Extinction Profiles Research Articles

Spectroscopic amplifier for ultrahigh plasmonic-based enhancement of the hyper-Raman scattering procedure

An anisotropic plasmonic trimer is proposed as an effective spectroscopic amplifier for the maximum signal enhancement of the Hyper-Raman Scattering (HRS) process. The three-particle system is composed of asymmetric Au nanorings arranged collinearly in a J-aggregate configuration and illuminated by a longitudinally polarized light. The optical properties of the considered trimer have been numerically simulated by the Finite-Difference Time-Domain (FDTD) method. The extinction profile of the heterotrimer exhibits the excitation of two plasmonic bands, superradiant and subradiant (Fano interference) modes. From the associated highly enhanced and strongly localized nearfield, the Enhancement Factor of the Surface-Enhanced HRS (EFSEHRS) is calculated. The simulation results demonstrate the impact of both the thickness and height of the interacting rings on the Raman factor. To reach the desired value of the EFSEHRS, the thickness of the rings should be maximized, and their height must be minimized. These two factors work together to enormously increase the charge density accumulated in the intercoupling region, the associated nearfield intensity, and therefore significantly augment the corresponding EFSEHRS. The EFSEHRS increases exponentially with decreasing height and increasing thickness of the trimer system. For selected values of both thickness and height, EFSEHRS can reach a value never reported before, as high as 5.6x1023.&#xD.

Insights into the Solution Processing of Non-van der Waals Boron Carbide.

Exfoliation of non-layered materials is crucial to unleash their enormous potential in wide range of applications. However, the presence of strong non-van der Waals interactions in all three dimensions makes exfoliation challenging. Boron carbide (B4C), known for its high hardness, holds great potential for diverse applications. In this work, B4C is exfoliated in 29 solvents to determine its Hansen solubility parameters (HSP) and understand the dispersion stability. The experimentally determined HSP values are 19.6, 15.3 and 15.1 MPa1/2 for dispersive interactions (δD), polar interactions (δP) and hydrogen bonding interactions (δH), respectively. Subsequently, in situ dispersion stability is analyzed qualitatively and quantitatively from the space-time resolved extinction profiles employing an analytical centrifuge. The sedimentation kinetics of B4C dispersions are analyzed using instability index, integral extinction and sedimentation velocity. B4C dispersions in solvents like ϵ-caprolactone, isopropyl alcohol, propylene carbonate and formamide exhibited excellent stability. Additionally, B4C nanosheets are utilized to investigate their field emission properties. These nanosheets exhibit a turn-on electric field of 3.35 V/μm at an emission current density of 1 μA cm-2, and it delivered a large emission current density of ~375 μA cm-2 at an applied electric field of 5.7 V/μm.

Retrieval of stratospheric aerosol extinction coefficients from sun-normalized Ozone Mapper and Profiler Suite Limb Profiler (OMPS-LP) measurements

Abstract. A new retrieval approach for obtaining vertical profiles of the aerosol extinction coefficient from measurements of scattered solar light in the limb-viewing geometry made by the Ozone Mapper and Profiler Suite Limb Profiler (OMPS-LP) instrument is presented. In contrast to many other published limb-scatter retrievals, our new algorithm does not employ normalization by a limb measurement at an upper tangent height. Instead, the measured limb radiances are normalized to solar irradiance. The main advantage of this approach is an almost complete elimination of the dependence of the retrieval results on the prior aerosol extinction profile used in the retrieval. This makes the retrieval better suited for the analysis of observation scenes with highly elevated aerosol plumes, such as those that occurred after the Hunga Tonga–Hunga Ha′apai volcanic eruption in January 2022. The results from the new approach were compared to the vertical profiles of the aerosol extinction coefficients retrieved from the Stratospheric Aerosol and Gas Experiment III on the International Space Station (SAGE III/ISS) and the Optical Spectrograph and InfraRed Imaging System (OSIRIS). In general, agreement within 25 % between the different data products was observed in the 18–23 km altitude range, although larger differences were seen after very strong volcanic eruptions and wildfires. In comparison with OSIRIS, larger differences are seen at high southern latitudes (above 60° S). The new data product was used to investigate the evolution of the aerosol plume after the Hunga Tonga–Hunga Ha′apai volcanic eruption.

