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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 379 records · Page 21
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

TEMPERATURE SPECTRA OF INTERSTELLAR DUST GRAINS HEATED BY COSMIC RAYS. I. TRANSLUCENT CLOUDS

Heating of whole interstellar dust grains by cosmic-ray (CR) particles affects the gas–grain chemistry in molecular clouds by promoting molecule desorption, diffusion, and chemical reactions on grain surfaces. The frequency of such heating, f{sub T}, s{sup −1}, determines how often a certain temperature T{sub CR}, K, is reached for grains hit by CR particles. This study aims to provide astrochemists with a comprehensive and updated data set on CR-induced whole-grain heating. We present calculations of f{sub T} and T{sub CR} spectra for bare olivine grains with radius a of 0.05, 0.1, and 0.2 μ m and such grains covered with ice mantles of thickness 0.1 a and 0.3 a . Grain shape and structure effects are considered, as well as 30 CR elemental constituents with an updated energy spectrum corresponding to a translucent cloud with A{sub V} = 2 mag. Energy deposition by CRs in grain material was calculated with the srim program. We report full T{sub CR} spectra for all nine grain types and consider initial grain temperatures of 10 K and 20 K. We also provide frequencies for a range of minimum T{sub CR} values. The calculated data set can be simply and flexibly implemented in astrochemical models. The results show that, in the case of translucent clouds, the currently adopted rate for heating of whole grains to temperatures in excess of 70 K is underestimated by approximately two orders of magnitude in astrochemical numerical simulations. Additionally, grains are heated by CRs to modest temperatures (20–30 K) with intervals of a few years, which reduces the possibility of ice chemical explosions.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS2002

Mesoscale Convective Systems in SCSMEX: Simulated by a Regional Climate Model and a Cloud Resolving Model

A Regional Land-Atmosphere Climate Simulation (RELACS) System is being developed and implemented at NASA Goddard Space Flight Center. One of the major goals of RELACS is to use a regional scale model with improved physical processes, in particular land-related processes, to understand the role of the land surface and its interaction with convection and radiation as well as the water and energy cycles in Indo-China/ South China Sea (SCS)/China, N. America and S. America. The Penn State/NCAR MM5 atmospheric modeling system, a state of the art atmospheric numerical model designed to simulate regional weather and climate, has been successfully coupled to the Goddard Parameterization for Land-Atmosphere-C loud Exchange (PLACE) land surface model. PLACE allows for the effects of vegetation, and thus important physical processes such as evapotranspiration and interception are included. The PLACE model incorporates vegetation type and has been shown in international comparisons to accurately predict evapotranspiration and runoff over a wide variety of land surfaces. The coupling of MM5 and PLACE creates a numerical modeling system with the potential to more realistically simulate the atmosphere and land surface processes including land-sea interaction, regional circulations such as monsoons, and flash flood events. RELACS has been used to simulate the onset of the South China Sea Monsoon in 1986, 1997 and 1998. Sensitivity tests on various land surface models, cumulus parameterization schemes (CPSs), sea surface temperature (SST) variations and midlatitude influences have been performed. These tests have indicated that the land surface model has a major impact on the circulation over the S. China Sea. CPSs can effect the precipitation pattern while SST variation can effect the precipitation amounts over both land and ocean. RELACS has also been used to understand the soil-precipitation interaction and feedback associated with a flood event that occurred in and around China's Yantz River during 1998. The exact location (region) of the flooding can be effected by the soil-rainfall feedback. Also, the Goddard Cumulus Ensemble (GCE) model which allows for realistic moist processes as well as explicit interactions between cloud and radiation, and cloud and surface processes will be used to simulate convective systems associated with the onset of the South China Sea Monsoon in 1998. The GCE model also includes the same PLACE and radiation scheme used in the RELACS. A detailed comparison between the results from the GCE model and RELACS will be performed.

