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All sourcesNASA NTRSDOE OSTI
NASA NTRS2021

Grid-Stretching Capability for the GEOS-Chem 13.0.0 Atmospheric Chemistry Model

Modeling atmospheric chemistry at fine resolution globally is computationally expensive; the capability to focus on specific geographic regions using a multi scale grid is desirable. Here, we develop, validate, and demonstrate stretched grids in the GEOS-Chem atmospheric chemistry model in its high-performance implementation (GCHP). These multiscale grids are specified at runtime by four parameters that offer users nimble control of the region that is refined and the resolution of the refinement. We validate the stretched-grid simulation versus global cubed-sphere simulations. We demonstrate the operation and flexibility of stretched-grid simulations with two case studies that compare simulated tropospheric NO2column densities from stretched-grid and cubed-sphere simulations to retrieved column densities from the TROPOspheric Monitoring Instrument (TROPOMI). The first case study uses a stretched grid with a broad refinement covering the contiguous US to produces imulated columns that perform similarly to a C180 (∼50 km) cubed-sphere simulation at less than one-ninth the computational expense. The second case study experiments with a large stretch-factor for a global stretched-grid simulation with a highly localized refinement with∼10 km resolution for California. We find that the refinement improves spatial agreement with TROPOMI columns compared to a C90 cubed-sphere simulation of comparable computational demands. Overall we find that stretched grids in GEOS-Chem are a practical tool for fine resolution regional- or continental-scale simulations of atmospheric chemistry. Stretched grids are available in GEOS-Chem version 13.0.0

GEOS-Chem↗
NASA NTRSDate not supplied

High resolution assimilation of multiple satellite retrievals with emissions adjustment to improve air quality forecasting with WRF-Chem/DART

We will present results from medium (15km, 6hr cycling) and high (4 km, 6 hr cycling) spatiotemporal resolution applications of the WRF-Chem/DART ensemble, regional, air quality (AQ) forecast/assimilation system.The medium-resolution setup is applied to the Discover AQ/Front Range Air Pollution and Photochemistry Experiment (FRAPPE) domain from July 14 to July 29, 2014. The high-resolution setup is applied to a Colorado domain from July 14 to July 29, 2020. For the FRAPPE application, we assimilate MOPITT CO; IASI CO;MODIS AOD; OMI O3, NO2; and AirNow CO, O3, NO2, SO2, PM10, and PM2.5. For the Colorado application, we assimilate the same MOPITT, MODIS, and AirNow constituents as in the FRAPPE application and TROPOMI CO, O3, NO2; and synthetic TEMPO O3and NO2. WRF-Chem/DART integrates the Weather Research and Forecast (WRF) model with on-line chemistry (WRF-Chem) into the Data Assimilation Research Testbed (DART). It assimilates AirNow CO, O3, NO2, SO2, PM10, and PM2.5 measurements, MOPITT CO; IASI CO, O3; OMI O3, NO2, SO2; TROPOMI CO, O3, NO2, SO2; MODIS AOD; and synthetic TEMPO O3 and NO2 total/partial column and/or profile retrievals.WRF-Chem/DART uses: (i) the state augmentation method for adjusting emissions; (ii) state-space localization; and (iii) a near-real time scripting system. We use the medium-resolution FRAPPE application to demonstrate the incremental benefits from assimilating OMI observations with emissions adjustment and the high-resolution Colorado application to demonstrate the incremental benefits from assimilating syntheticTEMPO observations with emissions adjustment. For both applications, we expect that: (i) assimilating chemical observations will increaseAQ forecast skill; (ii) including emissions adjustment will increase forecast skill/predictability; and (iii) including assimilation of synthetic TEMPO observations will further increase forecast skill/predictability.

