An Analysis of CMAQ Gas Phase Dry Deposition over North America Through Grid-Scale and Land-Use Specific Diagnostics in the Context of AQMEII4.

The fourth phase of the Air Quality Model Evaluation International Initiative (AQMEII4) is conducting a diagnostic intercomparison and evaluation of deposition simulated by regional-scale air quality models over North America and Europe. In this study, we analyze annual AQMEII4 simulations performed with the Community Multiscale Air Quality Model (CMAQ) version 5.3.1 over North America. These simulations were configured with both the M3Dry and Surface Tiled Aerosol and Gas Exchange (STAGE) dry deposition schemes available in CMAQ. A comparison of observed and modeled concentrations and wet deposition fluxes shows that the AQMEII4 CMAQ simulations perform similarly to other contemporary regional-scale modeling studies. During summer, M3Dry has higher ozone (O3) deposition velocities (Vd) and lower mixing ratios than STAGE for much of the eastern U.S. while the reverse is the case over eastern Canada and along the West Coast. In contrast, during winter STAGE has higher O3 Vd and lower mixing ratios than M3Dry over most of the southern half of the modeling domain while the reverse is the case for much of the northern U.S. and southern Canada. Analysis of the diagnostic variables defined for the AQMEII4 project, i.e. grid-scale and land-use (LU) specific effective conductances and deposition fluxes for the major dry deposition pathways, reveals generally higher summertime stomatal and wintertime cuticular grid-scale effective conductances for M3Dry and generally higher soil grid-scale effective conductances (for both vegetated and bare soil) for STAGE in both summer and winter. On a domain-wide basis, the stomatal grid-scale effective conductances account for about half of the total O3 Vd during daytime hours in summer for both schemes. Employing LU-specific diagnostics, results show that daytime Vd varies by a factor of 2 between LU categories. Furthermore, M3Dry vs. STAGE differences are most pronounced for the stomatal and vegetated soil pathway for the forest LU categories, with M3Dry estimating larger effective conductances for the stomatal pathway and STAGE estimating larger effective conductances for the vegetated soil pathway for these LU categories. Annual domain total O3 deposition fluxes differ only slightly between M3Dry (74.4 Tg/year) and STAGE (76.2 Tg/yr), but pathway-specific fluxes to individual LU types can vary more substantially on both annual and seasonal scales which would affect estimates of O3 damages to sensitive vegetation. A comparison of two simulations differing only in their LU classification scheme shows that the differences in LU cause seasonal mean O3 mixing ratio differences on the order of 1 ppb across large portions of the domain, with the differences generally largest during summer and in areas characterized by the largest differences in the fractional coverages of the forest, planted/cultivated, and grassland LU categories. These differences are generally smaller than the M3Dry vs. STAGE differences outside the summer season but have a similar magnitude during summer. Results indicate that the deposition impacts of LU differences are caused both by differences in the fractional coverages and spatial distributions of different LU categories as well as the characterization of these categories through variables like surface roughness and vegetation fraction in look-up tables used in the land-surface model and deposition schemes. Overall, the analyses and results presented in this study illustrate how the diagnostic grid-scale and LU-specific dry deposition variables adopted for AQMEII4 can provide insights into similarities and differences between the CMAQ M3Dry and STAGE dry deposition schemes that affect simulated pollutant budgets and ecosystem impacts from atmospheric pollution.

2002-2017 anthropogenic emissions data for air quality modeling over the United States.

The United States Environmental Protection Agency (US EPA) has developed a set of annual North American emissions data for multiple air pollutants across 18 broad source categories for 2002 through 2017. The sixteen new annual emissions inventories were developed using consistent input data and methods across all years. When a consistent method or tool was not available for a source category, emissions were estimated by scaling data from the EPA's 2017 National Emissions Inventory with scaling factors based on activity data and/or emissions control information. The emissions datasets are designed to support regional air quality modeling for a wide variety of human health and ecological applications. The data were developed to support simulations of the EPA's Community Multiscale Air Quality model but can also be used by other regional scale air quality models. The emissions data are one component of EPA's Air Quality Time Series Project which also includes air quality modeling inputs (meteorology, initial conditions, boundary conditions) and outputs (e.g., ozone, PM2.5 and constituent species, wet and dry deposition) for the Conterminous US at a 12 km horizontal grid spacing.

Human-health impacts of controlling secondary air pollution precursors.

