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At least 19 records

Vertically Resolved Retrievals of Aerosol Concentrations and Effective Radii from the DOE Combined HSRL and Raman lidar Measurement Study (CHARMS) Merged High-Spectral-Resolution Lidar-Raman Lidar Data Set

The Department of Energy’s (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility is a key component of DOE’s research strategy to address global climate change. The objective of the ARM Facility is to provide an experimental testbed for studying important atmospheric effects, particularly cloud and aerosol processes, and testing parameterizations of these processes for use in climate change models. ARM observational sites include a broad array of instruments to characterize cloud and aerosol properties, atmospheric state variables, and incoming and outgoing radiation. Advanced lidar systems provide valuable and unique information about the atmospheric column. We examine the potential for providing vertically resolved information about aerosol size and concentration with a combination of two such lidar systems, the Raman lidar and the High-Spectral-Resolution Lidar (HSRL). Currently ARM has a limited ability to remotely measure profiles of aerosol optical and microphysical properties on an operational basis. Although the Southern Great Plains (SGP), Eastern North Atlantic (ENA), and North Slope of Alaska (NSA, Oliktok Point location only) Raman lidars provide profiles of aerosol backscatter and extinction at 355 nm, additional information is required to better characterize the impacts of aerosols on radiation and clouds. Recent advances in lidar retrieval theory and algorithm development (Müller et al. 1999, 2014; Chemyakin et al. 2014) demonstrate that multi-wavelength lidar retrieval algorithms that use measurements of aerosol extinction at both 355 and 532 nm and backscatter at 355, 532, and 1064 nm have the potential to constrain both the aerosol optical (e.g., complex index of refraction, scattering, etc.) and microphysical properties (e.g., effective radius, concentration). This advancement greatly increases the utility of the remote-sensed aerosol observations. Based on this work, the HSRL group at the National Aeronautics and Space Administration (NASA)’s Langley Research Center (LaRC) developed automated algorithms for retrieving aerosol optical and microphysical properties, demonstrated these retrievals using data from the unique NASA/LaRC airborne multi-wavelength HSRL-2 system, and validated these retrievals using coincident airborne in situ data (Müller et al. 2014; Sawamura et al. 2017). We report here on the use of ARM instrumentation to gather a multi-wavelength ground-based lidar data set to test such retrievals. Continuous (24/7) operation of the co-located SGP Raman lidar and University of Wisconsin (UW) HSRL during the 10-week Combined HSRL and Raman lidar Measurement Study (CHARMS) (mid-July through September 2015) allowed the acquisition of a unique, multi-wavelength ground-based lidar data set. The ARM SGP Raman lidar (RLID) measured profiles of aerosol backscatter, extinction, and depolarization at 355 nm and profiles of water vapor mixing ratio and temperature. The UW HSRL simultaneously measured profiles of aerosol backscatter, extinction and depolarization at 532 nm and aerosol backscatter at 1064 nm. This RLID+HSRL combination provided a test data set to investigate these more advanced aerosol retrieval techniques with the potential to greatly improve aerosol characterization in the lower atmosphere.

54 ENVIRONMENTAL SCIENCES↗

Final Technical Report for Interagency Agreement No. DE-SC0005453 “Characterizing Aerosol Distributions, Types, and Optical and Microphysical Properties using the NASA Airborne High Spectral Resolution Lidar (HSRL) and the Research Scanning Polarimeter (RSP)”