High resolution↗
DOE OSTI2015

Seasonal and interannual variability in wetland methane emissions simulated by CLM4Me' and CAM-chem and comparisons to observations of concentrations

Understanding the temporal and spatial variation of wetland methane emissions is essential to the estimation of the global methane budget. Our goal for this study is three-fold: (i) to evaluate the wetland methane fluxes simulated in two versions of the Community Land Model, the Carbon-Nitrogen (CN; i.e., CLM4.0) and the Biogeochemistry (BGC; i.e., CLM4.5) versions using the methane emission model CLM4Me' so as to determine the sensitivity of the emissions to the underlying carbon model; (ii) to compare the simulated atmospheric methane concentrations to observations, including latitudinal gradients and interannual variability so as to determine the extent to which the atmospheric observations constrain the emissions; (iii) to understand the drivers of seasonal and interannual variability in atmospheric methane concentrations. Simulations of the transport and removal of methane use the Community Atmosphere Model with chemistry (CAM-chem) model in conjunction with CLM4Me' methane emissions from both CN and BGC simulations and other methane emission sources from literature. In each case we compare model-simulated atmospheric methane concentration with observations. In addition, we simulate the atmospheric concentrations based on the TransCom wetland and rice paddy emissions derived from a different terrestrial ecosystem model, Vegetation Integrative Simulator for Trace gases (VISIT). Our analysis indicates CN wetland methane emissions are higher in the tropics and lower at high latitudes than emissions from BGC. In CN, methane emissions decrease from 1993 to 2004 while this trend does not appear in the BGC version. In the CN version, methane emission variations follow satellite-derived inundation wetlands closely. However, they are dissimilar in BGC due to its different carbon cycle. CAM-chem simulations with CLM4Me' methane emissions suggest that both prescribed anthropogenic and predicted wetlands methane emissions contribute substantially to seasonal and interannual variability in atmospheric methane concentration. Simulated atmospheric CH 4 concentrations in CAM-chem are highly correlated with observations at most of the 14 measurement stations evaluated with an average correlation between 0.71 and 0.80 depending on the simulation (for the period of 1993–2004 for most stations based on data availability). Our results suggest that different spatial patterns of wetland emissions can have significant impacts on Northern and Southern hemisphere (N–S) atmospheric CH 4 concentration gradients and growth rates. In conclusion, this study suggests that both anthropogenic and wetland emissions have significant contributions to seasonal and interannual variations in atmospheric CH 4 concentrations. However, our analysis also indicates the existence of large uncertainties in terms of spatial patterns and magnitude of global wetland methane budgets, and that substantial uncertainty comes from the carbon model underlying the methane flux modules.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2017

Improvements to the WRF-Chem 3.5.1 model for quasi-hemispheric simulations of aerosols and ozone in the Arctic

In this study, the WRF-Chem regional model is updated to improve simulated short-lived pollutants (e.g., aerosols, ozone) in the Arctic. Specifically, we include in WRF-Chem 3.5.1 (with SAPRC-99 gas-phase chemistry and MOSAIC aerosols) (1) a correction to the sedimentation of aerosols, (2) dimethyl sulfide (DMS) oceanic emissions and gas-phase chemistry, (3) an improved representation of the dry deposition of trace gases over seasonal snow, and (4) an UV-albedo dependence on snow and ice cover for photolysis calculations. We also (5) correct the representation of surface temperatures over melting ice in the Noah Land Surface Model and (6) couple and further test the recent KF-CuP (Kain–Fritsch + Cumulus Potential) cumulus parameterization that includes the effect of cumulus clouds on aerosols and trace gases. The updated model is used to perform quasi-hemispheric simulations of aerosols and ozone, which are evaluated against surface measurements of black carbon (BC), sulfate, and ozone as well as airborne measurements of BC in the Arctic. The updated model shows significant improvements in terms of seasonal aerosol cycles at the surface and root mean square errors (RMSEs) for surface ozone, aerosols, and BC aloft, compared to the base version of the model and to previous large-scale evaluations of WRF-Chem in the Arctic. These improvements are mostly due to the inclusion of cumulus effects on aerosols and trace gases in KF-CuP (improved RMSE for surface BC and BC profiles, surface sulfate, and surface ozone), the improved surface temperatures over sea ice (surface ozone, BC, and sulfate), and the updated trace gas deposition and UV albedo over snow and ice (improved RMSE and correlation for surface ozone). DMS emissions and chemistry improve surface sulfate at all Arctic sites except Zeppelin, and correcting aerosol sedimentation has little influence on aerosols except in the upper troposphere.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