Balloon Baseline Stratospheric Aerosol Profiles (B2SAP)—Perturbations in the Southern Hemisphere, 2019–2022

AbstractVolcanic and pyrocumulonimbus (pyroCB) injections into the stratosphere perturb the aerosol layer and can have important radiative and chemical impacts on timescales spanning from months to several years. Repeated in situ balloon‐borne measurements of aerosol size and number concentration (>140 nm in diameter), ozone, water vapor, and atmospheric state variables made at midlatitudes in the southern hemisphere (SH) since 2019 enable us to better characterize such events. We use this record and coincident lidar extinction profiles to study several moderate to large stratospheric perturbations in the SH between 2019 and 2022 in detail, including the Australian New Year Super Outbreak (ANYSO) pyroCB in 2020. Median vertical profiles of aerosol number concentration, effective radius, and surface area in SH midlatitudes are also compared with those recorded in Northern Hemisphere midlatitudes under baseline conditions using an identical payload. These data depict the variability in stratospheric aerosol properties in the SH midlatitudes during this period and provide a benchmark for global sectional aerosol models. They reveal that sulfate particle size distributions under baseline conditions and in volcanic plumes are relatively well represented in the Community Earth System Model—Community Aerosol Radiation Model for Atmospheres (CESM‐CARMA), but more observations of biomass burning plumes are needed to improve model skill in simulating pyroCB. Comparisons between in situ and lidar observations also highlight a need for more observations of aerosol composition and refractive index in both fresh and aging biomass burning plumes.

CREST: a Climate Data Record of Stratospheric Aerosols

Abstract. Climate-related studies need information about the distribution of stratospheric aerosols, which influence the energy balance of the Earth's atmosphere. In this work, we present a merged dataset of vertically resolved stratospheric aerosol extinction coefficients, which is derived using data from six limb and occultation satellite instruments: SAGE (Stratospheric Aerosol and Gas Experiment) II on ERBS (Earth Radiation Budget Satellite), GOMOS (Global Ozone Monitoring by Occultation of Stars) and SCIAMACHY (Scanning Imaging Spectrometer for Atmospheric Chartography) on Envisat, OSIRIS (Optical Spectrograph and InfraRed Imaging System) on Odin, OMPS (Ozone Monitor Profiling Suite Limb Profiler) on Suomi NPP, and SAGE III on the ISS (International Space Station). The merging of aerosol profiles is performed via the transformation of the aerosol datasets from individual satellite instruments to the same wavelength (750 nm) and their de-biasing and homogenization by adjusting the seasonal cycles. After such homogenization, the data from individual satellite instruments are in good agreement. The merged aerosol extinction coefficient is computed as the median of the adjusted data from the individual instruments. The merged time series of vertically resolved monthly mean aerosol extinction coefficients at 750 nm is provided in 10° latitudinal bins from 90° S to 90° N, in the altitude range from 8.5 to 39.5 km. The time series of the stratospheric aerosol optical depth (SAOD) is created via the integration of aerosol extinction profiles from the tropopause to 39.5 km; it is also provided as monthly mean data in 10° latitudinal bins. The created aerosol climate record covers the period from October 1984 until December 2023, and it is intended to be extended in the future. The merged CREST aerosol dataset (v2) is available at https://doi.org/10.57707/fmib2share.dfe14351fd8548bcaca3c2956b17f665 (Sofieva et al., 2024a). It can be used in various climate-related studies.