Measurements of the vertical profile of atmospheric aerosols and aerosol optical and microphysical characteristics are required to: 1) determine aerosol direct and indirect radiative forcing, 2) compute radiative flux and heating rate profiles, 3) assess model simulations of aerosol distributions and types, and 4) establish the ability of surface and space-based remote sensors to measure the indirect effect. Consequently the ASR program calls for a combination of remote sensing and in situ measurements to determine aerosol properties and aerosol influences on clouds and radiation. As part of our previous DOE ASP project, we deployed the NASA Langley airborne High Spectral Resolution Lidar (HSRL) on the NASA B200 King Air aircraft during major field experiments in 2006 (MILAGRO and MaxTEX), 2007 (CHAPS), 2009 (RACORO), and 2010 (CalNex and CARES). The HSRL provided measurements of aerosol extinction (532 nm), backscatter (532 and 1064 nm), and depolarization (532 and 1064 nm). These measurements were typically made in close temporal and spatial coincidence with measurements made from DOE-funded and other participating aircraft and ground sites. On the RACORO, CARES, and CalNEX missions, we also deployed the NASA Goddard Institute for Space Studies (GISS) Research Scanning Polarimeter (RSP). RSP provided intensity and degree of linear polarization over a broad spectral and angular range enabling column-average retrievals of aerosol optical and microphysical properties. Under this project, we analyzed observations and model results from RACORO, CARES, and CalNex and accomplished the following objectives. 1. Identified aerosol types, characterize the vertical distribution of the aerosol types, and partition aerosol optical depth by type, for CARES and CalNex using HSRL data as we have done for previous missions. 2. Investigated aerosol microphysical and macrophysical properties using the RSP. 3. Used the aerosol backscatter and extinction profiles measured by the HSRL to characterize the planetary boundary layer height (PBL) and the transition zone thickness, for the RACORO and CARES and CalNex campaigns as we have done for previous campaigns. 4. Investigated how optical properties measured by HSRL vary near clouds. 5. Assessed model simulations of aerosol spatial distributions and optical and microphysical properties.

54 ENVIRONMENTAL SCIENCES↗

hsrl (01)

High-spectral-resolution lidar (HSRL) systems collect data about clouds and aerosols. These systems provide vertical profiles of optical depth, backscatter cross-section, depolarization, and backscatter phase function. All HSRL measurements are absolutely calibrated by reference to molecular scattering, which is measured at each point in the lidar profile. Like the Raman lidar, but unlike simple backscatter lidars such as the micropulse lidar, the HSRL can measure backscatter cross-sections and optical depths without prior assumptions about the scattering properties of the atmosphere. The depolarization observations also allow robust discrimination between ice and water clouds. In addition, rigorous error estimates can be computed for all measurements. A very narrow, angular field of view reduces multiple scattering contributions. The small field of view, coupled with a narrow optical bandwidth, nearly eliminates noise due to scattered sunlight. ARM operates two HSRL systems, one at the Barrow, North Slope of Alaska (NSA) site and the other in the second ARM Mobile Facility (AMF2), which is deployed at various locations on field campaigns.

54 ENVIRONMENTAL SCIENCES↗

hsrl (00)

High-spectral-resolution lidar (HSRL) systems collect data about clouds and aerosols. These systems provide vertical profiles of optical depth, backscatter cross-section, depolarization, and backscatter phase function. All HSRL measurements are absolutely calibrated by reference to molecular scattering, which is measured at each point in the lidar profile. Like the Raman lidar, but unlike simple backscatter lidars such as the micropulse lidar, the HSRL can measure backscatter cross-sections and optical depths without prior assumptions about the scattering properties of the atmosphere. The depolarization observations also allow robust discrimination between ice and water clouds. In addition, rigorous error estimates can be computed for all measurements. A very narrow, angular field of view reduces multiple scattering contributions. The small field of view, coupled with a narrow optical bandwidth, nearly eliminates noise due to scattered sunlight. ARM operates two HSRL systems, one at the Barrow, North Slope of Alaska (NSA) site and the other in the second ARM Mobile Facility (AMF2), which is deployed at various locations on field campaigns.