A new parameterization of ice heterogeneous nucleation coupled to aerosol chemistry in WRF-Chem model version 3.5.1: evaluation through ISDAC measurements

In the Arctic, during polar night and early spring, ice clouds are separated into two leading types of ice clouds (TICs): (1) TIC1 clouds characterized by a large concentration of very small crystals and TIC2 clouds characterized by a low concentration of large ice crystals. Using a suitable parameterization of heterogeneous ice nucleation is essential for properly representing ice clouds in meteorological and climate models and subsequently understanding their interactions with aerosols and radiation. Here, we describe a new parameterization for ice crystal formation by heterogeneous nucleation in water-subsaturated conditions coupled to aerosol chemistry in the Weather Research and Forecasting model coupled with chemistry (WRF-Chem). The parameterization is implemented in the Milbrandt and Yau (2005a, b) two-moment cloud microphysics scheme, and we assess how the WRF-Chem model responds to the run-time interaction between chemistry and the new parameterization. Well-documented reference cases provided us with in situ data from the spring 2008 Indirect and Semi-Direct Aerosol Campaign (ISDAC) over Alaska. Our analysis reveals that the new parameterization clearly improves the representation of the ice water content (IWC) in polluted or unpolluted air masses and shows the poor performance of the reference parameterization in representing ice clouds with low IWC. The new parameterization is able to represent TIC1 and TIC2 microphysical characteristics at the top of the clouds, where heterogenous ice nucleation is most likely occurring, even with the known bias of simulated aerosols by WRF-Chem over the Arctic.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

Twelve-month, 12 km resolution North American WRF-Chem v3.4 air quality simulation: performance evaluation

We present results from and evaluate the performance of a 12-month, 12 km horizontal resolution year 2005 air pollution simulation for the contiguous United States using the WRF-Chem (Weather Research and Forecasting with Chemistry) meteorology and chemical transport model (CTM). We employ the 2005 US National Emissions Inventory, the Regional Atmospheric Chemistry Mechanism (RACM), and the Modal Aerosol Dynamics Model for Europe (MADE) with a volatility basis set (VBS) secondary aerosol module. Overall, model performance is comparable to contemporary modeling efforts used for regulatory and health-effects analysis, with an annual average daytime ozone (O 3 ) mean fractional bias (MFB) of 12% and an annual average fine particulate matter (PM 2.5 ) MFB of −1%. WRF-Chem, as configured here, tends to overpredict total PM 2.5 at some high concentration locations and generally overpredicts average 24 h O 3 concentrations. Performance is better at predicting daytime-average and daily peak O 3 concentrations, which are more relevant for regulatory and health effects analyses relative to annual average values. Predictive performance for PM 2.5 subspecies is mixed: the model overpredicts particulate sulfate (MFB = 36%), underpredicts particulate nitrate (MFB = −110%) and organic carbon (MFB = −29%), and relatively accurately predicts particulate ammonium (MFB = 3%) and elemental carbon (MFB = 3%), so that the accuracy in total PM 2.5 predictions is to some extent a function of offsetting over- and underpredictions of PM 2.5 subspecies. Model predictive performance for PM 2.5 and its subspecies is in general worse in winter and in the western US than in other seasons and regions, suggesting spatial and temporal opportunities for future WRF-Chem model development and evaluation.