Tao, W.-K.↗
NASA NTRS2019

Jumping the Queue: From NASA to the Commercial Cloud

NASA's High-End Computing Capability (HECC) Project has made it possible for its users to run on commercial cloud resources in a seamless way. In the first of three phases, we implemented a pilot project for a few users, enabling them to “jump the queue” and burst jobs from the HECC environment to Amazon Web Services (AWS). By using GPU-accelerated nodes at AWS, the users were able to make significant advances in their research. The second phase of the project made AWS access available to all HECC users and added accounting to make users responsible for cloud charges. We are also enabling export-controlled work through the use of AWS GovCloud. In the third phase, we will add web-based mechanisms to permit non-HECC users to access cloud resources for their HPC projects.

Hood, Robert↗
DOE OSTI2022

Parameterization of cloud transmittance for expeditious assessment and forecasting of all-sky DNI

Radiative transfer models require vast computing resources to solve cloud transmittance and reflectance from the radiative transfer equation. As a result, models offering precise simulation in operations often acquire individual cloud transmittance or reflectance from a lookup table precomputed for practicable scenarios. To further expedite the computation of global horizontal irradiance and to reduce the storage requirements, the Fast All-sky Radiation Model for Solar applications (FARMS) parameterized the lookup table using elementary functions with specified coefficients. This study extends FARMS direct normal irradiance (DNI) computation by utilizing hyperbolic tangent functions and various polynomial functions to parameterize the cloud transmittance for scattered solar radiation in the circumsolar region. The parameterization is implemented in FARMS with DNI (FARMS-DNI) and accounts for the circumsolar radiation when assessing or forecasting DNI. The evaluation, with long-term observations at the National Renewable Energy Laboratory's, Solar Radiation Research Laboratory, and the Atmospheric Radiation Measurement, Southern Great Plains, Central Facility, shows that the parameterized DNIs are virtually identical with those computed by coupling FARMS-DNI to a lookup table of cloud transmittance. This parameterization has diverse applications in radiative transfer models and numerical weather prediction models used to assess or forecast direct solar radiation.

14 SOLAR ENERGY↗
DOE OSTI2026

Tendencies of Soil Microbial NO Emissions During HI‐SCALE as Predicted by a Nitrification/Denitrification Scheme

Many atmospheric chemical processes, including the formation of secondary organic aerosol (SOA), are strongly modulated by the reactions of NO and NO 2 (NO x ). Though NO x is controlled by anthropogenic emissions near urban areas, in rural areas soil microbes can be a significant contribution to NO emission globally. The relative rates of emissions of different nitrogen-containing species (e.g., NO, N 2 O, HONO, and N 2 ) are strong functions of soil properties such as temperature, moisture content, pH, and soil carbon and nitrogen pools. However, typical large-scale biogeochemical models either express these emissions simplistically, or not at all. Here we investigate the potential impact of soil NO emissions on atmospheric chemistry and SOA formation over regional and monthly time scales, specifically the 2016 spring and summer Intensive Observational Periods (IOPs) of the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems (HI-SCALE) field campaign. We implement the soil NO nitrification/denitrification parameterization of Rasool et al. (2019) into the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), supplemented by a 1-km soil moisture analysis. We then simulate both IOPs over the U.S. Great Plains, evaluating against ground stations and flight data. We show that soil NO emissions can account for a large fraction of total NO x and locally increase O 3 concentrations by up to 25%, while alleviating negative biases of gases and aerosols toward observations. Soil moisture and temperature changes between IOP1 and IOP2 lead to overall differences in emissions, but with large regional variability due to heterogeneous surface characteristics.

