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NASA NTRS2020

High Resolution Global Coupled Chemistry-Meteorology Simulations Using the NASA GEOS Composition Forecast System, GEOS-CF

We will give an overview of the NASA Global Earth Observing System Composition Forecast system (GEOS-CF), a high-resolution (0.25 degree) global composition model developed by the NASA Global Modeling and Assimilation Office (GMAO). This system combines the GEOS weather and aerosol model with the GEOS-Chem chemistry module (version 12) to provide a holistic view of atmospheric composition that captures a wide range of air pollutants such as ozone, nitrogen oxides, volatile organic compounds, and fine particulate matter. The spatial resolution of 0.25 degrees (approx. 25 km) is fine enough to resolve local features such as nighttime ozone titration previously resolved only by urban or regional models. Furthermore, since there are no boundary conditions for a global model, the GEOS-CF captures large-scale processes such as long-range transport of air pollutants from forest fires. Comparisons against surface observations highlight the model’s overall capability to reproduce the diurnal variability of air pollutants under a variety of meteorological conditions. In addition, we show how machine learning techniques can be used to correct for sub-grid variability, which further improves model estimates at a given surface observation site. The GEOS-CF system offers a new tool for scientists and the public health community alike and is being developed jointly with several government and non-profit partners. As an example, we will show the use of GEOS-CF during the Satellite Coastal and Oceanic Atmospheric Pollution Experiment (SCOAPE). The campaign, conducted in collaboration between NASA and the Bureau of Ocean Energy Management (BOEM), aims to investigate the response of onshore air quality to Outer Continental Shelf (OCS) oil and gas exploration, development and production. Detailed gas-phase chemistry, as provided by GEOS-CF, is critical to understand the formation of air pollution related to hydrocarbon emissions from offshore oil and gas activities. The accuracy of GEOS-CF can be further improved by incorporating detailed offshore emissions compiled by BOEM.

Knowland, K. Emma↗

NASA NTRS2015

Total Dust Deposition Flux During Precipitation in Toyama, Japan, in the Spring of 2009: A Sensitivity Analysis with the NASA GEOS-5 Model

We compared the observed total dust deposition fluxes during precipitation (TDP) mainly at Toyama in Japan during the period January - April 2009 with results available from four NASA GEOS-5 global model experiments. The modeled results were obtained from three previous experiments and carried out in one experiment, which were all driven by assimilated meteorology and simulating aerosol distributions for the time period. We focus mainly on the observations of two distinct TDP events, which were reported in Osada et al. (2011), at Toyama, Japan, in February (Event B) and March 2009 (Event C). Although all of our GEOS-5 simulations captured aspects of the observed TDP, we found that our low horizontal spatial resolution control experiment performed generally the worst. The other three experiments were run at a higher spatial resolution, with the first differing only in that respect from the control, the second adding imposed a prescribed corrected precipitation product, and the final experiment adding as well assimilation of aerosol optical depth based on MODIS observations. During Event C, the increased horizontal resolution could increase TDP with precipitation increase. There was no significant improvement, however, due to the imposition of the corrected precipitation product. The simulation that incorporated aerosol data assimilation performed was by far the best for this event, but even so could only reproduce less than half of the observed TDP despite the significantly increased atmospheric dust mass concentrations. All three of the high spatial resolution experiments had higher simulated precipitation at Toyama than was observed and that in the lower resolution control run. During Event B, the aerosol data assimilation run did not perform appreciably better than the other higher resolution simulations, suggesting that upstream conditions (i.e., upstream cloudiness), or vertical or horizontal misplacement of the dust plume did not allow for significant improvement in the simulated aerosol distributions. Furthermore, a detailed comparison of observed hourly precipitation and surface particulate mass concentration data suggests that the observed TDP during Event B was highly dependent on short periods of weak precipitation correlated with elevated dust surface concentrations, important details possibly not captured well in a current global model.