Tessum, C. W. (ORCID:0000000288647436)↗
NASA NTRS2005

Incorporation of a Chemical Equilibrium Equation of State into LOCI-Chem

Renewed interest in development of advanced high-speed transport, reentry vehicles and propulsion systems has led to a resurgence of research into high speed aerodynamics. As this flow regime is typically dominated by hot reacting gaseous flow, efficient models for the characteristic chemical activity are necessary for accurate and cost effective analysis and design of aerodynamic vehicles that transit this regime. The LOCI-Chem code recently developed by Ed Luke at Mississippi State University for NASA/MSFC and used by NASA/MSFC and SSC represents an important step in providing an accurate, efficient computational tool for the simulation of reacting flows through the use of finite-rate kinetics [3]. Finite rate chemistry however, requires the solution of an additional N-1 species mass conservation equations with source terms involving reaction kinetics that are not fully understood. In the equilibrium limit, where the reaction rates approach infinity, these equations become very stiff. Through the use of the assumption of local chemical equilibrium the set of governing equations is reduced back to the usual gas dynamic equations, and thus requires less computation, while still allowing for the inclusion of reacting flow phenomenology. The incorporation of a chemical equilibrium equation of state module into the LOCI-Chem code was the primary objective of the current research. The major goals of the project were: (1) the development of a chemical equilibrium composition solver, and (2) the incorporation of chemical equilibrium solver into LOCI-Chem. Due to time and resource constraints, code optimization was not considered unless it was important to the proper functioning of the code.

Cox, Carey F.↗
NASA NTRS2004

CHEM-Based Self-Deploying Spacecraft Radar Antennas

A document proposes self-deploying spacecraft radar antennas based on cold hibernated elastic memory (CHEM) structures. Described in a number of prior NASA Tech Briefs articles, the CHEM concept is one of utilizing open-cell shape-memory-polymer (SMP) foams to make lightweight structures that can be compressed for storage and can later be expanded, then rigidified for use. A CHEM-based antenna according to the proposal would comprise three layers of microstrip patches and transmission lines interspersed with two flat layers of SMP foam, which would serve as both dielectric spacers and as means of deployment. The SMP foam layers would be fabricated at full size at a temperature below the SMP glass-transition temperature (Tg). The layers would be assembled into a unitary structure, which, at temperature above Tg, would be compacted to much smaller thickness, then rolled up for storage. Next, the structure would be cooled to below Tg and kept there during launch. Upon reaching the assigned position in outer space, the structure would be heated above Tg to make it rebound to its original size and shape. The structure as thus deployed would then be rigidified by natural cooling to below Tg

Sokolowski, Witold↗
NASA NTRS2019

Analysis of A Severe Dust Storm and Its Impact on Air Quality Conditions Using Wrf-Chem Modeling, Satellite Imagery, and Ground Observations

This study presents a comprehensive analysis of an extreme dust event recorded in the Arabian Peninsula and the United Arab Emirates (UAE) between 31 March and 3 April 2015. Simulations of the dust event with the Weather Research and Forecasting model coupled with the Chemistry module (WRF-Chem) were analyzed and verified using MSG-SEVIRI imagery and aerosol optical depth (AOD) from the recent 1-km Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithm for MODIS Terra/Aqua. Data from the National Centers for Atmospheric Prediction/National Center for Atmospheric Research (NCEP/NCAR) and the upper-air radiosonde observations were used to understand the synoptic of the event. In addition, the impact of the event on atmospheric and air quality conditions is investigated. The Air Quality Index (AQI) was calculated prior, during, and after the event to assess the degradation of air quality conditions. Simulated temperature, relative humidity, wind speed, and surface radiation were compared to observations at six monitoring stations in the UAE giving R2 values of 0.84, 0.63, 0.60, and 0.84, respectively. From 1 to 2 April 2015, both observations and simulations showed an average drop in temperature from 33 to 26 °C and radiance reduction from about 950 to 520 Wm−2. The AOD modeled by WRF-Chem showed a good correlation with Aerosol Robotic Network (AERONET) measurements in the UAE with R2 of 0.83. The AQI over the UAE reached hazardous levels during the peak of the dust event before rapidly decreasing to moderate–good air quality levels. This work is the first attempt to demonstrate the potential of using WRF-Chem to estimate AQI over the UAE along with two satellite products (MODIS-MAIAC and MSG-SEVIRI) for dust detection and tracking.

dust storm↗
NASA NTRS2021

Harmonized Emissions Component (HEMCO) 3.0 as a Versatile Emissions Component for Atmospheric Models: Application in the GEOS-Chem, NASA GEOS, WRF-GC, CESM2, NOAA GEFS-Aerosol, and NOAA UFS Models

