Assessing lidar-based classification schemes for polar stratospheric clouds based on 16 years of measurements at Esrange, Sweden

This is an open access article under the terms of the Creative Commons Attribution-NonCommercial-NoDerivs License CC BY-NC-ND 3.0 https://creativecommons.org/licenses/by-nc-nd/3.0/, which permits use and distribution in any medium, provided the original work is properly cited, the use is non-commercial and no modifications or adaptations are made.Lidar measurements of polar stratospheric clouds (PSCs) are commonly analyzed in classification schemes that apply the backscatter ratio and the particle depolarization ratio. This similarity of input data suggests comparable results of different classification schemes - despite measurements being performed with a variety of mostly custom-made instruments. Based on a time series of 16 years of lidar measurements at Esrange (68°N, 21°E), Sweden, we show that PSC classification differs substantially depending on the applied scheme. The discrepancies result from varying threshold values of lidar-derived parameters used to define certain PSC types. The resulting inconsistencies could impact the understanding of long-term PSC observations documented in the literature. We identify two out of seven considered classification schemes that are most likely to give reliable results and should be used in future lidar-based studies. Using polarized backscatter ratios gives the advantage of increased contrast for observations of weakly backscattering and weakly depolarizing particles. Improved confidence in PSC classification can be achieved by a more comprehensive consideration of the effect of measurement uncertainties. The particle depolarization ratio is the key to a reliable identification of different PSC types. Hence, detailed information on the calibration of the polarization-sensitive measurement channels should be provided to assess the findings of a study. Presently, most PSC measurements with lidar are performed at 532 nm only. The information from additional polarization-sensitive measurements in the near infrared could lead to an improved PSC classification. Coincident lidar-based temperature measurements at PSC level might provide useful information for an assessment of PSC classification. Key Points Assessment of PSC classification schemes Statistical analysis of PSC observations Recommendations for lidar-based PSC studiesPeer reviewe

Pure rotational-Raman channels of the Esrange lidar for temperature and particle extinction measurements in the troposphere and lower stratosphere

The Department of Meteorology at Stockholm University operates the Esrange Rayleigh/Raman lidar at Esrange (68° N, 21° E) near the Swedish city of Kiruna. This paper describes the design and first measurements of the new pure rotational-Raman channel of the Esrange lidar. The Esrange lidar uses a pulsed Nd:YAG solid-state laser operating at 532 nm as light source with a repetition rate of 20 Hz and a pulse energy of 350 mJ. The minimum vertical resolution is 150 m and the integration time for one profile is 5000 shots. The newly implemented channel allows for measurements of atmospheric temperature at altitudes below 35 km and is currently optimized for temperature measurements between 180 and 200 K. This corresponds to conditions in the lower Arctic stratosphere during winter. In addition to the temperature measurements, the aerosol extinction coefficient and the aerosol backscatter coefficient at 532 nm can be measured independently. Our filter-based design minimizes the systematic error in the obtained temperature profile to less than 0.51 K. By combining rotational-Raman measurements (5–35 km height) and the integration technique (30–80 km height), the Esrange lidar is now capable of measuring atmospheric temperature profiles from the upper troposphere up to the mesosphere. With the improved setup, the system can be used to validate current lidar-based polar stratospheric cloud classification schemes. The new capability of the instrument measuring temperature and aerosol extinction furthermore enables studies of the thermal structure and variability of the upper troposphere/lower stratosphere. Although several lidars are operated at polar latitudes, there are few instruments that are capable of measuring temperature profiles in the troposphere, stratosphere, and mesosphere, as well as aerosols extinction in the troposphere and lower stratosphere with daylight capability

Cloud condensation nuclei in polluted air and biomass burning smoke near the mega-city Guangzhou, China – Part 1: Size-resolved measurements and implications for the modeling of aerosol particle hygroscopicity and CCN activity