Three-dimensional distribution of aerosols of multiple types at daily scale using TROPOMI spaceborne observations

We present new satellite-based daily observations of the 3D distribution of aerosols from most common types and origins, both over land and ocean, derived from TROpospheric Ozone Monitoring Instrument (TROPOMI) measurements. This is done using the so-called AEROS5P (AEROsol Sentinel 5 Precursor) approach which retrieves vertical profiles of aerosol extinction from passive measurements of high-resolution spectral reflectance in the visible and near infrared for cloud-free conditions. Previous work demonstrated the potential of this approach, but it was initially applicable only to biomass burning aerosols with limited spatial coverage over ocean. The new methodology presented here generalizes the method for the most common aerosol types and improves spatial coverage. We take advantage of an operational aerosol type product derived from Visible Infrared Imaging Radiometer Suite (VIIRS) observations, combined with those from TROPOMI, to choose a priori aerosol set of intensive properties (particle size and refractive index). AEROS5P shows good agreement in aerosol optical depth, when compared to observations from AErosol RObotic NETwork and other widely used satellite measurements. Additionally, the vertical distribution of aerosol plumes of different types derived from AEROS5P agrees well with lidar coincident observations from the Advanced Topographic Laser Altimeter System spaceborne sensor and ground-based measurements. We utilize AEROS5P to analyze the three-dimensional distribution of aerosols for four different scenarios. It traces the three-dimensional pathways of smoke from Canadian wildfires reaching the Eastern USA in July 2023, desert dust from the Namibian deserts over the southeast Atlantic Ocean confined near the surface during the same month, fine aerosol pollution over Western Europe during June 2019, and an extreme dust event mixed with fine aerosol pollution over Northern China in March 2021. These observations provide valuable insights into aerosol transport patterns, surface-level air quality impacts, and can potentially be used to assess the radiative effects at various atmospheric layers.

CALIPSO-based aerosol extinction profile estimation from MODIS and MERRA-2 data using a hybrid model of Transformer and CNN

Acquiring aerosol vertical distribution information is crucial to accurately quantify the aerosol radiation effect on climate and understand the environmental pollution mechanism of the atmosphere. Passive remote sensing has shown its capability to gain large-scale, high spatiotemporal resolution aerosol vertical information such as aerosol layer height (ALH). However, it is still challenging to extract detailed aerosol vertical distribution information, e.g., aerosol extinction profile (AEP), from passive observations. To fill this gap, this study proposed a hybrid model of Transformer and convolutional neural network (CNN) to estimate the AEP from passive multispectral remote sensing (MODIS) measurements with the aid of three-dimensional reanalysis data (MERRA-2). Specifically, the model is learned to estimate the AEP, which is called AproNet, by using the active space-borne lidar (CALIPSO) data as supervised information. Besides, we design a shape invariant loss (SIL) to better capture the shape characteristics of the AEP and incorporate an auxiliary scene awareness loss (SAL) to enhance the model's generalization capacity and physical reliability outside the CALIPSO orbit. The extensive quantitative experiments show that the AEPs estimated by the proposed model agree well with the CALIPSO measurements with an overall performance of IOA=0.821, R=0.800, MAE= 0.014, and RMSE= 0.041, respectively. Qualitative comparisons also demonstrate the model's reliability in estimating the aerosol three-dimensional spatial distribution. Independent year test and comparisons with ground-based lidar measurements further indicate the robustness of the proposed model despite some degradation in performance. However, the incompleteness and uncertainty of the CALIOP products limited the performance of the proposed model to some extent. In the future, the model needs to be further physically constrained and strengthened with more data sources to improve reliability. In general, this study paves the way for acquiring aerosol extinction profiles with high spatiotemporal resolution over a large geographical space.

Influence of columnar versus vertical distribution of aerosol properties on the modulation of shortwave radiative effects

Influence of columnar versus vertical distribution of aerosol properties on the modulation of shortwave radiative effects

Evidence of a dual African and Australian biomass burning influence on the vertical distribution of aerosol and carbon monoxide over the southwest Indian Ocean basin in early 2020

