Measurements of Aerosol Size and Microphysical Properties: A Comparison Between Raman Lidar and Airborne Sensors

This manuscript compares measurements of aerosol size distributions and microphysical properties retrieved from the Raman lidar BASIL with those obtained from a series of aircraft sensors during HyMeX-SOP1. The attention is focused on a measurement session on 02 October 2012, with BASIL measurements revealing the presence of a lower aerosol layer extending up to 3.3 km and an elevated layer extending from 3.6 to 4.6 km. Aerosol size distribution and microphysical properties are determined from multi-wavelength particle backscattering and extinction profile measurements through a retrieval approach based on Tikhonov regularization. A good agreement is found between BASIL and the microphysical sensors' measurements for all considered aerosol size and microphysical properties. Specifically, BASIL and in-situ volume concentration values are in the range 2-5 mu m(3) cm(-3) in the lower layer and in the range 1-3.5 mu m(3) cm(-3) in the upper layer. Values of the effective radius values from BASIL and the in-situ sensors are in the range 0.2-0.6 mu m in both the lower and upper layer. Aerosol size distributions are determined at 2.2, 2.8, 4 and 4.3 km, with a good agreement between the Raman lidar and the microphysical sensors at all considered heights. We combined these size and microphysical results with Lagrangian back-trajectory analyses and chemical composition measurements. From this combination of datasets we conclude that aerosol particles below 3 km were probably originated by wildfires in North America and/or by anthropogenic activities in North-Eastern Europe, while aerosols above 3 km were also probably originated by wildfires in North America

Linear Estimation of Particle Bulk Parameters from Multi-Wavelength Lidar Measurements

An algorithm for linear estimation of aerosol bulk properties such as particle volume, effective radius and complex refractive index from multiwavelength lidar measurements is presented. The approach uses the fact that the total aerosol concentration can well be approximated as a linear combination of aerosol characteristics measured by multiwavelength lidar. Therefore, the aerosol concentration can be estimated from lidar measurements without the need to derive the size distribution, which entails more sophisticated procedures. The definition of the coefficients required for the linear estimates is based on an expansion of the particle size distribution in terms of the measurement kernels. Once the coefficients are established, the approach permits fast retrieval of aerosol bulk properties when compared with the full regularization technique. In addition, the straightforward estimation of bulk properties stabilizes the inversion making it more resistant to noise in the optical data. Numerical tests demonstrate that for data sets containing three aerosol backscattering and two extinction coefficients (so called 3 + 2 ) the uncertainties in the retrieval of particle volume and surface area are below 45% when input data random uncertainties are below 20 %. Moreover, using linear estimates allows reliable retrievals even when the number of input data is reduced. To evaluate the approach, the results obtained using this technique are compared with those based on the previously developed full inversion scheme that relies on the regularization procedure. Both techniques were applied to the data measured by multiwavelength lidar at NASA/GSFC. The results obtained with both methods using the same observations are in good agreement. At the same time, the high speed of the retrieval using linear estimates makes the method preferable for generating aerosol information from extended lidar observations. To demonstrate the efficiency of the method, an extended time series of observations acquired in Turkey in May 2010 was processed using the linear estimates technique permitting, for what we believe to be the first time, temporal-height distributions of particle parameters

Assessing the Temperature Dependence of Narrow-Band Raman Water Vapor Lidar Measurements: A Practical Approach

Narrow-band detection of the Raman water vapor spectrum using the lidar technique introduces a concern over the temperature dependence of the Raman spectrum. Various groups have addressed this issue either by trying to minimize the temperature dependence to the point where it can be ignored or by correcting for whatever degree of temperature dependence exists. The traditional technique for performing either of these entails accurately measuring both the laser output wavelength and the water vapor spectral passband with combined uncertainty of approximately 0.01 nm. However, uncertainty in interference filter center wavelengths and laser output wavelengths can be this large or larger. These combined uncertainties translate into uncertainties in the magnitude of the temperature dependence of the Raman lidar water vapor measurement of 3% or more. We present here an alternate approach for accurately determining the temperature dependence of the Raman lidar water vapor measurement. This alternate approach entails acquiring sequential atmospheric profiles using the lidar while scanning the channel passband across portions of the Raman water vapor Q-branch. This scanning is accomplished either by tilt-tuning an interference filter or by scanning the output of a spectrometer. Through this process a peak in the transmitted intensity can be discerned in a manner that defines the spectral location of the channel passband with respect to the laser output wavelength to much higher accuracy than that achieved with standard laboratory techniques. Given the peak of the water vapor signal intensity curve, determined using the techniques described here, and an approximate knowledge of atmospheric temperature, the temperature dependence of a given Raman lidar profile can be determined with accuracy of 0.5% or better. A Mathematica notebook that demonstrates the calculations used here is available from the lead author

Improvements in Raman Lidar Measurements Using New Interference Filter Technology

Narrow-band interference filters with improved transmission in the ultra-violet have been developed under NASA-funded research and used in the Raman Airborne Spectroscopic Lidar (RASL) in ground-based, upward-looking tests. Measurements were made of atmospheric water vapor, cirrus cloud optical properties and carbon dioxide that improve upon any previously demonstrated using Raman lidar. Daytime boundary and mixed layer profiling of water vapor mixing ratio up to an altitude of approximately 4 h is performed with less than 5% random error using temporal and spatial resolution of 2-minutes and 60 - 210, respectively. Daytime cirrus cloud optical depth and extinction-to-backscatter ratio measurements are made using 1 -minute average. Sufficient signal strength is demonstrated to permit the simultaneous profiling of carbon dioxide and water vapor mixing ratio into the free troposphere during the nighttime. A description of the filter technology developments is provided followed by examples of the improved Raman lidar measurements