54 ENVIRONMENTAL SCIENCES↗

High-Spectral Resolution Lidar (HSRL) Instrument Handbook

High-spectral-resolution lidar (HSRL) systems provide vertical profiles of optical depth, backscatter cross-section, depolarization, and backscatter phase function. All HSRL measurements are calibrated by reference to molecular scattering, which is measured at each point in the lidar profile. Like the Raman lidar (RL), but unlike simple backscatter lidars such as the micropulse lidar (MPL), this enables the HSRL to measure backscatter cross-sections and optical depths without prior assumptions about the scattering properties of the atmosphere. The depolarization observations allow robust discrimination between ice and water clouds. Rigorous error estimates can be computed for all measurements. A very narrow angular field of view reduces multiple scattering contributions. The small field of view, coupled with a narrow optical bandwidth, nearly eliminates noise due to scattered sunlight. The laser transmitter is a diode-pumped, frequency-doubled Nd:YAG laser. Narrow-band, single-frequency operation is provided by injection seeding with a single-frequency, cw-diode-pumped diode laser. The main laser cavity is maintained in resonance with the seed laser by adjusting the cavity length to minimize the time between the Q-switch trigger and the emission of the laser pulse. The emission wavelength is tuned via temperature control of the seed laser crystal and is locked to line #1109 of the iodine absorption spectra. Locking is accomplished by minimizing the transmission through a 2-cm-long iodine absorption cell. Use of a high-repetition-rate laser and expansion of the transmitted beam through a 400-mm telescope reduces the transmitted energy density to eye-safe levels. It is possible to look directly into the output beam without hazard. The receiver and transmitter use the same afocal telescope, simplifying the maintenance of stable alignment of the transmitter and receiver although the angular FOV is only 100 μrad. The small FOV and the 4-kHz repetition rate also limit the near-field signal strength, making it possible to record continuous profiles that start at an altitude of ~100 m and extend to 30 km using photon counting detectors. The small FOV also suppresses multiple scattering contributions.

54 ENVIRONMENTAL SCIENCES↗

Airborne Multiwavelength High Spectral Resolution Lidar (HSRL-2) observations during TCAP 2012: vertical profiles of optical and microphysical properties of a smoke/urban haze plume over the northeastern coast of the US

Here, we present measurements acquired by the world's first airborne 3 backscatter (β) + 2 extinction (α) High Spectral Resolution Lidar (HSRL-2). HSRL-2 measures particle backscatter coefficients at 355, 532, and 1064 nm, and particle extinction coefficients at 355 and 532 nm. The instrument has been developed by the NASA Langley Research Center. The instrument was operated during Phase 1 of the Department of Energy (DOE) Two-Column Aerosol Project (TCAP) in July 2012. We observed pollution outflow from the northeastern coast of the US out over the western Atlantic Ocean. Lidar ratios were 50–60 sr at 355 nm and 60–70 sr at 532 nm. Extinction-related Ångström exponents were on average 1.2–1.7, indicating comparably small particles. Our novel automated, unsupervised data inversion algorithm retrieved particle effective radii of approximately 0.2 μm, which is in agreement with the large Angstrom exponents. We find good agreement with particle size parameters obtained from coincident in situ measurements carried out with the DOE Gulfstream-1 aircraft.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

HSRL Liquid cloud base height (nsaC1)

Liquid layers in clouds affect their microphysical processes, as well as the surface energy budget. Studies focusing on these and other areas of research are often in need of skillful estimation of liquid-bearing cloud-layer boundaries. The bases of these layers are predominantly determined by ground-based lidar instruments. Most studies requiring liquid cloud base height (LCBH) information use either fixed lidar depolarization and/or backscatter cross-section thresholds or cloud base height data products that do not distinguish between ice and liquid, all of which might introduce inconsistencies and errors in the resolved LCBH. This data set contains LCBH data at 1-min temoporal resolution based on an explicit LCBH detection algorithm, which uses the high-spectral-resolution lidar (HSRL) data. Examination of this algorithm in multiple cases and scenarios during numerous days and first-order comparison with microwave-radiometer data show satisfactory results.

54 ENVIRONMENTAL SCIENCES↗

HSRL Liquid cloud base height

Liquid layers in clouds affect their microphysical processes, as well as the surface energy budget. Studies focusing on these and other areas of research are often in need of skillful estimation of liquid-bearing cloud-layer boundaries. The bases of these layers are predominantly determined by ground-based lidar instruments. Most studies requiring liquid cloud base height (LCBH) information use either fixed lidar depolarization and/or backscatter cross-section thresholds or cloud base height data products that do not distinguish between ice and liquid, all of which might introduce inconsistencies and errors in the resolved LCBH. This data set contains LCBH data at 1-min temoporal resolution based on an explicit LCBH detection algorithm, which uses the high-spectral-resolution lidar (HSRL) data. Examination of this algorithm in multiple cases and scenarios during numerous days and first-order comparison with microwave radiometer data show satisfactory results.