Abstract. During the 2020 austral summer, the pristine atmosphere of the southwest Indian Ocean (SWIO) basin experienced significant perturbations. This study examines the variability of aerosols and carbon monoxide (CO) over this remote oceanic region and investigates the underlying processes in the upper troposphere–lower stratosphere (UT-LS). Aerosol profiles in January and February 2020 revealed a multi-layer structure in the tropical UT-LS. Numerical models – the FLEXible PARTicle dispersion model (FLEXPART) and the Modèle Isentropique de transport Mésoéchelle de l'Ozone Stratosphérique par Advection (MIMOSA) – indicated that the lower-stratospheric aerosol content was influenced by the intense and persistent stratospheric aerosol layer generated during the 2019–2020 extreme Australian bushfire events. A portion of this layer was transported eastward by prevailing easterly winds, leading to increased aerosol extinction profiles over Réunion on 27 and 28 January. Analysis of advected potential vorticity revealed isentropic transport of air masses containing Australian biomass burning aerosols from extratropical latitudes to Réunion at the 400 K isentropic level on 28 January. Interestingly, we found that biomass burning (BB) activity in eastern Africa, though weak during this season, significantly influenced (contributed up to 90 % of) the vertical distribution of CO and aerosols in the upper troposphere over the SWIO basin. Ground-based observations at Réunion confirmed the simultaneous presence of African and Australian aerosol layers. This study provides the first evidence of African BB emissions impacting the CO and aerosol distribution in the upper troposphere over the SWIO basin during the convective season.

Spline-based Abel Transform (SAT) radial property reconstruction for noise and trapping correction: Application to axisymmetric sooting flames

Spline-based Abel Transform (SAT) radial property reconstruction for noise and trapping correction: Application to axisymmetric sooting flames

High Spectral Resolution Lidar – generation 2 (HSRL-2) retrievals of ocean surface wind speed: methodology and evaluation

Abstract. Ocean surface wind speed (i.e., wind speed 10 m above sea level) is a critical parameter used by atmospheric models to estimate the state of the marine atmospheric boundary layer (MABL). Accurate surface wind speed measurements in diverse locations are required to improve characterization of MABL dynamics and assess how models simulate large-scale phenomena related to climate change and global weather patterns. To provide these measurements, this study introduces and evaluates a new surface wind speed data product from the NASA Langley Research Center nadir-viewing High Spectral Resolution Lidar – generation 2 (HSRL-2) using data collected as part of the NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) mission. The HSRL-2 can directly measure vertically resolved aerosol backscatter and extinction profiles without additional constraints or assumptions, enabling the instrument to accurately derive atmospheric attenuation and directly determine surface reflectance (i.e., surface backscatter). Also, the high horizontal spatial resolution of the HSRL-2 retrievals (0.5 s or ∼ 75 m along track) allows the instrument to probe the fine-scale spatial variability in surface wind speeds over time along the flight track and over breaks in broken cloud fields. A rigorous evaluation of these retrievals is performed by comparing coincident HSRL-2 and National Center for Atmospheric Research (NCAR) Airborne Vertical Atmosphere Profiling System (AVAPS) dropsonde data, owing to the joint deployment of these two instruments on the ACTIVATE King Air aircraft. These comparisons show correlations of 0.89, slopes of 1.04 and 1.17, and y intercepts of −0.13 and −1.05 m s−1 for linear and bisector regressions, respectively, and the overall accuracy is calculated to be 0.15 ± 1.80 m s−1. It is also shown that the dropsonde surface wind speed data most closely follow the HSRL-2 distribution of wave slope variance using the distribution proposed by Hu et al. (2008) rather than the ones proposed by Cox and Munk (1954) and Wu (1990) for surface wind speeds below 7 m s−1, with this category comprising most of the ACTIVATE data set. The retrievals are then evaluated separately for surface wind speeds below 7 m s−1 and between 7 and 13.3 m s−1 and show that the HSRL-2 retrieves surface wind speeds with a bias of ∼ 0.5 m s−1 and an error of ∼ 1.5 m s−1, a finding not apparent in the cumulative comparisons. Also, it is shown that the HSRL-2 retrievals are more accurate in the summer (−0.18 ± 1.52 m s−1) than in the winter (0.63 ± 2.07 m s−1), but the HSRL-2 is still able to make numerous (N=236) accurate retrievals in the winter. Overall, this study highlights the abilities and assesses the performance of the HSRL-2 surface wind speed retrievals, and it is hoped that further evaluation of these retrievals will be performed using other airborne and satellite data sets.