Liquid Water Cloud Measurements Using the Raman Lidar Technique: Current Understanding and Future Research Needs

This paper describes recent work in the Raman lidar liquid water cloud measurement technique. The range-resolved spectral measurements at the National Aeronautics and Space Administration Goddard Space Flight Center indicate that the Raman backscattering spectra measured in and below low clouds agree well with theoretical spectra for vapor and liquid water. The calibration coefficients of the liquid water measurement for the Raman lidar at the Atmospheric Radiation Measurement Program Southern Great Plains site of the U.S. Department of Energy were determined by comparison with the liquid water path (LWP) obtained with Atmospheric Emitted Radiance Interferometer (AERI) and the liquid water content (LWC) obtained with the millimeter wavelength cloud radar and water vapor radiometer (MMCR-WVR) together. These comparisons were used to estimate the Raman liquid water cross-sectional value. The results indicate a bias consistent with an effective liquid water Raman cross-sectional value that is 28%-46% lower than published, which may be explained by the fact that the difference in the detectors' sensitivity has not been accounted for. The LWP of a thin altostratus cloud showed good qualitative agreement between lidar retrievals and AERI. However, the overall ensemble of comparisons of LWP showed considerable scatter, possibly because of the different fields of view of the instruments, the 350-m distance between the instruments, and the horizontal inhomogeneity of the clouds. The LWC profiles for a thick stratus cloud showed agreement between lidar retrievals andMMCR-WVR between the cloud base and 150m above that where the optical depth was less than 3. Areas requiring further research in this technique are discussed

Wildfire smoke, Arctic haze, and aerosol effects on mixed-phase and cirrus clouds over the North Pole region during MOSAiC: an introduction

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 30gkm height. The expedition lasted from September 2019 to October 2020 and measurements were mostly taken between 85 and 88.5ggN. 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 10gkm deep wildfire smoke layer over the North Pole region between 7-8gkm and 17-18gkm height with an aerosol optical thickness (AOT) at 532gnm 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 532gnm AOT by volcanic sulfate aerosol (Raikoke eruption) was estimated to always be lower than 15g%. The optical and microphysical properties of the UTLS smoke layer are presented in an accompanying paper . 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

Australian wildfire smoke in the stratosphere: the decay phase in 2020/2021 and impact on ozone depletion

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

Characterization of Smoke/Dust Episode over West Africa: Comparison of MERRA-2 Modeling with Multiwavelength Mie-Raman Lidar Observations

Observations of multiwavelength Mie-Raman lidar taken during the SHADOW field campaign are used to analyze a smoke/dust episode over West Africa on 24-27 December 2015. For the case considered, the dust layer extended from the ground up to approximately 2000 m while the elevated smoke layer occurred in the 2500 m - 4000 m range. The profiles of lidar measured backscattering, extinction coefficients and depolarization ratios are compared with the vertical distribution of aerosol parameters provided by the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2). The MERRA-2 model simulated the correct location of the near-surface dust and elevated smoke layers. The value of modeled and observed aerosol extinction coefficients at both 355 nm and 532 nm are also rather close. In particular, for the episode reported, the mean value of difference between the measured and modeled extinction coefficients at 355 nm is 0.01 km(exp -1) with standard deviation of 0.042 km(exp -1). The model predicts significant concentration of dust particles inside the elevated smoke layer, which is supported by an increased depolarization ratio of 15% observed in the center of this layer. The modeled at 355 nm the lidar ratio of 65 sr in the near-surface dust layer is close to the observed value (70+/-10) sr. At 532 nm however, the simulated lidar ratio (about 40 sr) is lower than measurements (55+/-8 sr). The results presented demonstrate that the lidar and model data are complimentary and the synergy of observations and models is a key to improve the aerosols characterization

A comparative study of aerosol microphysical properties retrieved from ground-based remote sensing and aircraft in situ measurements during a Saharan dust event

In this work we present an analysis of aerosol microphysical properties during a mineral dust event taking advantage of the combination of different state-of-the-art retrieval techniques applied to active and passive remote sensing measurements and the evaluation of some of those techniques using independent data acquired from in situ aircraft measurements. Data were collected in a field campaign performed during a mineral dust outbreak at the Granada, Spain, experimental site (37.16° N, 3.61° W, 680 m a.s.l.) on 27 June 2011. Column-integrated properties are provided by sun- and star-photometry, which allows for a continuous evaluation of the mineral dust optical properties during both day and nighttime. Both the linear estimation and AERONET (Aerosol Robotic Network) inversion algorithms are applied for the retrieval of the column-integrated microphysical particle properties. In addition, vertically resolved microphysical properties are obtained from a multi-wavelength Raman lidar system included in EARLINET (European Aerosol Research Lidar Network), by using both LIRIC (Lidar Radiometer Inversion Code) algorithm during daytime and an algorithm applied to the Raman measurements based on the regularization technique during nighttime. LIRIC retrievals reveal the presence of dust layers between 3 and 5 km a.s.l. with volume concentrations of the coarse spheroid mode up to 60 µm3 cm−3. The combined use of the regularization and LIRIC methods reveals the night-to-day evolution of the vertical structure of the mineral dust microphysical properties and offers complementary information to that from column-integrated variables retrieved from passive remote sensing. Additionally, lidar depolarization profiles and LIRIC retrieved volume concentration are compared with aircraft in situ measurements. This study presents for the first time a comparison of the total volume concentration retrieved with LIRIC with independent in situ measurements, obtaining agreement within the estimated uncertainties for both methods and quite good agreement for the vertical distribution of the aerosol layers. Regarding the depolarization, the first published data set of the CAS-POL for polarization ratios is presented here and qualitatively compared with the lidar technique