Atmospheric aerosol particles serving as Cloud Condensation Nuclei (CCN) are key elements of the hydrological cycle and climate. We measured and characterized CCN in polluted air and biomass burning smoke during the PRIDE-PRD2006 campaign from 1–30 July 2006 at a rural site ~60 km northwest of the mega-city Guangzhou in southeastern China. CCN efficiency spectra (activated fraction vs. dry particle diameter; 20–290 nm) were recorded at water vapor supersaturations (S) in the range of 0.068% to 1.27%. The corresponding effective hygroscopicity parameters describing the influence of particle composition on CCN activity were in the range of κ≈0.1–0.5. The campaign average value of κ=0.3 equals the average value of κ for other continental locations. During a strong local biomass burning event, the average value of κ dropped to 0.2, which can be considered as characteristic for freshly emitted smoke from the burning of agricultural waste. At low S (≤0.27%), the maximum activated fraction remained generally well below one, indicating substantial portions of externally mixed CCN-inactive particles with much lower hygroscopicity – most likely soot particles (up to ~60% at ~250 nm). The mean CCN number concentrations (NCCN,S) ranged from 1000 cm−3 at S=0.068% to 16 000 cm−3 at S=1.27%, which is about two orders of magnitude higher than in pristine air. Nevertheless, the ratios between CCN concentration and total aerosol particle concentration (integral CCN efficiencies) were similar to the ratios observed in pristine continental air (~6% to ~85% at S=0.068% to 1.27%). Based on the measurement data, we have tested different model approaches for the approximation/prediction of NCCN,S. Depending on S and on the model approach, the relative deviations between observed and predicted NCCN,S ranged from a few percent to several hundred percent. The largest deviations occurred at low S with a simple power law. With a Köhler model using variable κ values obtained from individual CCN efficiency spectra, the relative deviations were on average less than ~10% and hardly exceeded 20%, confirming the applicability of the κ-Köhler model approach for efficient description of the CCN activity of atmospheric aerosols. Note, however, that different types of κ-parameters must be distinguished for external mixtures of CCN-active and -inactive aerosol particles (κa, κt, κcut). Using a constant average hygroscopicity parameter (κ=0.3) and variable size distributions as measured, the deviations between observed and predicted CCN concentrations were on average less than 20%. In contrast, model calculations using variable hygroscopicity parameters as measured and constant size distributions led to much higher deviations: ~70% for the campaign average size distribution, ~80% for a generic rural size distribution, and ~140% for a generic urban size distribution. These findings confirm earlier studies suggesting that aerosol particle number and size are the major predictors for the variability of the CCN concentration in continental boundary layer air, followed by particle composition and hygroscopicity as relatively minor modulators. Depending on the required and applicable level of detail, the information and parameterizations presented in this study should enable efficient description of the CCN activity of atmospheric aerosols in detailed process models as well as in large-scale atmospheric and climate models

Measurement of wind profiles by motion-stabilised ship-borne Doppler lidar

Three months of Doppler lidar wind measurements were obtained during the Arctic Cloud Summer Experiment on the icebreaker Oden during the summer of 2014. Such ship-borne Doppler measurements require active stabilisation to remove the effects of ship motion. We demonstrate that the combination of a commercial Doppler lidar with a custom-made motion-stabilisation platform enables the retrieval of wind profiles in the Arctic atmospheric boundary layer during both cruising and ice-breaking with statistical uncertainties comparable to land-based measurements. This held true particularly within the atmospheric boundary layer even though the overall aerosol load was very low. Motion stabilisation was successful for high wind speeds in open water and the resulting wave conditions. It allows for the retrieval of vertical winds with a random error below 0.2 m s?1. The comparison of lidar-measured wind and radio soundings gives a mean bias of 0.3 m s?1 (2°) and a mean standard deviation of 1.1 m s?1 (12°) for wind speed (wind direction). The agreement for wind direction degrades with height. The combination of a motion-stabilised platform with a low-maintenance autonomous Doppler lidar has the potential to enable continuous long-term high-resolution ship-based wind profile measurements over the oceans.<br/

Cloud condensation nuclei in polluted air and biomass burning smoke near the mega-city Guangzhou, China – Part 1: Size-resolved measurements and implications for the modeling of aerosol particle hygroscopicity and CCN activity