54 ENVIRONMENTAL SCIENCES↗

Combined High Spectral Resolution Lidar and Millimeter Wavelength Radar Measurement of Ice Crystal Precipitation

The goal of this research has been to improve measurements of snowfall using a combination of millimeter-wavelength radar and High Spectral Resolution Lidar (HSRL) Observations. Snowflakes are large compared to the 532nm HSRL wavelength and small compared to the 3.2 and 8.6 mm wavelength radars used in this study. This places the particles in the optical scattering regime of the HSRL, where extinction cross-section is proportional to the projected area of the particles, and in the Rayleigh regime for the radar, where the backscatter cross-section is proportional to the mass-squared of the particles. Forming a ratio of the radar measured cross-section to the HSRL measured cross section eliminates any dependence on the number of scattering particles, yielding a quantity proportional to the average mass-squared of the snowflakes over the average area of the flakes. Using simultaneous radar measurements of particle fall velocities, which are dependent particle mass and cross-sectional area it is possible to derive the average mass of the snow flakes, and with the radar measured fall velocities compute the snowfall rate. Since this retrieval requires the optical extinction cross-section we began by considering errors this quantity. The HSRL is particularly good at measuring the backscatter cross-section. In previous studies of snowfall in the high Arctic were able to estimate the extinction cross-section directly as a fixed ratio to the backscatter cross-section. Measurements acquired in the STORMVEX experiment in Colorado showed that this approach was not valid in mid-latitude snowfalls and that direct measurement of the extinction cross-section is required. Attempts to measure the extinction directly uncovered shortcomings in thermal regulation and mechanical stability of the newly deployed DOE HSRL systems. These problems were largely mitigated by modifications installed in both of the DOE systems. We also investigated other sources of error in the HSRL direct measurement of extinction (see appendix II of this report). We also developed improved algorithms to extract extinction from the HSRL data. These have been installed in the standard HSRL data processing software and are now available to all users of HSRL data. Validation of snowfall measurements has proven difficult due to the unreliability of conventional snowfall measurements coupled with the complexity of considering the vast variety of snowflake geometries. It was difficult to tell how well the algorithm’s approach to accommodating differences in snowflakes was working without good measurements for comparison. As a result, we decided to apply this approach to the somewhat simpler, but scientifically important, problem of drizzle measurement. Here the particle shape is known and the conventional measurement are more reliable. These algorithms where successfully applied to drizzle data acquired during the ARM MAGIC study of marine stratus clouds between California and Hawaii (see Appendix I). This technique is likely to become a powerful tool for studying lifetime of the climatically important marine stratus clouds.

47 OTHER INSTRUMENTATION↗

Comparison of Mixed Layer Heights from Airborne High Spectral Resolution Lidar, Ground-based Measurements, and the WRP-Chem Model during CalNex and CARES