Atmoshpheric Chemistry↗
DOE OSTI2024

Modeling diurnal and annual ethylene generation from solar-driven electrochemical CO 2 reduction devices

Integrated solar fuels devices for CO 2 reduction (CO 2 R) are a promising technology class towards reducing carbon emissions. Designing integrated CO 2 R solar fuels devices requires careful co-design of electrochemical and photovoltaic components as well as consideration of the diurnal and seasonal effects of solar irradiance, temperature, and other meteorological factors expected for ‘on-sun’ deployment. Using a photovoltaic-electrochemical (PV-EC) platform, we developed a temperature and potential-dependent diurnal and annual model using experimentally-determined CO 2 R performance of Cu-based electrocatalysts, local meteorological data from the National Solar Radiation Database (NSRD), and modeled performance of commercial c-Si PVs. Here we simulated gaseous diurnal product outputs with and without the effects of ambient temperature. From these outputs, we observed seasonal variation in gaseous product generation, with up to two-fold increases in ethylene productivity between the Winter and Summer, analyzed the consequences of dynamic cloud coverage, and identified periods where device cooling/heating mechanisms could be implemented to maximize ethylene generation. Finally, we modeled the annual ethylene generation for a scaled 1 MW solar farm at three different locations (Beijing, CN; Sydney, AUS; Barstow, CA) to determine the consequences of local meteorological climates on PV-EC CO 2 R product output, recording a maximum ethylene output of 18.5 tonne per year at Barstow. Overall, this model presents a critical tool for streamlining the translation of experimental solar-driven electrochemical research to real-world implementation.

14 SOLAR ENERGY↗
DOE OSTI2025

Comparing three generations of D-Wave quantum annealers for minor embedded combinatorial optimization problems

Abstract Quantum annealing (QA) is a novel type of analog computation that aims to use quantum mechanical fluctuations to search for optimal solutions of Ising problems. QA in the transverse Ising model, implemented on D-Wave quantum processing units, are available as cloud computing resources. In this study we report concise benchmarks across three generations of D-Wave quantum annealers, consisting of four different devices, for the NP-hard discrete combinatorial optimization problems unweighted maximum clique and unweighted maximum cut on random graphs. The Ising, or equivalently quadratic unconstrained binary optimization, formulation of these problems do not require auxiliary variables for order reduction, and their overall structure and weights are not highly variable, which makes these problems simple test cases to understand the sampling capability of current D-Wave quantum annealers. All-to-all minor embeddings of size 52, with relatively uniform chain lengths, are used for a direct comparison across the Chimera, Pegasus, and Zephyr device topologies. A grid-search over annealing times and the minor embedding chain strengths is performed in order to determine the level of reasonable performance for each device and problem type. Experiment metrics that are reported are approximation ratios for non-broken chain samples, chain break proportions, and time-to-solution for the maximum clique problem instances. How fairly the quantum annealers sample optimal maximum cliques, for instances which contain multiple maximum cliques, is quantified using entropy of the measured ground state distributions. The newest generation of quantum annealing hardware, which has a Zephyr hardware connectivity, performed the best overall with respect to approximation ratios and chain break frequencies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Modeling Diurnal and Annual Ethylene Generation from Solar-Driven Electrochemical CO 2 Reduction Devices

Integrated solar fuels devices for CO 2 reduction (CO 2 R) are a promising technology class towards achieving net-negative carbon emissions. Designing integrated CO 2 R solar fuels devices requires careful co-design of electrochemical and photovoltaic components as well as consideration of the diurnal and seasonal effects of solar irradiance, temperature, and other meteorological factors expected for ‘on-sun’ deployment. Here, using a photovoltaic-electrochemical (PV-EC) platform, we developed a temperature and potential-dependent diurnal and annual model using experimental CO 2 R performance of Cu-based electrocatalysts, local meteorological data from the National Solar Radiation Database (NSRD), and modeled performance of commercial c-Si PVs. We simulated diurnal product outputs with and without the effects of ambient temperature to determine gaseous product temperature sensitivity. From these outputs, we observed seasonal variation in gaseous product generation, with up to two-fold increases in ethylene productivity between the Winter and Summer, analyzed the consequences of dynamic cloud coverage, and identified periods where device cooling/heating mechanisms could be implemented to maximize ethylene generation. Finally, we modeled the annual ethylene generation for a scaled 1 MW solar farm at three different locations (Beijing, CN; Sydney, AUS; Barstow, CA) to determine the consequences of local meteorological climates on PV-EC CO 2 R product output, recording a maximum ethylene output of 18.5 tonne/yr at Barstow. Overall, this model presents a critical tool for streamlining the translation of experimental solar-driven electrochemical research to real-world implementation.