Atmospheric aerosol particles serving as Cloud Condensation Nuclei (CCN) are key elements of the hydrological cycle and climate. We measured and characterized CCN in polluted air and biomass burning smoke during the PRIDE-PRD2006 campaign from 1–30 July 2006 at a rural site ~60 km northwest of the mega-city Guangzhou in southeastern China. CCN efficiency spectra (activated fraction vs. dry particle diameter; 20–290 nm) were recorded at water vapor supersaturations (S) in the range of 0.068% to 1.27%. The corresponding effective hygroscopicity parameters describing the influence of particle composition on CCN activity were in the range of κ≈0.1–0.5. The campaign average value of κ=0.3 equals the average value of κ for other continental locations. During a strong local biomass burning event, the average value of κ dropped to 0.2, which can be considered as characteristic for freshly emitted smoke from the burning of agricultural waste. At low S (≤0.27%), the maximum activated fraction remained generally well below one, indicating substantial portions of externally mixed CCN-inactive particles with much lower hygroscopicity – most likely soot particles (up to ~60% at ~250 nm). The mean CCN number concentrations (NCCN,S) ranged from 1000 cm−3 at S=0.068% to 16 000 cm−3 at S=1.27%, which is about two orders of magnitude higher than in pristine air. Nevertheless, the ratios between CCN concentration and total aerosol particle concentration (integral CCN efficiencies) were similar to the ratios observed in pristine continental air (~6% to ~85% at S=0.068% to 1.27%). Based on the measurement data, we have tested different model approaches for the approximation/prediction of NCCN,S. Depending on S and on the model approach, the relative deviations between observed and predicted NCCN,S ranged from a few percent to several hundred percent. The largest deviations occurred at low S with a simple power law. With a Köhler model using variable κ values obtained from individual CCN efficiency spectra, the relative deviations were on average less than ~10% and hardly exceeded 20%, confirming the applicability of the κ-Köhler model approach for efficient description of the CCN activity of atmospheric aerosols. Note, however, that different types of κ-parameters must be distinguished for external mixtures of CCN-active and -inactive aerosol particles (κa, κt, κcut). Using a constant average hygroscopicity parameter (κ=0.3) and variable size distributions as measured, the deviations between observed and predicted CCN concentrations were on average less than 20%. In contrast, model calculations using variable hygroscopicity parameters as measured and constant size distributions led to much higher deviations: ~70% for the campaign average size distribution, ~80% for a generic rural size distribution, and ~140% for a generic urban size distribution. These findings confirm earlier studies suggesting that aerosol particle number and size are the major predictors for the variability of the CCN concentration in continental boundary layer air, followed by particle composition and hygroscopicity as relatively minor modulators. Depending on the required and applicable level of detail, the information and parameterizations presented in this study should enable efficient description of the CCN activity of atmospheric aerosols in detailed process models as well as in large-scale atmospheric and climate models

Properties of Arctic liquid and mixed phase clouds from ship-borne Cloudnet observations during ACSE 2014

This study presents Cloudnet retrievals of Arctic clouds from measurements conducted during a 3-month research expedition along the Siberian shelf during summer and autumn 2014. During autumn, we find a strong reduction in the occurrence of liquid clouds and an increase for both mixed-phase and ice clouds at low levels compared to summer. About 80 % of all liquid clouds observed during the research cruise show a liquid water path below the infrared black body limit of approximately 50 g m−2. The majority of mixed-phase and ice clouds had an ice water path below 20 g m−2. Cloud properties are analysed with respect to cloud-top temperature and boundary layer structure. Changes in these parameters have little effect on the geometric thickness of liquid clouds while mixed-phase clouds during warm-air advection events are generally thinner than when such events were absent. Cloud-top temperatures are very similar for all mixed-phase clouds. However, more cases of lower cloud-top temperature were observed in the absence of warm-air advection. Profiles of liquid and ice water content are normalized with respect to cloud base and height. For liquid water clouds, the liquid water content profile reveals a strong increase with height with a maximum within the upper quarter of the clouds followed by a sharp decrease towards cloud top. Liquid water content is lowest for clouds observed below an inversion during warm-air advection events. Most mixed-phase clouds show a liquid water content profile with a very similar shape to that of liquid clouds but with lower maximum values during events with warm air above the planetary boundary layer. The normalized ice water content profiles in mixed-phase clouds look different from those of liquid water content. They show a wider range in maximum values with the lowest ice water content for clouds below an inversion and the highest values for clouds above or extending through an inversion. The ice water content profile generally peaks at a height below the peak in the liquid water content profile – usually in the centre of the cloud, sometimes closer to cloud base, likely due to particle sublimation as the crystals fall through the cloud