Emissions are a central component of atmospheric chemistry models. The Harmonized Emissions Component (HEMCO) is a software component for computing emissions from a user-selected ensemble of emission inventories and algorithms. It allows users to re-grid, combine, overwrite, subset, and scale emissions from different inventories through a configuration file and with no change to the model source code. The configuration file also maps emissions to model species with appropriate units. HEMCO can operate in offline stand-alone mode, but more importantly it provides an online facility for models to compute emissions at runtime. HEMCO complies with the Earth System Modeling Framework (ESMF) for portability across models. We present a new version here, HEMCO 3.0, that features an improved three-layer architecture to facilitate implementation into any atmospheric model and improved capability for calculating emissions at any model resolution including multiscale and unstructured grids. The three-layer architecture of HEMCO 3.0 includes (1) the Data Input Layer that reads the configuration file and accesses the HEMCO library of emission inventories and other environmental data, (2) the HEMCO Core that computes emissions on the user-selected HEMCO grid, and (3) the Model Interface Layer that re-grids (if needed) and serves the data to the atmospheric model and also serves model data to the HEMCO Core for computing emissions dependent on model state (such as from dust or vegetation). The HEMCO Core is common to the implementation in all models, while the Data Input Layer and the Model Interface Layer are adaptable to the model environment. Default versions of the Data Input Layer and Model Interface Layer enable straightforward implementation of HEMCO in any simple model architecture, and options are available to disable features such as re-gridding that may be done by independent couplers in more complex architectures. The HEMCO library of emission inventories and algorithms is continuously enriched through user contributions so that new inventories can be immediately shared across models. HEMCO can also serve as a general data broker for models to process input data not only for emissions but for any gridded environmental datasets. We describe existing implementations of HEMCO 3.0 in (1) the GEOS-Chem “Classic” chemical transport model with shared-memory infrastructure, (2) the high-performance GEOS-Chem (GCHP) model with distributed-memory architecture, (3) the NASA GEOS Earth System Model (GEOS ESM), (4) the Weather Research and Forecasting model with GEOS-Chem (WRF-GC), (5) the Community Earth System Model Version 2 (CESM2), and (6) the NOAA Global Ensemble Forecast System – Aerosols (GEFS-Aerosols), as well as the planned implementation in the NOAA Unified Forecast System (UFS). Implementation of HEMCO in CESM2 contributes to the Multi-Scale Infrastructure for Chemistry and Aerosols (MUSICA) by providing a common emissions infrastructure to support different simulations of atmospheric chemistry across scales.

Haipeng Lin↗
DOE OSTI2025

Sensitivity of Regional WRF‐Chem Air Quality and Weather Simulations to Biomass‐Burning Emission Data Sets: A Case Study of the Impact of Canadian Wildfire on the US°

This study focuses on the period from June 26 to 29, 2023, when record‐breaking Canadian wildfires severely impacted air quality in the Midwest United States. Using the Weather Research and Forecasting Model with Chemistry (WRF‐Chem) and four biomass‐burning data sets (Fire Inventory from NCAR version 1, Fire Inventory from NCAR version 2.5, Quick Fire Emissions Data set [QFED], and Regional ABI‐VIIRS Emission), we analyzed aerosol transport from Canada to the US and assessed the model's accuracy in predicting PM 2.5 , O 3 , CO and aerosol weather feedback. Model simulations were compared with ground‐based and remote sensing observations as well as field measurements from the Community Research on Climate and Urban Science (CROCUS) project. Our findings show that the movement of a low‐pressure system from the Great Lakes to the Atlantic, combined with the high‐pressure system over the Atlantic, caused the transport of aerosols from Canadian wildfires to the US. Results show WRF‐Chem significantly underestimated key atmospheric components: aerosol optical depth (AOD) by over 50%, PM 2.5 by 65%–90% and peak O 3 concentrations by 50%–55% across four biomass burning data sets. Additionally, CO and NO 2 concentrations were underpredicted. The substantial underestimation of PM 2.5 led to an overestimation of temperature by up to 3.6 °C primarily due to excessive downward shortwave radiation, which resulted from the underestimation of direct aerosol effects and an increase in sensible heat flux. Among the biomass‐burning data sets, QFED produced the most accurate AOD and PM 2.5 predictions due to improved wildfire emission estimates, leading to a 1.0 to 1.5 °C reduction in temperature overestimation during the daytime. These findings underscore the need for improving wildfire emission estimates for trace gases and aerosols to enhance air quality and weather feedback predictions.