Dust; Wet deposition; Numerical modeling; Japan; P↗

NASA NTRS2014

Systematic Satellite Observations of the Impact of Aerosols from Passive Volcanic Degassing on Local Cloud Properties

The impact of volcanic emissions is a significant source of uncertainty in estimations of aerosol indirect radiative forcing, especially with respect to emissions from passive de-gassing and minor explosions. Understanding the impact of volcanic emissions on indirect radiative forcing is important assessing present day atmospheric properties and also to define the pre-industrial baseline to assess anthropogenic perturbations. We present observations of the time-averaged indirect aerosol effect within 200 km downwind of isolated island volcanoes in regions of low present-day aerosol burden using MODIS and AATSR data. Retrievals of aerosol and cloud properties at Kilauea (Hawaii), Yasur (Vanuatu) and Piton de la Fournaise (Reunion) are rotated about the volcanic vent according to wind direction, so that retrievals downwind of the volcano can be averaged to improve signal to noise ratio. The emissions from all three volcanoes, including those from passive degassing, strombolian activity and minor explosions lead to measurably increased aerosol optical depth downwind of the active vent. Average cloud droplet effective radius is lower downwind of the volcano in all cases, with the peak difference in effective radius ranging from 48 microns at the different volcanoes. A comparison of these observations with cloud properties at isolated islands with no significant source of aerosol suggests that these patterns are not purely orographic in origin. This approach sets out a first step for the systematic measurement of the effects of present day low altitude volcanic emissions on cloud properties, and our observations of unpolluted, isolated marine settings may capture processes similar to those in the preindustrial marine atmosphere.

cloud properties↗

DOE OSTI2020

Second ARM Aerosol Chemical Speciation Monitor Users’ Meeting Report

The aerosol chemical speciation monitor (ACSM) was developed to adapt the technology of the aerosol mass spectrometer (AMS) to routine, long-term, standalone monitoring. The calculation of particulate mass concentration from ACSM data requires the measurement of the response of the instrument to aerosol of specific size and composition as well as assumptions about the instrument response based on laboratory measurements and field experience acquired over more than two decades of operation of AMS and a decade of operation of the ACSM. Three parameters in the concentration calculations that are particularly important are the NO3 response factor (RFNO3), relative ionization efficiency (RIE), and the collection efficiency (CE). The values of RFNO3 and RIEs are determined from calibration, however the jump calibration method previously used in calibration can result in errors in the RIE for sulfate. This has been corrected by implementing a continuous calibration method. The default collection efficiency is 0.5. This has been shown to result in mass loadings that do not agree with mass determinations from other instruments because of effects of composition on the vaporization of the particles. The previous work of investigators addressing this issue is discussed. After preliminary work on ACSM and scanning mobility particle sizer (SMPS) data from the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility Southern Great Plains (SGP) observatory collected in late 2016 and 2017 produced a parameterization of composition dependent collection efficiency very different from the results of previous studies, SMPS data were examined and we determined that there was significant mass that the instrument did not capture because the particles with diameters larger than 465 nm are not counted by this instrument. Data for the ultra-high-sensitivity aerosol spectrometer (UHSAS), SMPS, and ACSM are available for nearly all of 2019. The data from UHSAS and SMPS collected in 2019 were compared. We found that the UHSAS data has particle counts and total volumes significantly less than measured by the condensation particle counter (CPC) and SMPS. The SMPS data were extended by fitting the average volume distribution with a log normal curve and using this relationship to estimate a mass value for the SMPS over extended diameter range. The extended SMPS mass values result in a CDCE parameterization that is in better agreement with the results of other investigators, but is still different from other formulations. The working group recommends that the ACSM data be processed with a collective efficiency (CE)=1, that this be documented clearly in the metadata, and the use of the default CE of 0.5 or a formulation of composition-dependent collection efficiencies (CDCE) chosen by the user should be implemented based on the ammonium nitrate mass fraction. This is clearly necessary for the wintertime SGP ACSM data because of the high nitrate concentrations.

47 OTHER INSTRUMENTATION↗

NASA NTRS2008

The On-Orbit Performance of the CALIOP Lidar on CALIPSO

CALIPSO is a joint NASA - CNES satellite currently in its third year of operation in low earth orbit. The satellite is making optical measurements of the Earth s atmosphere to help quantify the impact of aerosols and clouds on the Earth s radiation budget. To do this, it carries three instruments: CALIOP, a two-wavelength polarization-sensitive elastic backscatter lidar; the IIR a three band thermal imaging radiometer; and the WFC a visible single-band imager. CALIOP utilizes a Nd:YAG laser which incorporates a harmonic crystal to provide laser light at both 1064 nm and 532 nm. This beam is expanded and transmitted into the atmosphere at near nadir. The laser light scattered from clouds and aerosols back to the satellite, along with any solar background light, is collected by a one meter diameter beryllium telescope. The captured light is separated into its two wavelengths and optically filtered. The 1064 nm component is detected with an avalanche photodiode, while the 532 nm component is further resolved into two linear polarization components which are then detected by matching photomultiplier tubes. This presentation will describe the lidar and give examples of its on-orbit performance.