Enhancing mobile aerosol monitoring with CE376 dual-wavelength depolarization lidar

Abstract. We present the capabilities of a compact dual-wavelength depolarization lidar to assess the spatiotemporal variations in aerosol properties aboard moving vectors. Our approach involves coupling the lightweight Cimel CE376 lidar, which provides measurements at 532 and 808 nm and depolarization at 532 nm, with a photometer to monitor aerosol properties. The assessments, both algorithmic and instrumental, were conducted at ATOLL (ATmospheric Observatory of LiLle) platform operated by the Laboratoire d'Optique Atmosphérique (LOA), in Lille, France. An early version of the CE376 lidar co-located with the CE318-T photometer and with a multi-wavelength Raman lidar were considered for comparisons and validation. We developed a modified Klett inversion method for simultaneous two-wavelength elastic lidar and photometer measurements. Using this setup, we characterized aerosols during two distinct events of Saharan dust and dust smoke aerosols transported over Lille in spring 2021 and summer 2022. For validation purposes, comparisons against the Raman lidar were performed, demonstrating good agreement in aerosol properties with relative differences of up to 12 % in the depolarization measurements. Moreover, a first dataset of CE376 lidar and photometer performing on-road measurements was obtained during the FIREX-AQ (Fire Influence on Regional to Global Environments and Air Quality) field campaign deployed in summer 2019 over the northwestern USA. By lidar and photometer mapping in 3D, we investigated the transport of released smoke from active fire spots at William Flats (northeast WA, USA). Despite extreme environmental conditions, our study enabled the investigation of aerosol optical properties near the fire source, distinguishing the influence of diffuse, convective, and residual smoke. Backscatter, extinction profiles, and column-integrated lidar ratios at 532 and 808 nm were derived for a quality-assured dataset. Additionally, the extinction Ångström exponent (EAE), color ratio (CR), attenuated color ratio (ACR), and particle linear depolarization ratio (PLDR) were derived. In this study, we discuss the capabilities (and limitations) of the CE376 lidar in bridging observational gaps in aerosol monitoring, providing valuable insights for future research in this field.

The Recovery and Re-Calibration of a 13-Month Aerosol Extinction Profiles Dataset from Searchlight Observations from New Mexico, after the 1963 Agung Eruption

The recovery and re-calibration of a dataset of vertical aerosol extinction profiles of the 1963/64 stratospheric aerosol layer measured by a searchlight at 32° N in New Mexico, US, is reported. The recovered dataset consists of 105 aerosol extinction profiles at 550 nm that cover the period from December 1963 to December 1964. It is a unique record of the portion of the aerosol cloud from the March 1963 Agung volcanic eruption that was transported into the Northern Hemisphere subtropics. The data-recovery methodology involved re-digitizing the 105 original aerosol extinction profiles from individual Figures within a research report, followed by the re-calibration. It involves inverting the original equation used to compute the aerosol extinction profile to retrieve the corresponding normalized detector response profile. The re-calibration of the original aerosol extinction profiles used Rayleigh extinction profiles calculated from local soundings. Rayleigh and aerosol slant transmission corrections are applied using the MODTRAN code in transmission mode. Also, a best-estimate aerosol phase function was calculated from observations and applied to the entire column. The tropospheric aerosol phase function from an AERONET station in the vicinity of the searchlight location was applied between 2.76 to 11.7 km. The stratospheric phase function, applied for a 12.2 to 35.2 km altitude range, is calculated from particle-size distributions measured by a high-altitude aircraft in the vicinity of the searchlight in early 1964. The original error estimate was updated considering unaccounted errors. Both the re-calibrated aerosol extinction profiles and the re-calibrated stratospheric aerosol optical depth magnitudes showed higher magnitudes than the original aerosol extinction profiles and the original stratospheric aerosol optical depth, respectively. However, the magnitudes of the re-calibrated variables show a reasonable agreement with other contemporary observations. The re-calibrated stratospheric aerosol optical depth demonstrated its consistency with the tropics-to-pole decreasing trend, associated with the major volcanic eruption stratospheric aerosol pattern when compared to the time-coincident stratospheric aerosol optical depth lidar observations at Lexington at 42° N.