Exposure to ozone and fine particle (PM2.5) air pollution results in premature death. These pollutants are predominantly secondary in nature and can form from nitrogen oxides (NOX), sulfur oxides (SOX), and volatile organic compounds (VOCs). Predicted health benefits for emission reduction scenarios often incompletely account for VOCs as precursors as well as the secondary organic aerosol (SOA) component of PM2.5. Here, we show that anthropogenic VOC emission reductions are more than twice as effective as equivalent fractional reductions of SOX or NOX at reducing air pollution-associated cardiorespiratory mortality in the United States. A 25% reduction in anthropogenic VOC emissions from 2016 levels is predicted to avoid 13,000 premature deaths per year, and most (85%) of the VOC-reduction benefits result from reduced SOA with the remainder from ozone. While NOX (-5.7 ± 0.2 % yr-1) and SOX (-12 ± 1 % yr-1) emissions have declined precipitously across the U.S. since 2002, anthropogenic VOC emissions (-1.8 ± 0.3 % yr-1) and concentrations of non-methane organic carbon (-2.4 ± 1.0 % yr-1) have changed less. This work indicates preferentially controlling VOCs could yield significant benefits to human health.

Secondary organic aerosol association with cardiorespiratory disease mortality in the United States.

Fine particle pollution, PM2.5, is associated with increased risk of death from cardiorespiratory diseases. A multidecadal shift in the United States (U.S.) PM2.5 composition towards organic aerosol as well as advances in predictive algorithms for secondary organic aerosol (SOA) allows for novel examinations of the role of PM2.5 components on mortality. Here we show SOA is strongly associated with county-level cardiorespiratory death rates in the U.S. independent of the total PM2.5 mass association with the largest associations located in the southeastern U.S. Compared to PM2.5, county-level variability in SOA across the U.S. is associated with 3.5× greater per capita county-level cardiorespiratory mortality. On a per mass basis, SOA is associated with a 6.5× higher rate of mortality than PM2.5, and biogenic and anthropogenic carbon sources both play a role in the overall SOA association with mortality. Our results suggest reducing the health impacts of PM2.5 requires consideration of SOA.

The Community Multiscale Air Quality (CMAQ) model versions 5.3 and 5.3.1: system updates and evaluation.

The Community Multiscale Air Quality (CMAQ) model version 5.3 (CMAQ53), released to the public in August 2019 and followed by version 5.3.1 (CMAQ531) in December 2019, contains numerous science updates, enhanced functionality, and improved computation efficiency relative to the previous version of the model, 5.2.1 (CMAQ521). Major science advances in the new model include a new aerosol module (AERO7) with significant updates to secondary organic aerosol (SOA) chemistry, updated chlorine chemistry, updated detailed bromine and iodine chemistry, updated simple halogen chemistry, the addition of dimethyl sulfide (DMS) chemistry in the CB6r3 chemical mechanism, updated M3Dry bidirectional deposition model, and the new Surface Tiled Aerosol and Gaseous Exchange (STAGE) bidirectional deposition model. In addition, support for the Weather Research and Forecasting (WRF) model's hybrid vertical coordinate (HVC) was added to CMAQ53 and the Meteorology-Chemistry Interface Processor (MCIP) version 5.0 (MCIP50). Enhanced functionality in CMAQ53 includes the new Detailed Emissions Scaling, Isolation and Diagnostic (DESID) system for scaling incoming emissions to CMAQ and reading multiple gridded input emission files. Evaluation of CMAQ531 was performed by comparing monthly and seasonal mean daily 8 h average (MDA8) O3 and daily PM2.5 values from several CMAQ531 simulations to a similarly configured CMAQ521 simulation encompassing 2016. For MDA8 O3, CMAQ531 has higher O3 in the winter versus CMAQ521, due primarily to reduced dry deposition to snow, which strongly reduces wintertime O3 bias (2-4 ppbv monthly average). MDA8 O3 is lower with CMAQ531 throughout the rest of the year, particularly in spring, due in part to reduced O3 from the lateral boundary conditions (BCs), which generally increases MDA8 O3 bias in spring and fall ( 0.5 µg m-3). For daily 24 h average PM2.5, CMAQ531 has lower concentrations on average in spring and fall, higher concentrations in summer, and similar concentrations in winter to CMAQ521, which slightly increases bias in spring and fall and reduces bias in summer. Comparisons were also performed to isolate updates to several specific aspects of the modeling system, namely the lateral BCs, meteorology model version, and the deposition model used. Transitioning from a hemispheric CMAQ (HCMAQ) version 5.2.1 simulation to a HCMAQ version 5.3 simulation to provide lateral BCs contributes to higher O3 mixing ratios in the regional CMAQ simulation in higher latitudes during winter (due to the decreased O3 dry deposition to snow in CMAQ53) and lower O3 mixing ratios in middle and lower latitudes year-round (due to reduced O3 over the ocean with CMAQ53). Transitioning from WRF version 3.8 to WRF version 4.1.1 with the HVC resulted in consistently higher (1.0-1.5 ppbv) MDA8 O3 mixing ratios and higher PM2.5 concentrations (0.1-0.25 µg m-3) throughout the year. Finally, comparisons of the M3Dry and STAGE deposition models showed that MDA8 O3 is generally higher with M3Dry outside of summer, while PM2.5 is consistently higher with STAGE due to differences in the assumptions of particle deposition velocities to non-vegetated surfaces and land use with short vegetation (e.g., grasslands) between the two models. For ambient NH3, STAGE has slightly higher concentrations and smaller bias in the winter, spring, and fall, while M3Dry has higher concentrations and smaller bias but larger error and lower correlation in the summer.