Winker, David↗

DOE OSTI2022

Monitoring Xenon Capture in a Metal Organic Framework Using Laser-Induced Breakdown Spectroscopy

Molten salt reactor operation will necessitate circulation of a cover gas to remove certain evolved fission products and maintain an inert atmosphere. The cover gas leaving the reactor core is expected to contain both noble and non-noble gases, aerosols, volatile species, tritium, and radionuclides and their daughters. To remove these radioactive gases, it is necessary to develop a robust off-gas system, along with novel sensors to monitor the gas stream and the treatment system performance. In this study, a metal organic framework (MOF) was engineered for the capture of Xe, a major contributor to the off-gas source term. The engineered MOF column was tested with a laser-induced breakdown spectroscopy (LIBS) sensor for noble gas monitoring. The LIBS sensor was used to monitor breakthrough tests with various Xe, Kr, and Ar mixtures to determine the Xe selectivity of the MOF column. This study offers an initial demonstration of the feasibility of monitoring off-gas treatment systems using a LIBS sensor to aid in the development of new capture systems for molten salt reactors.

47 OTHER INSTRUMENTATION↗

NASA NTRS2022

Interactive Biogenic Emissions and Drought Stress Effects on Atmospheric Composition in NASA GISS ModelE

Drought is a hydroclimatic extreme that causes perturbations to the terrestrial biosphere and acts as a stressor on vegetation, affecting emissions patterns. During severe drought, isoprene emissions are reduced. In this paper, we focus on capturing this reduction signal by implementing a new percentile isoprene drought stress (y d ) algorithm in NASA GISS ModelE based on the MEGAN3 (Model of Emissions of Gases and Aerosols from Nature Version 3) approach as a function of a photosynthetic parameter (V c,max ) and water stress (β). Four global transient simulations from 2003–2013 are used to demonstrate the effect without y d (Default_ModelE) and with online y d (DroughtStress_ModelE). DroughtStress_ModelE is evaluated against the observed isoprene measurements at the Missouri Ozarks AmeriFlux (MOFLUX) site during the 2012 severe drought where improvements in the correlation coefficient indicate it is a suitable drought stress parameterization to capture the reduction signal during severe drought. The application of y d globally leads to a decadal average reduction of ∼ 2.7 %, which is equivalent to ∼14.6 Tg yr -1 of isoprene. The changes have larger impacts in regions such as the southeastern US. DroughtStress_ModelE is validated using the satellite ΩHCHO column from the Ozone Monitoring Instrument (OMI) and surface O 3 observations across regions of the US to examine the effect of drought on atmospheric composition. It was found that the inclusion of isoprene drought stress reduced the overestimation of ΩHCHO in Default_ModelE during the 2007 and 2011 southeastern US droughts and led to improvements in simulated O 3 during drought periods. We conclude that isoprene drought stress should be tuned on a model-by-model basis because the variables used in the parameterization responses are relative to the land surface model hydrology scheme (LSM) and the effects of y d application could be larger than seen here due to ModelE not having large biases of isoprene during severe drought.

drought stress effects↗

NASA NTRSDate not supplied

AERACEPT (AErosol Rapid Analysis Combined Entry Probe/sonde Technology) for the Nephele Venus Cloud Mission Concept