Meteorological and cloud conditions during the Arctic Ocean 2018 expedition

The Arctic Ocean 2018 (AO2018) took place in the central Arctic Ocean in August and September 2018 on the Swedish icebreaker Oden. An extensive suite of instrumentation provided detailed measurements of surface water chemistry and biology, sea ice and ocean physical and biogeochemical properties, surface exchange processes, aerosols, clouds, and the state of the atmosphere. The measurements provide important information on the coupling of the ocean and ice surface to the atmosphere and in particular to clouds. This paper provides (i) an overview of the synoptic-scale atmospheric conditions and their climatological anomaly to help interpret the process studies and put the detailed observations from AO2018 into a larger context, both spatially and temporally; (ii) a statistical analysis of the thermodynamic and near-surface meteorological conditions, boundary layer, cloud, and fog characteristics; and (iii) a comparison of the results to observations from earlier Arctic Ocean expeditions – in particular AOE1996 (Arctic Ocean Expedition 1996), SHEBA (Surface Heat Budget of the Arctic Ocean), AOE2001 (Arctic Ocean Experiment 2001), ASCOS (Arctic Summer Cloud Ocean Study), ACSE (Arctic Clouds in Summer Experiment), and AO2016 (Arctic Ocean 2016) – to provide an assessment of the representativeness of the measurements. The results show that near-surface conditions were broadly comparable to earlier experiments; however the thermodynamic vertical structure was quite different. An unusually high frequency of well-mixed boundary layers up to about 1 km depth occurred, and only a few cases of the “prototypical” Arctic summer single-layer stratocumulus deck were observed. Instead, an unexpectedly high amount of multiple cloud layers and mid-level clouds were present throughout the campaign. These differences from previous studies are related to the high frequency of cyclonic activity in the central Arctic in 2018

Cloud condensation nuclei in polluted air and biomass burning smoke near the mega-city Guangzhou, China – Part 2: Size-resolved aerosol chemical composition, diurnal cycles, and externally mixed weakly CCN-active soot particles

Size-resolved chemical composition, mixing state, and cloud condensation nucleus (CCN) activity of aerosol particles in polluted mega-city air and biomass burning smoke were measured during the PRIDE-PRD2006 campaign near Guangzhou, China, using an aerosol mass spectrometer (AMS), a volatility tandem differential mobility analyzer (VTDMA), and a continuous-flow CCN counter (DMT-CCNC). The size-dependence and temporal variations of the effective average hygroscopicity parameter for CCN-active particles (κa) could be parameterized as a function of organic and inorganic mass fractions (forg, finorg) determined by the AMS: κa,p=κorg·forg + κinorg·finorg. The characteristic κ values of organic and inorganic components were similar to those observed in other continental regions of the world: κorg≈0.1 and κinorg≈0.6. The campaign average κa values increased with particle size from ~0.25 at ~50 nm to ~0.4 at ~200 nm, while forg decreased with particle size. At ~50 nm, forg was on average 60% and increased to almost 100% during a biomass burning event. The VTDMA results and complementary aerosol optical data suggest that the large fractions of CCN-inactive particles observed at low supersaturations (up to 60% at S≤0.27%) were externally mixed weakly CCN-active soot particles with low volatility (diameter reduction <5% at 300 °C) and effective hygroscopicity parameters around κLV≈0.01. A proxy for the effective average hygroscopicity of the total ensemble of CCN-active particles including weakly CCN-active particles (κt) could be parameterized as a function of κa,p and the number fraction of low volatility particles determined by VTDMA (φLV): κt,p=κa,p−φLV·(κa,p−κLV). Based on κ values derived from AMS and VTDMA data, the observed CCN number concentrations (NCCN,S≈102–104 cm−3 at S = 0.068–0.47%) could be efficiently predicted from the measured particle number size distribution. The mean relative deviations between observed and predicted CCN concentrations were ~10% when using κt,p, and they increased to ~20% when using only κa,p. The mean relative deviations were not higher (~20%) when using an approximate continental average value of κ≈0.3, although the constant κ value cannot account for the observed temporal variations in particle composition and mixing state (diurnal cycles and biomass burning events). Overall, the results confirm that on a global and climate modeling scale an average value of κ≈0.3 can be used for approximate predictions of CCN number concentrations in continental boundary layer air when aerosol size distribution data are available without information about chemical composition. Bulk or size-resolved data on aerosol chemical composition enable improved CCN predictions resolving regional and temporal variations, but the composition data need to be highly accurate and complemented by information about particle mixing state to achieve high precision (relative deviations <20%)