Yap, Kyra M. K.↗
DOE OSTI2019

Managing genomic variant calling workflows with Swift/T

Bioinformatics research is frequently performed using complex workflows with multiple steps, fans, merges, and conditionals. This complexity makes management of the workflow difficult on a computer cluster, especially when running in parallel on large batches of data: hundreds or thousands of samples at a time. Scientific workflow management systems could help with that. Many are now being proposed, but is there yet the “best” workflow management system for bioinformatics? Such a system would need to satisfy numerous, sometimes conflicting requirements: from ease of use, to seamless deployment at peta- and exa-scale, and portability to the cloud. We evaluated Swift/T as a candidate for such role by implementing a primary genomic variant calling workflow in the Swift/T language, focusing on workflow management, performance and scalability issues that arise from production-grade big data genomic analyses. In the process we introduced novel features into the language, which are now part of its open repository. Additionally, we formalized a set of design criteria for quality, robust, maintainable workflows that must function at-scale in a production setting, such as a large genomic sequencing facility or a major hospital system. The use of Swift/T conveys two key advantages. (1) It operates transparently in multiple cluster scheduling environments (PBS Torque, SLURM, Cray aprun environment, etc.), thus a single workflow is trivially portable across numerous clusters. (2) The leaf functions of Swift/T permit developers to easily swap executables in and out of the workflow, which makes it easy to maintain and to request resources optimal for each stage of the pipeline. While Swift/T’s data-level parallelism eliminates the need to code parallel analysis of multiple samples, it does make debugging more difficult, as is common for implicitly parallel code. Nonetheless, the language gives users a powerful and portable way to scale up analyses in many computing architectures.

Science & Technology - Other Topics↗
NASA NTRS1981

Applications systems verification and transfer project. Volume 4: Operational applications of satellite snow cover observations. Colorado Field Test Center

The study was conducted on six watersheds ranging in size from 277 km to 3460 km in the Rio Grande and Arkansas River basins of southwestern Colorado. Six years of satellite data in the period 1973-78 were analyzed and snowcover maps prepared for all available image dates. Seven snowmapping techniques were explored; the photointerpretative method was selected as the most accurate. Three schemes to forecast snowmelt runoff employing satellite snowcover observations were investigated. They included a conceptual hydrologic model, a statistical model, and a graphical method. A reduction of 10% in the current average forecast error is estimated when snowcover data in snowmelt runoff forecasting is shown to be extremely promising. Inability to obtain repetitive coverage due to the 18 day cycle of LANDSAT, the occurrence of cloud cover and slow image delivery are obstacles to the immediate implementation of satellite derived snowcover in operational streamflow forecasting programs.

Shafer, B. A.↗
DOE OSTI2021

Comparing Satellite- and Ground-Based Observations of Cloud Occurrence Over High Southern Latitudes