Nephele is a small atmospheric probe mission concept to determine whether the Venus clouds contain organic matter. Nephele complements larger missions that seek to conduct Venus atmospheric analyses, such as DAVINCI, Venera-D, and the Morning Star missions, by directly sampling and analyzing cloud and haze particles. AERACEPT is an aerosol sampling technology designed to minimize the mass, volume, and complexity required for in situ planetary atmosphere characterization. A single aeroshell functions as a combined entry vehicle, descent probe, and instrumented sonde, combining recent advances in thermal protection materials with heritage technology from planetary and airborne science. The velocity of descent drives aerosol through inlets embedded in the aeroshell’s thermal protection material; inertial separation isolates the particles from the gas stream; and the particle capture surface doubles as the analysis substrate. This method can work without heat shield separation, descent control, or active sample handling; these advantages trade against a smaller sample volume, higher risk of sample heating, and shorter time for analysis and data return. AERACEPT further benefits from modeling of the internal and external flow to understand the particle capture efficiency and bias for size and concentration distributions. AERACEPT is well suited for a Venus mission such as Nephele, where a passive descent trajectory is both subsonic over the altitudes of interest and provides sufficient velocity and pressure differential for the particle sizes of interest. A thermal and flow toolchain developed in-house (Traj→ DPLR→ PATO→ openFOAM) was used to model an 80-cm aeroshell with science operations 63–39 km. These models indicate that AERACEPT will provide ~24 µL accumulated sample of particles ≥ 0.2 µm, substantially above the 2 µL threshold requirement. The worst-case particle heating will be ~14 K above ambient, for the smallest particles at the lowest altitude; most particles will experience ≤ 1 K rise, at which almost all analytes of interest will be unaffected. Plasma jet testing of a small-scale aeroshell-material inlet was recently conducted to validate the thermal model parameters; wind tunnel testing to validate the flow model parameters is underway.

AERACEPT↗

DOE OSTI2024

Real-Time Elemental and Isotopic Measurements of Molten Salt Systems through Laser-Induced Breakdown Spectroscopy

Molten salt reactors are an emerging advanced nuclear reactor concept in which the fuel is dissolved into the working fluid in the form of a high-temperature molten salt. The complex, mobile, and corrosive nature of this fluid presents a fundamental challenge for analytical measurements. Tracking species throughout the reactor is important for ensuring proper operation. This article presents laser-induced breakdown spectroscopy (LIBS) used to monitor the elemental composition of a molten salt and corresponding hydrogen isotopic shifts in real-time. A NaNO 3 –KNO 3 eutectic salt was saturated with protium and deuterium gases, then the effluent aerosol stream formed using an argon sparging vessel was monitored with LIBS. This modular LIBS system permitted several spectrometers to be used simultaneously to capture high-resolution isotopic shifts and provide broadband elemental coverage. Further, the results exhibit how LIBS can be used to understand salt–gas chemical and physical interactions such as diffusion. Furthermore, LIBS’ broad elemental coverage can provide greater insight into the chemical reactions within the salt vessel such as the formation of water vapor by monitoring hydrogen and oxygen signatures simultaneously. Ultimately, this study demonstrates the analytical possibilities of LIBS for real-time monitoring of isotopes and elemental composition in molten salt systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Emergence of seasonal delay of tropical rainfall during 1979–2019

Fundamental to Earth’s climate, tropical rainfall marks a dominant annual cycle characterized by its amplitude and phase, representing the range between wet and dry seasons and their onset timing, respectively. Under global warming, previous studies revealed enhanced amplitude of rainfall annual cycle over ocean and delayed phase over land in the tropics, underpinned by solid theories. It is unclear however whether these changes have already emerged in the observational records. Here, we report a robust delay of 3.02 and 3.43 days over the northern tropical land and Sahel respectively during 1979-2018 based on five observation datasets. Furthermore, most of the delay is captured by multiple ensemble simulations driven by external forcings, with greenhouse gases (GHG) more important over the northern tropical land and anthropogenic aerosols (AER) more important over the Sahel. Both GHG and AER delay the annual cycle of regional precipitation similarly by producing a moister and more ocean-like atmosphere, thus increasing its lag in response to seasonal solar forcing. Our findings provide new evidence of the human footprints on Earth’s hydrological cycle at continental and regional scales. As GHG and AER continue to increase and decrease respectively, these seasonal delays will be further amplified in the future.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Sorption and Desorption Study of a Nerve-Agent Simulant from Office Materials for Forensic Applications