Cloud condensation nuclei (CCN) from fresh and aged air pollution in the megacity region of Beijing

Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate. CCN properties were measured and characterized during the CAREBeijing-2006 campaign at a regional site south of the megacity of Beijing, China. Size-resolved CCN efficiency spectra recorded for a supersaturation range of &lt;i&gt;S&lt;/i&gt;=0.07% to 0.86% yielded average activation diameters in the range of 190 nm to 45 nm. The corresponding effective hygroscopicity parameters (&amp;kappa;) exhibited a strong size dependence ranging from ~0.25 in the Aitken size range to ~0.45 in the accumulation size range. The campaign average value (&amp;kappa; =0.3 ± 0.1) was similar to the values observed and modeled for other populated continental regions. &lt;br&gt;&lt;br&gt; The hygroscopicity parameters derived from the CCN measurements were consistent with chemical composition data recorded by an aerosol mass spectrometer (AMS) and thermo-optical measurements of apparent elemental and organic carbon (EC and OC). The CCN hygroscopicity and its size dependence could be parameterized as a function of only AMS based organic and inorganic mass fractions (&lt;i&gt;f&lt;/i&gt;&lt;sub&gt;org&lt;/sub&gt;, &lt;i&gt;f&lt;/i&gt;&lt;sub&gt;inorg&lt;/sub&gt;) using the simple mixing rule &amp;kappa;&lt;sub&gt;p&lt;/sub&gt; ≈ 0.1 · &lt;i&gt;f&lt;/i&gt;&lt;sub&gt;org&lt;/sub&gt; + 0.7 · &lt;i&gt;f&lt;/i&gt;&lt;sub&gt;inorg&lt;/sub&gt;. &lt;br&gt;&lt;br&gt; When the measured air masses originated from the north and passed rapidly over the center of Beijing (fresh city pollution), the average particle hygroscopicity was reduced (&amp;kappa; = 0.2 ± 0.1), which is consistent with enhanced mass fractions of organic compounds (~50%) and EC (~30%) in the fine particulate matter (PM&lt;sub&gt;1&lt;/sub&gt;). Moreover, substantial fractions of externally mixed weakly CCN-active particles were observed at low supersaturation (&lt;i&gt;S&lt;/i&gt;=0.07%), which can be explained by the presence of freshly emitted soot particles with very low hygroscopicity (&amp;kappa; &lt; 0.1). Particles in stagnant air from the industrialized region south of Beijing (aged regional pollution) were on average larger and more hygroscopic, which is consistent with enhanced mass fractions (~60%) of soluble inorganic ions (mostly sulfate, ammonium, and nitrate). Accordingly, the number concentration of CCN in aged air from the megacity region was higher than in fresh city outflow ((2.5–9.9) × 10&lt;sup&gt;3&lt;/sup&gt; cm&lt;sup&gt;−3&lt;/sup&gt; vs. (0.4–8.3) × 10&lt;sup&gt;3&lt;/sup&gt; cm&lt;sup&gt;−3&lt;/sup&gt; for &lt;i&gt;S&lt;/i&gt;=0.07–0.86%) although the total aerosol particle number concentration was lower (1.2 × 10&lt;sup&gt;4&lt;/sup&gt; cm&lt;sup&gt;−3&lt;/sup&gt; vs. 2.3 × 10&lt;sup&gt;4&lt;/sup&gt; cm&lt;sup&gt;−3&lt;/sup&gt;). A comparison with related studies suggests that the fresh outflow from Chinese urban centers generally may contain more, but smaller and less hygroscopic aerosol particles and thus fewer CCN than the aged outflow from megacity regions