The 2B-CLDCLASS-LIDAR R05 (2BCL5) and the raDAR/liDAR (DARDAR) satellite retrievals of cloud occurrence are compared as a function of altitude and latitude. The largest disparities are observed at low altitudes over high southern latitudes. These data sets are cross referenced to ground-based measurements from the Atmospheric Radiation Measurement (ARM) West Antarctic Radiation Experiment (AWARE) campaign at McMurdo Station, Antarctica. Compared with AWARE observations, both 2BCL5 and DARDAR underestimate cloud occurrence below 1.5 km, with 2BCL5 and DARDAR distinguishing roughly one third of cloud occurrences observed by AWARE at 0.5 km. While DARDAR identifies greater cloud occurrences than 2BCL5 below 1.5 km, cloud occurrence values for the two data sets have similar differences relative to ground-based measurements. Therefore, the DARDAR retrievals of greater cloud occurrence at low altitudes are likely due to a larger quantity of false positives associated with radar ground clutter or attenuated lidar retrievals. DARDAR cloud occurrences match better with AWARE than 2BCL5 above 5 km. However, the likely underestimation of ground-based measurements at higher altitudes suggests DARDAR may underestimate high level cloud occurrence. Finally, both data sets indicate the presence of liquid containing clouds at temperatures within the homogeneous freezing regime, despite the fact that the ECMWF-AUX data set implemented in their processing clearly indicates temperatures below -38°C. Finally, using AWARE radiosonde (ECMWF-AUX) temperature data, we find that 2BCL5 detects 13.3% (13.8%) of mixed phase clouds below -38°C, while DARDAR detects 5.7% (6.6%) of mixed phase and 1.1% (1.3%) of liquid phase clouds below -38°C.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Automated nuclear cloud feature extraction from film

Chemical, biological, radiological, nuclear, and explosives incidents require rapid detection and characterization for appropriate response. For a nuclear detonation, visible-light cameras may be used to locate the cloud and characterize fallout deposition when coupled with numerical models. Films from the United States’ nuclear testing era compose the only sizeable collection of imagery depicting high-yield detonations. These films offer unique insights into characteristics of flows involving scales that are difficult to replicate experimentally, and they are a valuable source of data for the validation of models for nuclear fallout transport, either as part of emergency response or forensic activities. In this work, we implement modern computer vision and machine learning techniques to identify and track the cloud automatically and subsequently determine the time dependence of some of its features. We trained a ResNet-18 image classifier on hundreds of images to categorize nuclear cloud morphology. Each category or cloud regime is determined by early cloud evolution and is associated to constitutive properties of the flow, such as distribution of vorticity. Next, we identified keypoint features using the KAZE algorithm and tracked these keypoints in the images, allowing us to determine the dimensions and velocities of the cloud across film frames. These measurements converted to real-world units provide valuable experimental data that can be used in the development and validation of nuclear cloud models. We compared the results of this method against manual cloud rise measurements from two different films. In one, our automated method accelerated the feature extraction process without sacrificing measurement accuracy.

Khristy, Joel [ORNL] (ORCID:0000000209963060)↗
NASA NTRS2015

Aerosol-Cloud Interactions in the South-East Atlantic: Knowledge Gaps, Planned Observations to Address Them, and Implications for Global Climate Change Modeling

Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. Particles lofted into the mid-troposphere are transported westward over the South-East (SE) Atlantic, home to one of the three permanent subtropical Stratocumulus (Sc) cloud decks in the world. The stratocumulus "climate radiators" are critical to the regional and global climate system. They interact with dense layers of BB aerosols that initially overlay the cloud deck, but later subside and are mixed into the clouds. These interactions include adjustments to aerosol-induced solar heating and microphysical effects. As emphasized in the latest IPCC report, the global representation of these aerosol-cloud interaction processes in climate models is one of the largest uncertainty in estimates of future climate. Hence, new observations over the SE Atlantic have significant implications for global climate change scenarios. We discuss the current knowledge of aerosol and cloud property distributions based on satellite observations and sparse suborbital sampling, and describe planned field campaigns in the region. Specifically, we describe the scientific objectives and implementation of the following four synergistic, international research activities aimed at providing a process-level understanding of aerosol-cloud interactions over the SE Atlantic: 1) ORACLES (Observations of Aerosols above Clouds and their interactions), a five-year investigation between 2015 and 2019 with three Intensive Observation Periods (IOP), recently funded by the NASA Earth-Venture Suborbital Program, 2) CLARIFY-2016 (Cloud-Aerosol-Radiation Interactions and Forcing: Year 2016), a comprehensive observational and modeling programme funded by the UK's Natural Environment Research Council (NERC), and supported by the UK Met Office. 3) LASIC (Layered Atlantic Smoke Interactions with Clouds), a funded deployment of the DOE (Department of Energy) ARM Mobile Facility (AMF1) to Ascension Island, nominally for April 1 2016 - March 31 2017, and 4) ONFIRE (Observations of Fire's Impact on the southeast Atlantic Region), a proposed deployment of the NCAR C-130 aircraft to Sao Tome Island in 2017.