The California Research at the Nexus of Air Quality and Climate Change (CalNex) and Carbonaceous Aerosol and Radiative Effects Study (CARES) field campaigns during May and June 2010 provided a data set appropriate for studying characteristics of the planetary boundary layer (PBL). The NASA Langley Research Center (LaRC) airborne High Spectral Resolution Lidar (HSRL) was deployed to California onboard the NASA LaRC B-200 aircraft to aid incharacterizing aerosol properties during these two field campaigns. Measurements of aerosol extinction (532 nm), backscatter (532 and 1064 nm), and depolarization (532 and 1064 nm) profiles during 31 flights, many in coordination with other research aircraft and ground sites, constitute a diverse data set for use in characterizing the spatial and temporal distribution of aerosols, as well as the depth and variability of the daytime mixed layer (ML), which is a subset within the PBL. This work illustrates the temporal and spatial variability of the ML in the vicinity of Los Angeles and Sacramento, CA. ML heights derived from HSRL measurements are compared to PBL heights derived from radiosonde profiles, ML heights measured from ceilometers, and simulated PBL heights from the Weather Research and Forecasting Chemistry (WRF-Chem) community model. Comparisons between the HSRL ML heights and the radiosonde profiles in Sacramento result in a correlation coefficient value (R) of 0.93 (root7 mean-square (RMS) difference of 157 m and bias difference (HSRL radiosonde) of 5 m). HSRL ML heights compare well with those from the ceilometer in the LA Basin with an R of 0.89 (RMS difference of 108 m and bias difference (HSRL Ceilometer) of -9.7 m) for distances of up to 30 km between the B-200 flight track and the ceilometer site. Simulated PBL heights from WRF-Chem were compared with those obtained from all flights for each campaign, producing an R of 0.58 (RMS difference of 604 m and a bias difference (WRF-Chem HSRL) of -157 m) for CalNex and 0.59 (RMS difference of 689 m and a bias difference (WRF-Chem HSRL) of 220 m) for CARES. Aerosol backscatter simulations are also available from WRF15 Chem and are compared to those from HSRL to examine differences among the methods used to derive ML heights.

Scarino, Amy Jo↗

Boundary Layer Structures Over the Northwest Atlantic Derived From Airborne High Spectral Resolution Lidar and Dropsonde Measurements During the ACTIVATE Campaign

The Planetary Boundary Layer height (PBLH) is essential for studying PBL and ocean-atmosphere interactions. Marine PBL is usually defined to include a mixed layer (ML) and a capping inversion layer. The ML height (MLH) estimated from the measurements of aerosol backscatter by a lidar was usually compared with PBLH determined from radiosondes/dropsondes in the past, as the PBLH is usually similar to MLH in nature. However, PBLH can be much greater than MLH for decoupled PBL. Here, in this study, we evaluate the retrieved MLH from an airborne lidar (HSRL-2) by utilizing 506 co-located dropsondes during the ACTIVATE field campaign over the Northwest Atlantic from 2020 to 2022. First, we define and determine the MLH and PBLH from the temperature and humidity profiles of each dropsonde, and find that the MLH values from HSRL-2 and dropsondes agree well with each other, with a coefficient of determination of 0.66 and median difference of 18 m. In contrast, the HSRL-2 MLH data do not correspond to dropsonde-derived PBLH, with a median difference of -47 m. Therefore, we modify the current operational and automated HSRL-2 wavelet-based algorithm for PBLH retrieval, decreasing the median difference significantly to -8 m. Further data analysis indicates that these conclusions remain the same for cases with higher or lower cloud fractions, and for decoupled PBLs. These results demonstrate the potential of using HSRL-2 aerosol backscatter data to estimate both marine MLH and PBLH and suggest that lidar-derived MLH should be compared with radiosonde/dropsonde-determined MLH (not PBLH) in general.

54 ENVIRONMENTAL SCIENCES↗

Elevated aerosol layers modify the O2–O2 absorption measured by ground-based MAX-DOAS

The oxygen collisional complex (O2-O2, or O4) is a greenhouse gas, and a calibration trace gas used to infer aerosol and cloud properties by Differential Optical Absorption Spectroscopy (DOAS). Recent reports suggest the need for an O4 correction factor (CFO4) when comparing simulated and measured O4 differential slant column densities (dSCD) by passive DOAS. We investigate the sensitivity of O4 dSCD simulations at ultraviolet (360 nm) and visible (477 nm) wavelengths towards separately measured aerosol extinction profiles. Measurements were conducted by the University of Colorado 2D-MAX-DOAS instrument and NASA’s multispectral High Spectral Resolution Lidar (HSRL-2) during the Two Column Aerosol Project (TCAP) at Cape Cod, MA in July 2012. During two case study days with (1) high aerosol load (17 July, AOD ~ 0.35 at 477 nm), and (2) near molecular scattering conditions (22 July, AOD < 0.10 at 477 nm) the measured and calculated O4 dSCDs agreed within 6.4±0.4% (360 nm) and 4.7±0.6% (477 nm) if the HSRL-2 profiles were used as input to the calculations. However, if in the calculations the aerosol is confined to the surface layer (while keeping AOD constant) we find 0.53<CFO4<0.75, similar to previously reported CFO4. Our results suggest that elevated aerosol layers, unless accounted for, can cause negative bias in the simulated O4 dSCDs that can explain CFO4. The air density and aerosol profile aloft needs to be taken into account when interpreting the O4 from ground-based MAX-DOAS. Opportunities to identify and better characterize these layers are also discussed.