The Detailed Emissions Scaling, Isolation, and Diagnostic (DESID) module in the Community Multiscale Air Quality (CMAQ) modeling system version 5.3.2.

Air quality modeling for research and regulatory applications often involves executing many emissions sensitivity cases to quantify impacts of hypothetical scenarios, estimate source contributions, or quantify uncertainties. Despite the prevalence of this task, conventional approaches for perturbing emissions in chemical transport models like the Community Multiscale Air Quality (CMAQ) model require extensive offline creation and finalization of alternative emissions input files. This workflow is often time-consuming, error-prone, inconsistent among model users, difficult to document, and dependent on increased hard disk resources. The Detailed Emissions Scaling, Isolation, and Diagnostic (DESID) module, a component of CMAQv5.3 and beyond, addresses these limitations by performing these modifications online during the air quality simulation. Further, the model contains an Emission Control Interface which allows users to prescribe both simple and highly complex emissions scaling operations with control over individual or multiple chemical species, emissions sources, and spatial areas of interest. DESID further enhances the transparency of its operations with extensive error-checking and optional gridded output of processed emission fields. These new features are of high value to many air quality applications including routine perturbation studies, atmospheric chemistry research, and coupling with external models (e.g., energy system models, reduced-form models).

Novel experimental setup for megahertz X-ray diffraction in a diamond anvil cell at the High Energy Density (HED) instrument of the European X-ray Free-Electron Laser (EuXFEL).

The high-precision X-ray diffraction setup for work with diamond anvil cells (DACs) in interaction chamber 2 (IC2) of the High Energy Density instrument of the European X-ray Free-Electron Laser is described. This includes beamline optics, sample positioning and detector systems located in the multipurpose vacuum chamber. Concepts for pump-probe X-ray diffraction experiments in the DAC are described and their implementation demonstrated during the First User Community Assisted Commissioning experiment. X-ray heating and diffraction of Bi under pressure, obtained using 20 fs X-ray pulses at 17.8 keV and 2.2 MHz repetition, is illustrated through splitting of diffraction peaks, and interpreted employing finite element modeling of the sample chamber in the DAC.

Impact of real mirror profiles inside a split-and-delay unit on the spatial intensity profile in pump/probe experiments at the European XFEL.