Aerosol-cloud↗
DOE OSTI2019

Improvement of aerosol activation/ice nucleation in a source-oriented WRF-Chem model to study a winter Storm in California

The source-oriented Weather Research and Forecasting chemistry (SOWC) model is modified to improve mixed-phase cloud parameterization by including aerosol aging processes (external mixture) in cloud activation/nucleation. The improved SOWC model is applied to investigate how aerosol mixing state influences cloud and ice formation and atmospheric optical properties during a winter storm. SOWC tracks 6-dimensional chemical variables (X, Z, Y, Size Bins, Source Types, Species) through an explicit simulation of atmospheric chemistry and physics. A new module is implemented into the enhanced SOWC model to simulate microphysics processes with all source-oriented hydrometeors (cloud, ice, rain, snow and graupel) by using the modified Morrison two-moment microphysics scheme. In this study, all aerosol source types can activate to form cloud droplets based on the Köhler theory, but the dust source type is the only source of ice nuclei (IN). Here, the Goddard shortwave and longwave radiation schemes are modified to use a new geometric optics method to estimate cloud optical properties by considering the chemistry components and the physical shape of each hydrometeor.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2008

Forecasting Lightning Threat using Cloud-Resolving Model Simulations

Two new approaches are proposed and developed for making time and space dependent, quantitative short-term forecasts of lightning threat, and a blend of these approaches is devised that capitalizes on the strengths of each. The new methods are distinctive in that they are based entirely on the ice-phase hydrometeor fields generated by regional cloud-resolving numerical simulations, such as those produced by the WRF model. These methods are justified by established observational evidence linking aspects of the precipitating ice hydrometeor fields to total flash rates. The methods are straightforward and easy to implement, and offer an effective near-term alternative to the incorporation of complex and costly cloud electrification schemes into numerical models. One method is based on upward fluxes of precipitating ice hydrometeors in the mixed phase region at the-15 C level, while the second method is based on the vertically integrated amounts of ice hydrometeors in each model grid column. Each method can be calibrated by comparing domain-wide statistics of the peak values of simulated flash rate proxy fields against domain-wide peak total lightning flash rate density data from observations. Tests show that the first method is able to capture much of the temporal variability of the lightning threat, while the second method does a better job of depicting the areal coverage of the threat. Our blended solution is designed to retain most of the temporal sensitivity of the first method, while adding the improved spatial coverage of the second. Exploratory tests for selected North Alabama cases show that, because WRF can distinguish the general character of most convective events, our methods show promise as a means of generating quantitatively realistic fields of lightning threat. However, because the models tend to have more difficulty in predicting the instantaneous placement of storms, forecasts of the detailed location of the lightning threat based on single simulations can be in error. Although these model shortcomings presently limit the precision of lightning threat forecasts from individual runs of current generation models,the techniques proposed herein should continue to be applicable as newer and more accurate physically-based model versions, physical parameterizations, initialization techniques and ensembles of forecasts become available.