54 ENVIRONMENTAL SCIENCES↗

Merged Cloud and Precipitation Dataset from the HIAPER GV for the Cloud System Evolution in the Trades (CSET) Campaign

The Cloud System Evolution in the Trades (CSET) aircraft campaign was conducted in the summer of 2015 in the northeast Pacific to observe the transition from stratocumulus to cumulus cloud regime. Fourteen transects were made between Sacramento, California, and Kona, Hawaii, using the NCAR's High-Performance Instrumented Airborne Platform for Environmental Research (HIAPER) Gulfstream V (GV) aircraft. The HIAPER W-band Doppler cloud radar (HCR) and the high-spectral-resolution lidar (HSRL), in their first deployment together on board the GV, provided crucial cloud and precipitation observations. The HCR recorded the raw in-phase (I) and quadrature (Q) components of the digitized signal, from which the Doppler spectra and its first three moments were calculated. HCR/HSRL data were merged to develop a hydrometeor mask on a uniform georeferenced grid of 2-Hz temporal and 20-m vertical resolutions. The hydrometeors are classified as cloud or precipitation using a simple fuzzy logic technique based on the HCR mean Doppler velocity, HSRL backscatter, and the ratio of HCR reflectivity to HSRL backscatter. This is primarily applied during zenith-pointing conditions under which the lidar can detect the cloud base and the radar is more sensitive to clouds. The microphysical properties of below-cloud drizzle and optically thin clouds were retrieved using the HCR reflectivity, HSRL backscatter, and the HCR Doppler spectrum width after it is corrected for the aircraft speed. These indicate that as the boundary layers deepen and cloud-top heights increase toward the equator, both the cloud and rain fractions decrease.

54 ENVIRONMENTAL SCIENCES↗

The CU 2-D-MAX-DOAS instrument – Part 2: Raman scattering probability measurements and retrieval of aerosol optical properties

Abstract. The multiannual global mean of aerosol optical depth at 550 nm (AOD550) over land is ∼ 0.19, and that over oceans is ∼ 0.13. About 45 % of the Earth surface shows AOD550 smaller than 0.1. There is a need for measurement techniques that are optimized to measure aerosol optical properties under low AOD conditions. We present an inherently calibrated retrieval (i.e., no need for radiance calibration) to simultaneously measure AOD and the aerosol phase function parameter, g, based on measurements of azimuth distributions of the Raman scattering probability (RSP), the near-absolute rotational Raman scattering (RRS) intensity. We employ radiative transfer model simulations to show that for solar azimuth RSP measurements at solar elevation and solar zenith angle (SZA) smaller than 80°, RSP is insensitive to the vertical distribution of aerosols and maximally sensitive to changes in AOD and g under near-molecular scattering conditions. The University of Colorado two-dimensional Multi-AXis Differential Optical Absorption Spectroscopy (CU 2-D-MAX-DOAS) instrument was deployed as part of the Two Column Aerosol Project (TCAP) at Cape Cod, MA, during the summer of 2012 to measure direct sun spectra and RSP from scattered light spectra at solar relative azimuth angles (SRAAs) between 5 and 170°. During two case study days with (1) high aerosol load (17 July, 0.3 < AOD430 < 0.6) and (2) near-molecular scattering conditions (22 July, AOD430 < 0.13) we compare RSP-based retrievals of AOD430 and g with data from a co-located CIMEL sun photometer, Multi-Filter Rotating Shadowband Radiometer (MFRSR), and an airborne High Spectral Resolution Lidar (HSRL-2). The average difference (relative to DOAS) for AOD430 is +0.012 ± 0.023 (CIMEL), −0.012 ± 0.024 (MFRSR), −0.011 ± 0.014 (HSRL-2), and +0.023 ± 0.013 (CIMELAOD − MFRSRAOD) and yields the following expressions for correlations between different instruments: DOASAOD = −(0.019 ± 0.006) + (1.03 ± 0.02) × CIMELAOD (R2 = 0.98), DOASAOD = −(0.006 ± 0.005) + (1.08 ± 0.02) × MFRSRAOD (R2 = 0.98), and CIMELAOD = (0.013 ± 0.004) + (1.05 ± 0.01) × MFRSRAOD (R2 = 0.99). The average g measured by DOAS on both days was 0.66 ± 0.03, with a difference of 0.014 ± 0.05 compared to CIMEL. Active steps to minimize the error in the RSP help to reduce the uncertainty in retrievals of AOD and g. As AOD decreases and SZA increases, the RSP signal-to-noise ratio increases. At AOD430 ∼ 0.4 and 0.10 the absolute AOD errors are ∼ 0.014 and 0.003 at 70° SZA and 0.02 and 0.004 at 35° SZA. Inherently calibrated, precise AOD and g measurements are useful to better characterize the aerosol direct effect in urban polluted and remote pristine environments.