WRF-chem model↗
NASA NTRSDate not supplied

Assimilation of GEO and LEO Satellite Retrievals in WRF-Chem (15 km and 4 km) with ‘Top-Down’ Emissions Estimation

We are constraining concentrations and emissions for all criteria pollutants (CO, O3, NO2, SO2, PM10, and PM2.5) with WRF-Chem/DART in applications for FRAPPE (15-km grid) and COLORADO (4-km grid). Our results show that: (i) dynamic emissions estimation at medium resolutions (15 km) improves forecast skill; (ii) At high resolutions, the results look good, but we do not have validation data; (iii) for what may be the first time, we assimilate O3 retrieval profiles in a regional model. The problem is that the averaging kernels generally extend above the upper boundary of regional models. We use O3 upper boundary conditions from the global model to solve that problem; and (iv) In the high resolution experiments, we document the potential benefits of assimilating TEMPO O3 profile and NO2 tropospheric column retrievals. Here, we assimilate proxy TEMPO retrievals from a GEOS-Chem nature run, so there’s a conceptual problem due to the potential bias of the proxy retrievals, but the point is to demonstrate our ability to assimilate TEMPO and identify its potential impacts.

Chemical data assimilation↗
DOE OSTI2017

Improvement of the prediction of surface ozone concentration over conterminous U.S. by a computationally efficient second-order Rosenbrock solver in CAM4-Chem

The global chemistry-climate model (CAM4-Chem) overestimates the surface ozone concentration over the conterminous U.S. (CONUS). Reasons for this positive bias include emission, meteorology, chemical mechanism, and solver. In this study, we explore the last possibility by examining the sensitivity to the numerical methods for solving the chemistry equations. A second-order Rosenbrock (ROS-2) solver is implemented in CAM4-Chem to examine its influence on the surface ozone concentration and the computational performance of the chemistry program. Results show that under the same time step size (1800 s), statistically significant reduction of positive bias is achieved by the ROS-2 solver. The improvement is as large as 5.2 ppb in Eastern U.S. during summer season. The ROS-2 solver is shown to reduce the positive bias in Europe and Asia as well, indicating the lower surface ozone concentration over the CONUS predicted by the ROS-2 solver is not a trade-off consequence with increasing the ozone concentration at other global regions. In addition, by refining the time step size to 180 s, the first-order implicit solver does not provide statistically significant improvement of surface ozone concentration. It reveals that the better prediction from the ROS-2 solver is not only due to its accuracy but also due to its suitability for stiff chemistry equations. As an added benefit, the computation cost of the ROS-2 solver is almost half of first-order implicit solver. The improved computational efficiency of the ROS-2 solver is due to the reuse of the Jacobian matrix and lower upper (LU) factorization during its multistage calculation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Using gap-filled MAIAC AOD and WRF-Chem to estimate daily PM 2.5 concentrations at 1 km resolution in the Eastern United States

To link short-term exposures of air pollutants to health outcomes, scientists must use high temporal and spatial resolution estimates of PM 2.5 concentrations. We develop a daily PM 2.5 product at 1 × 1 km 2 spatial resolution across the eastern United States (east of 90° W) with the aid of 1 × 1 km 2 MAIAC aerosol optical depth (AOD) data, 36 × 36 km 2 WRF-Chem output, 1 × 1 km 2 land-use type from the National Land Cover Database, and 0.125° × 0.125° ERA-Interim re-analysis meteorology. A gap-filling technique is applied to MAIAC AOD data to construct robust daily estimates of AOD when the satellite data are missing (e.g., areas obstructed by clouds or snow cover). The input data are incorporated into a multiple-linear regression model trained to surface observations of PM 2.5 from the EPA Air Quality System (AQS) monitoring network. The model generates a high-fidelity estimate (r 2 = 0.75 using a 10-fold random cross-validation) of daily PM 2.5 throughout the eastern United States. Of the inputs to the statistical model, WRF-Chem output (r 2 = 0.66) is the most important contributor to the skill of the model. MAIAC AOD is also a strong contributor (r 2 = 0.52). Daily PM 2.5 output from our statistical model can be easily integrated into county-level epidemiological studies. The novelty of this project is that we are able to simulate PM 2.5 in a computationally efficient manner that is constrained to ground monitors, satellite data, and chemical transport model output at high spatial resolution (1 × 1 km 2 ) without sacrificing the temporal resolution (daily) or spatial coverage (>2,000,000 km 2 ).