Multi-wavelength dataset of aerosol extinction profiles retrieved from GOMOS stellar occultation measurements

Abstract. In this paper, we present the new multi-wavelength dataset of aerosol extinction profiles, which are retrieved from the averaged transmittance spectra by the Global Ozone Monitoring by Occultation of Stars instrument aboard the Envisat satellite. Using monthly and zonally averaged transmittances as a starting point for the retrievals enables us to improve the signal-to-noise ratio and eliminate possible modulation of transmittance spectra by uncorrected scintillations. The two-step retrieval method is used: the spectral inversion is followed by the vertical inversion. The spectral inversion relies on the removal of contributions from ozone, NO2, NO3 and Rayleigh scattering from the optical depth spectra for each ray perigee altitude. In the vertical inversion, the profiles of aerosol extinction coefficients at several wavelengths are retrieved from the collection of slant aerosol optical depth profiles. The retrieved aerosol extinction profiles (FMI-GOMOSaero dataset v1) are provided in the altitude range 10–40 km at wavelengths of 400, 440, 452, 470, 500, 525, 550, 672 and 750 nm for the whole GOMOS operating period from August 2002 to March 2012. Extensive intercomparisons of the retrieved FMI-GOMOSaero aerosol profiles with aerosol profile data from other satellite instruments at several wavelengths have been performed. It is found that the average difference between FMI-GOMOSaero and other datasets is within 20 %–40 % in the lower and middle stratosphere, the standard deviation is ∼ 20 %–50 %, and the correlation coefficient of the time series is 0.65–0.85. The created FMI-GOMOSaero dataset can be used in merged datasets of stratospheric aerosols. It might be also used as a priori information for satellite retrievals during 2002–2012.

An iterative algorithm to simultaneously retrieve aerosol extinction and effective radius profiles using CALIOP

Abstract. The Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) on board the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite has been widely used in climate and environment studies to obtain the vertical profiles of atmospheric aerosols. To retrieve the vertical profile of aerosol extinction, the CALIOP algorithm assumes column-averaged lidar ratios based on a clustering of aerosol optical properties measured at surface stations. On one hand, these lidar ratio assumptions may not be appropriate or representative at certain locations. One the other hand, the two-wavelength design of CALIOP has the potential to constrain aerosol size information, which has not been considered in the operational algorithm. In this study, we present a modified inversion algorithm to simultaneously retrieve aerosol extinction and effective radius profiles using two-wavelength elastic lidars such as CALIOP. Specifically, a lookup table is built to relate the lidar ratio with the Ångström exponent calculated using aerosol extinction at the two wavelengths, and the lidar ratio is then determined iteratively without a priori assumptions. The retrieved two-wavelength extinction at each layer is then converted to the particle effective radius assuming a lognormal distribution. The algorithm is tested on synthetic data, Raman lidar measurements and then finally the real CALIOP backscatter measurements. Results show improvements over the CALIPSO operational algorithm by comparing with ground-based Raman lidar profiles.

Impacts of spatial heterogeneity of anthropogenic aerosol emissions in a regionally refined global aerosol–climate model