54 ENVIRONMENTAL SCIENCES↗

On the differences in the vertical distribution of modeled aerosol optical depth over the southeastern Atlantic

Abstract. The southeastern Atlantic is home to an expansive smoke aerosol plume overlying a large cloud deck for approximately a third of the year. The aerosol plume is mainly attributed to the extensive biomass burning activities that occur in southern Africa. Current Earth system models (ESMs) reveal significant differences in their estimates of regional aerosol radiative effects over this region. Such large differences partially stem from uncertainties in the vertical distribution of aerosols in the troposphere. These uncertainties translate into different aerosol optical depths (AODs) in the planetary boundary layer (PBL) and the free troposphere (FT). This study examines differences of AOD fraction in the FT and AOD differences among ESMs (WRF-CAM5, WRF-FINN, GEOS-Chem, EAM-E3SM, ALADIN, GEOS-FP, and MERRA-2) and aircraft-based measurements from the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) field campaign. Models frequently define the PBL as the well-mixed surface-based layer, but this definition misses the upper parts of decoupled PBLs, in which most low-level clouds occur. To account for the presence of decoupled boundary layers in the models, the height of maximum vertical gradient of specific humidity profiles from each model is used to define PBL heights. Results indicate that the monthly mean contribution of AOD in the FT to the total-column AOD ranges from 44 % to 74 % in September 2016 and from 54 % to 71 % in August 2017 within the region bounded by 25∘ S–0∘ N–S and 15∘ W–15∘ E (excluding land) among the ESMs. ALADIN and GEOS-Chem show similar aerosol plume patterns to a derived above-cloud aerosol product from the Moderate Resolution Imaging Spectroradiometer (MODIS) during September 2016, but none of the models show a similar above-cloud plume pattern to MODIS in August 2017. Using the second-generation High Spectral Resolution Lidar (HSRL-2) to derive an aircraft-based constraint on the AOD and the fractional AOD, we found that WRF-CAM5 produces 40 % less AOD than those from the HSRL-2 measurements, but it performs well at separating AOD fraction between the FT and the PBL. AOD fractions in the FT for GEOS-Chem and EAM-E3SM are, respectively, 10 % and 15 % lower than the AOD fractions from the HSRL-2. Their similar mean AODs reflect a cancellation of high and low AOD biases. Compared with aircraft-based observations, GEOS-FP, MERRA-2, and ALADIN produce 24 %–36 % less AOD and tend to misplace more aerosols in the PBL. The models generally underestimate AODs for measured AODs that are above 0.8, indicating their limitations at reproducing high AODs. The differences in the absolute AOD, FT AOD, and the vertical apportioning of AOD in different models highlight the need to continue improving the accuracy of modeled AOD distributions. These differences affect the sign and magnitude of the net aerosol radiative forcing, especially when aerosols are in contact with clouds.

54 ENVIRONMENTAL SCIENCES↗