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

Global Simulations of Phase State and Equilibration Time Scales of Secondary Organic Aerosols with GEOS-Chem

The phase state of secondary organic aerosols (SOA) can range from liquid through amorphous semisolid to glassy solid, which is important to consider as it influences various multiphase processes including SOA formation and partitioning, multiphase chemistry, and cloud activation. In this study, we simulate the glass transition temperature and viscosity of SOA over the globe using the global chemical transport model, GEOS-Chem. The simulated spatial distributions show that SOA at the surface exist as liquid over equatorial regions and oceans, semisolid in the midlatitude continental regions, and glassy solid over lands with low relative humidity. The predicted SOA viscosities are mostly consistent with the available measurements. In the free troposphere, SOA particles are mostly predicted to be semisolid at 850 hPa and glassy solid at 500 hPa, except over tropical regions including Amazonia, where SOA are predicted to be low viscous. Phase state also exhibits seasonal variation with a higher frequency of semisolid and solid particles in winter compared to warmer seasons. We calculate equilibration time scales of SOA partitioning (τ eq ) and effective mass accommodation coefficient (α eff ), indicating that τ eq is shorter than the chemical time step of GEOS-Chem of 20 min and αeff is close to unity for most locations at the surface level, supporting the application of equilibrium SOA partitioning. However, τ eq is prolonged and α eff is lowered over drylands and most regions in the upper troposphere, suggesting that kinetically limited growth would need to be considered for these regions in future large-scale model studies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Sensitivity of Simulated Aerosol Properties Over Eastern North America to WRF-Chem Parameterizations

Aerosol properties and their climatic feedbacks are characterized by high uncertainty in both global and regional model simulations. We explore sources of uncertainty in the representation of aerosol properties using an ensemble of simulations performed at 24 km resolution with WRF-Chem over eastern North America. The sensitivity of aerosol optical depth (AOD) and near-surface fine particle concentrations (PM 2.5 ) to planetary boundary layer (PBL) and aerosol schemes (modal with secondary organic aerosol (SOA) versus sectional but excluding SOA), as well as different emission inventories (National Emission Inventory (NEI) 2005 versus 2011) is examined. Here, we quantify the spread among ensemble members with respect to the model setup and compute statistical metrics to identify the run configuration that exhibits greatest fidelity relative to observations of aerosol and meteorological properties. Use of the Modal Aerosol Dynamics Model for Europe/Secondary Organic Aerosol Model scheme leads to highest agreement with MODIS clear-sky AOD observations particularly when the 2005 NEI is used (with either PBL scheme). These members exhibit small negative mean fractional bias over the simulation domain (<2%), and relatively high spatial correlation in summertime mean monthly AOD (>0.5). The aerosol scheme and NEI dominate the ensemble spread in AOD. Near-surface PM 2.5 is also dependent on PBL scheme and is best reproduced in runs adopting a sectional approach and emissions for 2011. Thus, WRF-Chem configuration associated with highest agreement with AOD observations is not the same as for PM 2.5 , possibly reflecting the importance of columnar water vapor in dictating AOD.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Impact of light-absorbing particles on snow albedo darkening and associated radiative forcing over high-mountain Asia: high-resolution WRF-Chem modeling and new satellite observations