Dimethyl methylphosphonate (DMMP) was used as a simulant to investigate the sorption and desorption of G-series nerve agents such as sarin (GB) released into an office space. DMMP was disseminated systematically as an aerosol and vapor on three common office materials, cardboard, polyurethane foam, and cured acrylic-based paint. The amount of DMMP initially captured on the office materials and the amount retained over a period of 10 hours was tracked gravimetrically and by solvent extraction and gas chromatography/mass spectrometry (GC/MS). Physicochemical properties of the office media including the specific surface area per mass, polarity, and Henry’s constants were determined to help explain the capture and release of DMMP that was observed. Polyurethane foam was found to have the largest sorption capacity for DMMP in a low-humidity setting, however, cardboard was found to have the largest sorption capacity at higher humidity. A fraction of the DMMP collected desorbed with first-order kinetics from all of the office materials in an open-air atmosphere over 8 hours. However, importantly for forensic purposes relevant to an indoor attack, a significant quantity (most notably on cardboard) of the nerve agent simulant was retained after 6 weeks and could be analyzed efficiently using solvent extraction followed by GC/MS.

chemical forensics↗

DOE OSTI2020

Fingerprints of external forcings on Sahel rainfall: aerosols, greenhouse gases, and model-observation discrepancies

Over the 20th and 21st centuries, both anthropogenic greenhouse gas increases and changes in anthropogenic aerosols have affected rainfall in the Sahel. Using multiple characteristics of Sahel precipitation, we construct a multivariate fingerprint that allows us to distinguish between the model-predicted responses to greenhouse gases and anthropogenic aerosols. Models project the emergence of a detectable signal of aerosol forcing in the middle of the 20th century and a detectable signal of greenhouse gas forcing at the beginning of the 21st. However, the signals of both aerosol and greenhouse gas forcing in observations emerge earlier and are stronger than in the models, far stronger in the case of aerosols. The similarity between the response to aerosol forcing and the leading mode of internal variability makes it difficult to attribute this model-observation discrepancy to errors in the forcing, errors in the forced response, model inability to capture the amplitude of internal variability, or some combination of these. For greenhouse gases, however, the forced response is distinct from internal variability as estimated by models, and the observations are largely commensurate with the model projections.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2020

Fingerprints of External Forcing Agents on Sahel Rainfall: Aerosols, Greenhouse Gases, and Model-Observation Discrepancies

Sahel↗

DOE OSTI2025

Transformational Sorbent-Based Process for a Substantial Reduction in the Cost of CO2 Capture

Adsorption processes have the potential to significantly reduce the CO2 capture cost from power plants and industrial flue gases. InnoSepra has developed several sorbent-based technologies to obtain very high CO2 recovery and high purity CO2 while meeting the EOR/sequestration product specifications. A first-generation process was shown to achieve CO2 recoveries greater than 94% at CO2 purities in the range of 98.5-99.5%. The absolute heat energy required for the process was not only 40% lower than MEA but also was needed at a much lower temperature. This work will present the performance of the second-generation InnoSepra process which is based on a breakthrough sorbent regeneration method. This process has a projected 45% lower capital cost compared to MEA, less than 16% loss in plant output for CO2 capture and compression, and a CO2 capture cost at least 55% lower than MEA. Lab scale testing and the process simulations indicate a CO2 capture performance similar to or better than the first-generation process. Pilot scale drying and breakthrough tests were carried out at the Technology Centre Mongstad (TCM), Norway, and lab-scale cyclic tests were carried out at InnoSepra to confirm the process improvement. During these tests, InnoSepra’s flue gas purification technology was also tested at TCM. It can provide a low-cost option for the removal of NO2 and SOX to sub-ppm levels as well as a significant reduction in aerosol emissions.

08 HYDROGEN↗

NASA NTRSDate not supplied

Variation and evolution of atmospheric structure over the SEA BB season as seen from aircraft and reanalysis