Abstract. Emissions of anthropogenic aerosol and their precursors are often prescribed in global aerosol models. Most of these emissions are spatially heterogeneous at model grid scales. When remapped from low-resolution data, the spatial heterogeneity in emissions can be lost, leading to large errors in the simulation. It can also cause the conservation problem if non-conservative remapping is used. The default anthropogenic emission treatment in the Energy Exascale Earth System Model (E3SM) is subject to both problems. In this study, we introduce a revised emission treatment for the E3SM Atmosphere Model (EAM) that ensures conservation of mass fluxes and preserves the original emission heterogeneity at the model-resolved grid scale. We assess the error estimates associated with the default emission treatment and the impact of improved heterogeneity and mass conservation in both globally uniform standard-resolution (∼ 165 km) and regionally refined high-resolution (∼ 42 km) simulations. The default treatment incurs significant errors near the surface, particularly over sharp emission gradient zones. Much larger errors are observed in high-resolution simulations. It substantially underestimates the aerosol burden, surface concentration, and aerosol sources over highly polluted regions, while it overestimates these quantities over less-polluted adjacent areas. Large errors can persist at higher elevation for daily mean estimates, which can affect aerosol extinction profiles and aerosol optical depth (AOD). We find that the revised treatment significantly improves the accuracy of the aerosol emissions from surface and elevated sources near sharp spatial gradient regions, with significant improvement in the spatial heterogeneity and variability of simulated surface concentration in high-resolution simulations. In the next-generation E3SM running at convection-permitting scales where the resolved spatial heterogeneity is significantly increased, the revised emission treatment is expected to better represent the aerosol emissions as well as their lifecycle and impacts on climate.

The investigation of retrieval method for aerosol and water vapor profiles based on MAX-DOAS technology

The investigation of retrieval method for aerosol and water vapor profiles based on MAX-DOAS technology

Tropospheric sulfate from Cumbre Vieja (La Palma) observed over Cabo Verde contrasted with background conditions: a lidar case study of aerosol extinction, backscatter, depolarization and lidar ratio profiles at 355, 532 and 1064 nm

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.

Lidar AOD inversion and aerosol extinction profile correction method based on GA-BP neural network

Lidar is an effective remote sensing method to obtain the vertical distribution of aerosols, and how to select the aerosol extinction-backscattering ratio (AE-BR) during the inversion process is a key step to guarantee the accuracy of the lidar inversion of aerosol optical thickness (AOD) and aerosol extinction coefficient profile (AECP). In this paper, an inversion algorithm for AOD and AECP based on a genetic BP (GA-BP) neural network is proposed. Simultaneous measurements are carried out using CE318 sun photometer and lidar, and the mapping relationship between the lidar echo signal and AOD is established based on the genetic BP (GA-BP) neural network method, which achieves the accurate inversion of AOD with an absolute error mean value of 0.0156. Based on the AOD output from the GA-BP neural network, the real-time best AE- BR to improve the inversion accuracy of AECP. Finally, practical tests show that the method achieves accurate inversion of AOD, determines the range of AE-BR from 20-50sr, realizes real-time dynamic correction of AECP, and has strong generalization ability and applicability in practical situations.

Silicate Extinction Profile Based on the Stellar Spectrum by Spitzer/IRS

The 9.7 and 18 μm interstellar spectral features, arising from the Si–O stretching and O–Si–O bending modes of amorphous silicate dust, are the strongest extinction features in the infrared. Here we use the “pair method” to determine the silicate extinction profile by comparing the Spitzer/IRS spectra of 49 target stars with obvious extinction with those of unreddened stars of the same spectral type. The 9.7 μm extinction profile is determined from all the 49 stars and the 18 μm profile is determined from six stars. It is found that the profile has a peak wavelength at ∼9.2–9.8 and ∼18–22 μm, respectively. The peak wavelength of the 9.7 μm feature seems to become shorter for stars of late spectral types; meanwhile the FWHM seems irrelevant to the spectral type, which may be related to circumstellar silicate emission. The silicate optical depth at 9.7 μm, Δτ 9.7, mostly increases with the color excess in J − K S ( EJKS ). The mean ratio of the visual extinction to the 9.7 μm silicate absorption optical depth is A V /Δτ 9.7 ≈ 17.8, in close agreement with that of the solar-neighborhood diffuse interstellar medium. When EJKS>4 , this proportionality changes. The correlation coefficient between the peak wavelength and the FWHM of the 9.7 μm feature is 0.4, which indicates a positive correlation considering the uncertainties of the parameters. The method is compared with replacing the reference star by an atmospheric model spectral energy distribution and no significant difference is observed.