as providing a quantitatively observational basis for EZ parameterization in numerical models.

Validation of aerosol backscatter profiles from Raman lidar and ceilometer using balloon-borne measurements

Remote-sensing measurements by light detection and ranging (lidar) instruments are fundamental for the monitoring of altitude-resolved aerosol optical properties. Here we validate vertical profiles of aerosol backscatter coefficient (βaer) measured by two independent lidar systems using co-located balloon-borne measurements performed by Compact Optical Backscatter Aerosol Detector (COBALD) sondes. COBALD provides high-precision in situ measurements of βaer at two wavelengths (455 and 940 nm). The two analyzed lidar systems are the research Raman Lidar for Meteorological Observations (RALMO) and the commercial CHM15K ceilometer (Lufft, Germany). We consider in total 17 RALMO and 31 CHM15K profiles, co-located with simultaneous COBALD soundings performed throughout the years 2014–2019 at the MeteoSwiss observatory of Payerne (Switzerland). The RALMO (355 nm) and CHM15K (1064 nm) measurements are converted to 455 and 940 nm, respectively, using the Ångström exponent profiles retrieved from COBALD data. To account for the different receiver field-of-view (FOV) angles between the two lidars (0.01–0.02∘) and COBALD (6∘), we derive a custom-made correction using Mie-theory scattering simulations. Our analysis shows that both lidar instruments achieve on average a good agreement with COBALD measurements in the boundary layer and free troposphere, up to 6 km altitude. For medium-high-aerosol-content measurements at altitudes below 3 km, the mean ± standard deviation difference in βaer calculated from all considered soundings is −2 % ± 37 % (−0.018 ± 0.237 Mm−1 sr−1 at 455 nm) for RALMO−COBALD and +5 % ± 43 % (+0.009 ± 0.185 Mm−1 sr−1 at 940 mm) for CHM15K−COBALD. Above 3 km altitude, absolute deviations generally decrease, while relative deviations increase due to the prevalence of air masses with low aerosol content. Uncertainties related to the FOV correction and spatial- and temporal-variability effects (associated with the balloon's drift with altitude and different integration times) contribute to the large standard deviations observed at low altitudes. The lack of information on the aerosol size distribution and the high atmospheric variability prevent an accurate quantification of these effects. Nevertheless, the excellent agreement observed in individual profiles, including fine and complex structures in the βaer vertical distribution, shows that under optimal conditions, the discrepancies with the in situ measurements are typically comparable to the estimated statistical uncertainties in the remote-sensing measurements. Therefore, we conclude that βaer profiles measured by the RALMO and CHM15K lidar systems are in good agreement with in situ measurements by COBALD sondes up to 6 km altitude.

Consistency of the Single Calculus Chain Optical Products with Archived Measurements from an EARLINET Lidar Station

A long-term analysis and climatology of aerosol backscatter and extinction coefficients profiles using a five-year study period lidar dataset derived from a multiwavelenth Raman lidar at Thessaloniki station is presented. All measurements have been processed with the latest version of the Single Calculus Chain (SCCv5.1.6) fully automated algorithm, which has been developed to provide a common lidar processing tool, within EARLINET (European Aerosol Research Lidar NETwork) stations. The optical products delivered by the SCC tool have already been compared with the optical products derived from the operational algorithm of Thessaloniki (THessaloniki Aerosol LIdar Algorithm-THALIA) and discussed in terms of inhomogeneities. In this contribution, we analyze these products for climatological purposes, in order to investigate the aerosol columnar properties over Thessaloniki lidar station, drawing conclusions about the issues to be considered when switching from the current operational algorithm to the SCCv5. The SCCv5 algorithm is evaluated for the AOD both for 355 and 532 nm. The agreement with THALIA algorithm seems promising with correlations of 0.89 and 0.84, respectively, and absolute deviations within the range of the EARLINET quality requirements. Time series of the AOD at 355 nm denote a decrease of 0.017 per year in the free troposphere, a trend that is also shown in the AOD values derived from the operational algorithm (0.014). A decrease of 0.01 per year in the lower troposphere is also noted from the SCC, whereas the corresponding AOD values derived from the operational algorithm denote a decrease of 0.017.

Strong day-to-day variability of the Asian Tropopause Aerosol Layer (ATAL) in August 2016 at the Himalayan foothills

The South Asian summer monsoon is associated with a large-scale anticyclonic circulation in the upper troposphere and lower stratosphere (UTLS), which confines the air mass inside. During boreal summer, the confinement of this air mass leads to an accumulation of aerosol between about 13 and 18 km (360 and 440 K potential temperature); this accumulation of aerosol constitutes the Asian Tropopause Aerosol Layer (ATAL). We present balloon-borne aerosol backscatter measurements of the ATAL performed by the Compact Optical Backscatter Aerosol Detector (COBALD) instrument in Nainital in northern India in August 2016, and compare these with COBALD measurements in the post-monsoon time in November 2016. The measurements demonstrate a strong variability of the ATAL's altitude, vertical extent, aerosol backscatter intensity and cirrus cloud occurrence frequency. Such a variability cannot be deduced from climatological means of the ATAL as they are derived from satellite measurements. To explain this observed variability we performed a Lagrangian back-trajectory analysis using the Chemical Lagrangian Model of the Stratosphere (CLaMS). We identify the transport pathways as well as the source regions of air parcels contributing to the ATAL over Nainital in August 2016. Our analysis reveals a variety of factors contributing to the observed day-to-day variability of the ATAL: continental convection, tropical cyclones (maritime convection), dynamics of the anticyclone and stratospheric intrusions. Thus, the air in the ATAL is a mixture of air masses coming from different atmospheric altitude layers. In addition, contributions from the model boundary layer originate in different geographic source regions. The location of the strongest updraft along the backward trajectories reveals a cluster of strong upward transport at the southern edge of the Himalayan foothills. From the top of the convective outflow level (about 13 km; 360 K) the air parcels ascend slowly to ATAL altitudes within a large-scale upward spiral driven by the diabatic heating in the anticyclonic flow of the South Asian summer monsoon at UTLS altitudes. Cases with a strong ATAL typically show boundary layer contributions from the Tibetan Plateau, the foothills of the Himalayas and other continental regions below the Asian monsoon. Weaker ATAL cases show higher contributions from the maritime boundary layer, often related to tropical cyclones, indicating a mixing of clean maritime and polluted continental air. On the one hand increasing anthropogenic emissions in the future are expected due to the strong growth of Asian economies; on the other hand the implementation of new emission control measures (in particular in China) has reduced the anthropogenic emissions of some pollutants contributing to the ATAL substantially. It needs to be monitored in the future whether the thickness and intensity of the ATAL will further increase, which will likely impact the surface climate.