The presence of absorbing aerosols and atmospheric water vapor will impact clouds both radiatively and dynamically. The atmosphere over the southeast Atlantic Ocean (SEA) experiences consistent springtime biomass burning (BB) smoke from widespread agricultural fires on the African continent. This smoke layer is initially lofted high in a continental mixed layer (~5-6km) and is then transported westward into the free troposphere where it overlies and ultimately mixes into the underlying stratocumulus-topped oceanic boundary layer. Coincident with this smoke is an elevated humidity signal which is present from the time a given airmass is over the continental source region. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) was a NASA Earth Venture Suborbital mission with the goal of measuring aerosol, cloud, and atmospheric properties over this region over three deployments in September 2016, August 2017, and October 2018. Measurements included in situ profile measurements of aerosol physical and optical properties, trace gas concentrations, and cloud properties, as well as column measurements of aerosol optical depth and trace gas concentrations from an airborne sun photometer, allowing for calculation of radiative heating at different altitudes. Here we present results from the three ORACLES deployments over the southeast Atlantic Ocean. The airborne observations capture both seasonal patterns (August through October) and spatial patterns (north/south and east/west) in the vertical smoke distribution and its correlation to atmospheric specific humidity over the SEA basin. We describe the observed variations and show that the variability in both meteorological and emissions is largely captured in the European Centre for Medium-range Weather Forecasting Copernicus Atmosphere Monitoring Service (ECMWF CAMS) reanalysis, which allows for a more systematic examination of the relative frequency of observed conditions and their radiative impact over the region. Finally, we discuss the broader radiative and dynamical implications of these results for conditions of biomass burning aerosols overlying stratocumulus clouds.

Kristina Marie Myers Pistone↗

DOE OSTI2023

CSAPR2 Optimized Convective Cell Tracking Data during TRACER

One of the challenges in analyzing convective cell properties is to observe the quick evolution of individual convective cells. While the operational radar data provide a volumetric data set to analyze radar observables of convective precipitation clouds, previous studies also suggested the quick evolution of cell life cycle that might not be captured by conventional radar volume scan strategies that take ~5-7 minutes. Aiming at enhancing our understanding of the links between convective cloud kinematic and microphysical processes as well as life cycles, the Tracking Aerosol Convection Interactions ExpeRiment (TRACER; Jensen et al. 2019) was conducted at Houston, Texas, in 2022. The TRACER campaign deployed the 2nd generation C-band Scanning ARM Precipitation Radar (CSAPR2), which performed frequent updates of range height indicator (RHI) and sector plan position indicator (PPI) scans to track individual convective cells every < 2 minutes, guided by a new cell tracking framework, Multisensor Agile Adaptive Sampling (MAAS; Kollias et al. 2020). This allows for capturing fast-evolving radar observables. We provide the processed CSAPR2 cell tracking data in CfRadial format collected during the TRACER field campaign from June to September 2022. The data files include processed radar variables: noise-masked reflectivity and differential reflectivity corrected for rain attenuation and systematic biases, noise-masked dealiased radial velocity, specific differential phase, locations of target cells (latitude, longitude, radar range), and radar-echo classification. Figure 1 provides an example of a 3D image of CSAPR2 reflectivity from the lowest PPI scan and an RHI scan after data processing.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Ice Nucleating Particles, Aerosols and Clouds over the Higher Latitude Southern Ocean

Improved understanding of aerosol-cloud-precipitation interactions is a key goal of the DOE-ASR program. Ice Nucleating Particles (INPs) are rare aerosol particles that trigger ice formation in clouds. By doing so they may initiate precipitation in clouds, and this impacts cloud lifetime. Nowhere may the role of INPs be manifested so dramatically as in the Southern Ocean (SO). This vast region was the focus of the DOE-ARM MARCUS (Measurement of Aerosols, Radiation and CloUds over the Southern Oceans) and MICRE (Macquarie Island Cloud and Radiation Experiment) campaigns. In the SO, a deficit of INPs has been a leading hypothesis for why liquid clouds persist, which underlays the bias of global climate models in predicting excess shortwave radiation reaching the ocean surface between 55°S and Antarctica. In this study, we used the 6-month acquisition of INP data on four MARCUS cruises from Hobart, Tasmania, to Antarctica, and the single-location full annual INP cycle observed in MICRE, to gain a holistic, quantitative picture of the INP number concentrations as a function of temperature and their variability over SO latitudes from 43°S to Antarctica. Augmenting initial processing of filter collections of aerosol particles during MARCUS and MICRE, additional freezing studies following thermal treatment (to removes INPs associated with microbes) and peroxide treatment (to remove all organics), as well as ionic chemistry and total organic carbon analysis, were applied to samples to improve time and space resolution, and differentiate marine from terrestrial contributions. We also performed Next Generation Sequencing to determine that bacterial composition can tag periods of enhanced and degraded marine organic INPs and the relative lack of occurrence of land-sourced bio-particles. Through these and other analyses, INP data were categorized into representative source types (e.g., marine versus terrestrially-influenced). The products of our analyses are being used to parameterize ice formation for use in numerical modeling studies to determine if, and when, ocean-derived INPs control the microphysical composition and radiative balance of SO clouds in a manner not presently captured by global models. The specific objectives and approaches proposed were largely accomplished, including: 1) Additional and value-added chemical and biological analyses of archived samples of aerosols were completed to categorize and quantify INP types and concentrations over the SO. 2) Analyses were completed to place INP data in meteorological and aerosol context. 3) Sea spray aerosol INPs were demonstrated to dominate the SO region in all but episodic events. 4) New parameterizations for INP sources relevant to the SO were constructed. 5) Collaborative modeling studies demonstrating the crucial role of INPs in determining cloud radiative and precipitation properties were conducted with MARCUS and MICRE partners. Collaborative publication submissions in this regard ensued within the two year study. This work will advance the science of interactions of aerosols, clouds and precipitation, to improve their representation in regional and global climate models. Results have informed representation of primary ice crystal nucleation, give inference to the role of secondary processes, and improve investigations of aerosol influences on clouds via ice nucleation over SO high latitudes and similar vast ocean regions. Application will improve representation of such interactions for clouds in both regional and global climate models. The data base and analyses methods applied will continue to serve research studies in the future.