Aerosol optical properties in a rural environment near the mega-city Guangzhou, China: implications for regional air pollution, radiative forcing and remote sensing

The scattering and absorption of solar radiation by atmospheric aerosols is a key element of the Earth&apos;s radiative energy balance and climate. The optical properties of aerosol particles are, however, highly variable and not well characterized, especially near newly emerging mega-cities. In this study, aerosol optical properties were measured at a rural site approximately 60 km northwest of the mega-city Guangzhou in southeast China. The measurements were part of the PRIDE-PRD2006 intensive campaign, covering the period of 1–30 July 2006. Scattering and absorption coefficients of dry aerosol particles with diameters up to 10 μm (PM&lt;sub&gt;10&lt;/sub&gt;) were determined with a three-wavelength integrating nephelometer and with a photoacoustic spectrometer, respectively. &lt;br&gt;&lt;br&gt; Averaged over the measurement campaign (arithmetic mean &amp;plusmn; standard deviation), the total scattering coefficients were 200&amp;plusmn;133 Mm&lt;sup&gt;&amp;minus;1&lt;/sup&gt; (450 nm), 151&amp;plusmn;103 Mm&lt;sup&gt;&amp;minus;1&lt;/sup&gt; (550 nm) and 104&amp;plusmn;72 Mm&lt;sup&gt;&amp;minus;1&lt;/sup&gt; (700 nm) and the absorption coefficient was 34.3&amp;plusmn;26.5 Mm&lt;sup&gt;&amp;minus;1&lt;/sup&gt; (532 nm). The average Ångström exponent was 1.46&amp;plusmn;0.21 (450 nm/700 nm) and the average single scattering albedo was 0.82&amp;plusmn;0.07 (532 nm) with minimum values as low as 0.5. The low single scattering albedo values indicate a high abundance, as well as strong sources, of light absorbing carbon (LAC). The ratio of LAC to CO concentration was highly variable throughout the campaign, indicating a complex mix of different combustion sources. The scattering and absorption coefficients, as well as the Ångström exponent and single scattering albedo, exhibited pronounced diurnal cycles, which can be attributed to boundary layer mixing effects and enhanced nighttime emissions of LAC (diesel soot from regulated truck traffic). The daytime average mid-visible single scattering albedo of 0.87 appears to be more suitable for climate modeling purposes than the 24-h average of 0.82, as the latter value is strongly influenced by fresh emissions into a shallow nocturnal boundary layer. In spite of high photochemical activity during daytime, we found no evidence for strong local production of secondary aerosol mass. &lt;br&gt;&lt;br&gt; The average mass scattering efficiencies with respect to PM&lt;sub&gt;10&lt;/sub&gt; and PM&lt;sub&gt;1&lt;/sub&gt; concentrations derived from particle size distribution measurements were 2.8 m&lt;sup&gt;2&lt;/sup&gt; g&lt;sup&gt;&amp;minus;1&lt;/sup&gt; and 4.1 m&lt;sup&gt;2&lt;/sup&gt; g&lt;sup&gt;&amp;minus;1&lt;/sup&gt;, respectively. The Ångström exponent exhibited a wavelength dependence (curvature) that was related to the ratio of fine and coarse particle mass (PM&lt;sub&gt;1&lt;/sub&gt;/PM&lt;sub&gt;10&lt;/sub&gt;) as well as the surface mode diameter of the fine particle fraction. The results demonstrate consistency between in situ measurements and a remote sensing formalism with regard to the fine particle fraction and volume mode diameter, but there are also systematic deviations for the larger mode diameters. Thus we suggest that more data sets from in situ measurements of aerosol optical parameters and particle size distributions should be used to evaluate formalisms applied in aerosol remote sensing. Moreover, we observed a negative correlation between single scattering albedo and backscatter fraction, and we found that it affects the impact that these parameters have on aerosol radiative forcing efficiency and should be considered in model studies of the PRD and similarly polluted mega-city regions