For the High-Energy-Density (HED) beamline at the SASE2 undulator of the European XFEL, a hard X-ray split-and-delay unit (SDU) has been built enabling time-resolved pump/probe experiments with photon energies between 5 keV and 24 keV. The optical layout of the SDU is based on geometrical wavefront splitting and multilayer Bragg mirrors. Maximum delays between Δτ = ±1 ps at 24 keV and Δτ = ±23 ps at 5 keV will be possible. Time-dependent wavefront propagation simulations were performed by means of the Synchrotron Radiation Workshop (SRW) software in order to investigate the impact of the optical layout, including diffraction on the beam splitter and recombiner edges and the three-dimensional topography of all eight mirrors, on the spatio-temporal properties of the XFEL pulses. The radiation is generated from noise by the code FAST which simulates the self-amplified spontaneous emission (SASE) process. A fast Fourier transformation evaluation of the disturbed interference pattern yields for ideal mirror surfaces a coherence time of τc = 0.23 fs and deduces one of τc = 0.21 fs for the real mirrors, thus with an error of Δτ = 0.02 fs which is smaller than the deviation resulting from shot-to-shot fluctuations of SASE2 pulses. The wavefronts are focused by means of compound refractive lenses in order to achieve fluences of a few hundred mJ mm-2 within a spot width of 20 µm (FWHM) diameter. Coherence effects and optics imperfections increase the peak intensity between 200 and 400% for pulse delays within the coherence time. Additionally, the influence of two off-set mirrors in the HED beamline are discussed. Further, we show the fluence distribution for Δz = ±3 mm around the focal spot along the optical axis. The simulations show that the topographies of the mirrors of the SDU are good enough to support X-ray pump/X-ray probe experiments.

High-resolution inelastic x-ray scattering at the high energy density scientific instrument at the European X-Ray Free-Electron Laser.

We introduce a setup to measure high-resolution inelastic x-ray scattering at the High Energy Density scientific instrument at the European X-Ray Free-Electron Laser (XFEL). The setup uses the Si (533) reflection in a channel-cut monochromator and three spherical diced analyzer crystals in near-backscattering geometry to reach a high spectral resolution. An energy resolution of 44 meV is demonstrated for the experimental setup, close to the theoretically achievable minimum resolution. The analyzer crystals and detector are mounted on a curved-rail system, allowing quick and reliable changes in scattering angle without breaking vacuum. The entire setup is designed for operation at 10 Hz, the same repetition rate as the high-power lasers available at the instrument and the fundamental repetition rate of the European XFEL. Among other measurements, it is envisioned that this setup will allow studies of the dynamics of highly transient laser generated states of matter.

An approach for the measurement of the bulk temperature of single crystal diamond using an X-ray free electron laser.

We present a method to determine the bulk temperature of a single crystal diamond sample at an X-Ray free electron laser using inelastic X-ray scattering. The experiment was performed at the high energy density instrument at the European XFEL GmbH, Germany. The technique, based on inelastic X-ray scattering and the principle of detailed balance, was demonstrated to give accurate temperature measurements, within [Formula: see text] for both room temperature diamond and heated diamond to 500 K. Here, the temperature was increased in a controlled way using a resistive heater to test theoretical predictions of the scaling of the signal with temperature. The method was tested by validating the energy of the phonon modes with previous measurements made at room temperature using inelastic X-ray scattering and neutron scattering techniques. This technique could be used to determine the bulk temperature in transient systems with a temporal resolution of 50 fs and for which accurate measurements of thermodynamic properties are vital to build accurate equation of state and transport models.

Inducing signal-verified lucid dreams in 40% of untrained novice lucid dreamers within two nights in a sleep laboratory setting.

Dreams in which the dreamer is aware of the dream state (lucid dreams, LD) are difficult to induce in naïve subjects in-laboratory. Recently, Stumbrys and Erlacher (2014) used a combination of existing induction techniques together with a self-developed experiment protocol and achieved comparatively high LD induction rates. In this study, we simplified their methodology slightly and repeated their experiment with twenty naïve subjects who spent one or two nights in our sleep laboratory. After about six hours of sleep, they were woken up during REM sleep and engaged in a series of cognitive tasks before going back to bed. Ten subjects reported a LD during the following period of sleep in one of the nights. Eight of these subjects gave a predefined eye signal, which was clearly visible in the electrooculogram during REM sleep. In summary, we replicated Stumbrys and Erlacher's results using a simplified version of their induction protocol.

The impact of air pollutant deposition on solar energy system efficiency: An approach to estimate PV soiling effects with the Community Multiscale Air Quality (CMAQ) model.