58 GEOSCIENCES↗

NASA NTRS2024

Global Sensitivity Analysis of Simulated Remote Sensing Polarimetric Observations Over Snow

This study presents a detailed theoretical assessment of the information content of passive polarimetric observations over snow scenes, using a global sensitivity analysis (GSA) method. Conventional sensitivity studies focus on varying a single parameter while keeping all other parameters fixed. In contrast, the GSA correctly addresses the covariance of state parameters across their entire parameter space, hence favoring a more correct interpretation of inversion algorithms and the optimal design of their state vectors. The forward simulations exploit a vector radiative transfer model to obtain the Stokes vector emerging at the top of the atmosphere for different solar zenith angles, when the bottom boundary consists of a vertically resolved snowpack of non-spherical grains. The presence of light-absorbing particulates (LAPs), either embedded in the snow or aloft in the atmosphere above in the form of aerosols, is also considered. The results are presented for a set of wavelengths spanning the visible (VIS), near-infrared (NIR), and shortwave infrared (SWIR) region of the spectrum. The GSA correctly captures the expected, high sensitivity of the reflectance to LAPs in the VIS–NIR and to grain size at different depths in the snowpack in the NIR–SWIR. With adequate viewing geometries, mono-angle measurements of total reflectance in the VIS–SWIR (akin to those of the Moderate Resolution Imaging Spectroradiometer, MODIS) resolve grain size in the top layer of the snowpack sufficiently well. The addition of multi-angle polarimetric observations in the VIS–NIR provides information on grain shape and microscale roughness. The simultaneous sensitivity in the VIS–NIR to both aerosols and snow-embedded impurities can be disentangled by extending the spectral range to the SWIR, which contains information on aerosol optical depth while remaining essentially unaffected when the same particulates are mixed with the snow. Multi-angle polarimetric observations can therefore (i) effectively partition LAPs between the atmosphere and the surface, which represents a notorious challenge for snow remote sensing based on measurements of total reflectance only and (ii) lead to better estimates of grain shape and roughness and, in turn, the asymmetry parameter, which is critical for the determination of albedo. The retrieval uncertainties are minimized when the degree of linear polarization is used in place of the polarized reflectance. The Sobol indices, which are the main metric for the GSA, were used to select the state parameters in retrievals performed on data simulated for multiple instrument configurations. Improvements in retrieval quality with the addition of measurements of polarization, multi-angle views, and different spectral channels reflect the information content, identified by the Sobol indices, relative to each configuration. The results encourage the development of new remote sensing algorithms that fully leverage multi-angle and polarimetric capabilities of modern remote sensors. They can also aid flight planning activities, since the optimal exploitation of the information content of multi-angle measurements depends on the viewing geometry. The better characterization of surface and atmospheric parameters in snow-covered regions advances research opportunities for scientists of the cryosphere and ultimately benefits albedo estimates in climate models.

remote sensing↗