McCaul, Eugene W., Jr.↗
NASA NTRS2012

Improved Cloud and Snow Screening in MAIAC Aerosol Retrievals Using Spectral and Spatial Analysis

An improved cloud/snow screening technique in the Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithm is described. It is implemented as part of MAIAC aerosol retrievals based on analysis of spectral residuals and spatial variability. Comparisons with AERONET aerosol observations and a large-scale MODIS data analysis show strong suppression of aerosol optical thickness outliers due to unresolved clouds and snow. At the same time, the developed filter does not reduce the aerosol retrieval capability at high 1 km resolution in strongly inhomogeneous environments, such as near centers of the active fires. Despite significant improvement, the optical depth outliers in high spatial resolution data are and will remain the problem to be addressed by the application-dependent specialized filtering techniques.

Lyapustin, A.↗
DOE OSTI2025

Simulating Marine Stratocumulus Clouds using Lagrangian Superdroplet Method in ERF

This study investigates the simulation of marine stratocumulus (stratoCu) clouds – common in many offshore and coastal wind energy regions - using Lagrangian Superdroplet Method (SDM) implemented in Energy Research and Forecasting (ERF) model. Developed by the Wind Energy Technologies Office (WETO), ERF is a high-resolution atmospheric modeling tool that relies on traditional bulk microphysics schemes. Under an LLNL-led Laboratory Directed Research and Development (LDRD) project, SDM was integrated into ERF to improve cloud process fidelity by explicitly tracking individual “superdroplets”. This enables a realistic representation of the droplet size spectrum, cloud-atmosphere interactions, and potential feedbacks from wind plants on atmospheric flow and cloud structure.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Modeling Novel Aqueous Particle and Cloud Chemistry Processes of Biomass Burning Phenols and Their Potential to Form Secondary Organic Aerosols

Phenols emitted from biomass burning contribute significantly to secondary organic aerosol (SOA) formation through the partitioning of semivolatile products formed from gas-phase chemistry and multiphase chemistry in aerosol liquid water and clouds. The aqueous-phase SOA (aqSOA) formed via hydroxyl radical (˙OH), singlet molecular oxygen ( 1 O 2 *), and triplet excited states of organic compounds ( 3 C*), which oxidize dissolved phenols in the aqueous phase, might play a significant role in the evolution of organic aerosol (OA). However, a quantitative and predictive understanding of aqSOA has been challenging. Here, we develop a stand-alone box model to investigate the formation of SOA from gas-phase ˙OH chemistry and aqSOA formed by the dissolution of phenols followed by their aqueous-phase reactions with ˙OH, 1 O 2 *, and 3 C* in cloud droplets and aerosol liquid water. Here, we investigate four phenolic compounds, i.e., phenol, guaiacol, syringol, and guaiacyl acetone (GA), which represent some of the key potential sources of aqSOA from biomass burning in clouds. For the same initial precursor organic gas that dissolves in aerosol/cloud liquid water and subsequently reacts with aqueous phase oxidants, we predict that the aqSOA formation potential (defined as aqSOA formed per unit dissolved organic gas concentration) of these phenols is higher than that of isoprene-epoxydiol (IEPOX), a well-known aqSOA precursor. Cloud droplets can dissolve a broader range of soluble phenols compared to aqueous aerosols, since the liquid water contents of aerosols are orders of magnitude smaller than cloud droplets. Further, our simulations suggest that highly soluble and reactive multifunctional phenols like GA would predominantly undergo cloud chemistry within cloud layers, while gas-phase chemistry is likely to be more important for less soluble phenols. But in the absence of clouds, the condensation of low-volatility products from gas-phase oxidation followed by their reversible partitioning to organic aerosols dominates SOA formation, while the SOA formed through aqueous aerosol chemistry increases with relative humidity (RH), approaching 40% of the sum of gas and aqueous aerosol chemistry at 95% RH for GA. Our model developments of biomass-burning phenols and their aqueous chemistry can be readily implemented in regional and global atmospheric chemistry models to investigate the aqueous aerosol and cloud chemistry of biomass-burning organic gases in the atmosphere.

09 BIOMASS FUELS↗