Light-absorbing particles (LAPs), mainly dust and black carbon, can significantly impact snowmelt and regional water availability over high-mountain Asia (HMA). In this study, for the first time, online aerosol–snow interactions are enabled and a fully coupled chemistry Weather Research and Forecasting (WRF-Chem) regional model is used to simulate LAP-induced radiative forcing on snow surfaces in HMA at relatively high spatial resolution (12 km, WRF-HR) compared with previous studies. Simulated macro- and microphysical properties of the snowpack and LAP-induced snow darkening are evaluated against new spatially and temporally complete datasets of snow-covered area, grain size, and impurity-induced albedo reduction over HMA. A WRF-Chem quasi-global simulation with the same configuration as WRF-HR buta coarser spatial resolution (1°, WRF-CR) is also used to illustrate the impact of spatial resolution on simulations of snow properties and aerosol distribution over HMA. Due to a more realistic representation of terrain slopes over HMA, the higher-resolution model (WRF-HR) shows significantly better performance in simulating snow area cover, duration of snow cover, snow albedo and snow grain size over HMA, as well as an evidently better atmospheric aerosol loading and mean LAP concentration in snow. However, the differences in albedo reduction from model and satellite retrievals is large during winter due to associated overestimation in simulated snow fraction. It is noteworthy that Himalayan snow cover has high magnitudes of LAP-induced snow albedo reduction (4% - 8%) in pre-monsoon seasons (both from WRF-HR and satellite estimates), which induces a snow-mediated radiative forcing of ~30-50 W m -2 . As a result, the Himalayas (specifically the western Himalayas) hold the most vulnerable glaciers and mountain snowpack to the LAP-induced snow darkening effect within HMA. In summary, coarse spatial resolution and absence of snow–aerosol interactions over the Himalayan cryosphere will result insignificant underestimation of aerosol effects on snow melting and regional hydroclimate.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Simulation of radon-222 with the GEOS-Chem global model: Emissions, seasonality, and convective transport

Radon-222 (222Rn) is a short-lived radioactive gas naturally emitted from land surface, and has long been used to assess convective transport in atmospheric models. In this study, we simulate 222Rn using the GEOS-Chem chemical transport model with aims to improve our understanding of 222Rn emissions and surface concentration seasonality, and to characterize convective transport associated with two Goddard Earth Observing System (GEOS) meteorological products, MERRA and GEOS-FP. We evaluate four available 222Rn emission scenarios by comparing model results with surface observations at 51 global surface sites. The default emission scenario in GEOS-Chem yields a moderate agreement with global surface observations (< 70% data within a factor of 2) and a large underestimate of wintertime surface 222Rn concentrations at Northern Hemisphere mid- and high-latitudes due to an oversimplified formulation of 222Rn emission fluxes (1 atom cm-2 s-1 over land with a reduction by a factor of 3 under freezing conditions). We compose a new global 222Rn emission scenario based on Zhang et al. (2011) and show its potential to improve simulated surface 222Rn concentrations and seasonality. The regional components of this emission scenario include spatially and temporally varying emission fluxes derived from previous measurements of soil radium content and soil exhalation models, which are key factors to 222Rn emission flux rates. However, large model underestimates of surface 222Rn concentrations still exist in Asia, suggesting unusually high regional 222Rn emissions. We propose a conservative up-scaling factor of 1.2 for 222Rn emission fluxes in China, as also constrained by the observed deposition fluxes of 210Pb (decay daughter of 222Rn). With this modification, the model shows better agreement with the observations in Europe and North America (>80% data within a factor of 2), and reasonable agreement in Asia (close to 70%). Further constraints on 222Rn emissions would require additional observations of surface 222Rn concentrations and emission fluxes in central U.S., Canada, Africa, and Asia. We also compare and assess convective transport in model simulations driven by MERRA and GEOS-FP using observed 222Rn vertical profiles during northern mid-latitude summertime and from two short-term airborne campaigns. While the simulations with both GEOS products are able to capture the observed vertical gradient of 222Rn concentrations in the lower troposphere (0-4 km), neither correctly represents the level of convective detrainment, resulting in biases in the middle and upper troposphere. Compared to GEOS-FP, MERRA leads to stronger convective transport of 222Rn, which is partially compensated by its weaker large-scale vertical advection, resulting in similar global vertical distributions of 222Rn concentrations between the two simulations.

Zhang, Bo↗