Deposition and accumulation of aerosol particles on photovoltaics (PV) panels, which is commonly referred to as "soiling of PV panels," impacts the performance of the PV energy system. It is desirable to estimate the soiling effect at different locations and times for modeling the PV system performance and devising cost-effective mitigation. This study presents an approach to estimate the soiling effect by utilizing particulate matter (PM) dry deposition estimates from air quality model simulations. The Community Multiscale Air Quality (CMAQ) modeling system used in this study was developed by the U.S. Environmental Protection Agency (U.S. EPA) for air quality assessments, rule-making, and research. Three deposition estimates based on different surface roughness length parameters assumed in CMAQ were used to illustrate the soling effect in different land-use types. The results were analyzed for three locations in the U.S. for year 2011. One urban and one suburban location in Colorado were selected because there have been field measurements of particle deposition on solar panels and analysis on the consequent soiling effect performed at these locations. The third location is a coastal city in Texas, the City of Brownsville. These three locations have distinct ambient environments. CMAQ underestimates particle deposition by 40% to 80% when compared to the field measurements at the two sites in Colorado due to the underestimations in both the ambient PM10 concentration and deposition velocity. The estimated panel transmittance sensitivity due to the deposited particles is higher than the sensitivity obtained from the measurements in Colorado. The final soiling effect, which is transmittance loss, is estimated as 3.17 ±â€¯4.20% for the Texas site, 0.45 ±â€¯0.33%, and 0.31 ±â€¯0.25% for the Colorado sites. Although the numbers are lower compared to the measurements in Colorado, the results are comparable with the soiling effects observed in U.S.

Setup for meV-resolution inelastic X-ray scattering measurements and X-ray diffraction at the Matter in Extreme Conditions endstation at the Linac Coherent Light Source.

We describe a setup for performing inelastic X-ray scattering and X-ray diffraction measurements at the Matter in Extreme Conditions (MEC) endstation of the Linac Coherent Light Source. This technique is capable of performing high-, meV-resolution measurements of dynamic ion features in both crystalline and non-crystalline materials. A four-bounce silicon (533) monochromator was used in conjunction with three silicon (533) diced crystal analyzers to provide an energy resolution of ∼50 meV over a range of ∼500 meV in single shot measurements. In addition to the instrument resolution function, we demonstrate the measurement of longitudinal acoustic phonon modes in polycrystalline diamond. Furthermore, this setup may be combined with the high intensity laser drivers available at MEC to create warm dense matter and subsequently measure ion acoustic modes.

Constraining chemical transport PM2.5 modeling outputs using surface monitor measurements and satellite retrievals: application over the San Joaquin Valley.

Advances in satellite retrieval of aerosol type can improve the accuracy of near-surface air quality characterization by providing broad regional context and decreasing metric uncertainties and errors. The frequent, spatially extensive and radiometrically consistent instantaneous constraints can be especially useful in areas away from ground monitors and progressively downwind of emission sources. We present a physical approach to constraining regional-scale estimates of PM2.5, its major chemical component species estimates, and related uncertainty estimates of chemical transport model (CTM; e.g., the Community Multi-scale Air Quality Model) outputs. This approach uses ground-based monitors where available, combined with aerosol optical depth and qualitative constraints on aerosol size, shape, and light-absorption properties from the Multi-angle Imaging SpectroRadiometer (MISR) on the NASA Earth Observing System's Terra satellite. The CTM complements these data by providing complete spatial and temporal coverage. Unlike widely used approaches that train statistical regression models, the technique developed here leverages CTM physical constraints such as the conservation of aerosol mass and meteorological consistency, independent of observations. The CTM also aids in identifying relationships between observed species concentrations and emission sources. Aerosol air mass types over populated regions of central California are characterized using satellite data acquired during the 2013 San Joaquin field deployment of the NASA Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) project. We investigate the optimal application of incorporating 275 m horizontal-resolution aerosol air-mass-type maps and total-column aerosol optical depth from the MISR Research Aerosol retrieval algorithm (RA) into regional-scale CTM output. The impact on surface PM2.5 fields progressively downwind of large single sources is evaluated using contemporaneous surface observations. Spatiotemporal R 2 and RMSE values for the model, constrained by both satellite and surface monitor measurements based on 10-fold cross-validation, are 0.79 and 0.33 for PM2.5, 0.88 and 0.65 for NO3 -, 0.78 and 0.23 for SO4 2-, and 1.01 for NH+, 0.73 and 0.23 for OC, and 0.31 and 0.65 for EC, respectively. Regional cross-validation temporal and spatiotemporal R2 results for the satellite-based PM2.5 improve by 30 % and 13 %, respectively, in comparison to unconstrained CTM simulations and provide finer spatial resolution. SO4 2- cross-validation values showed the largest spatial and spatiotemporal R2 improvement, with a 43 % increase. Assessing this physical technique in a well- instrumented region opens the possibility of applying it globally, especially over areas where surface air quality measurements are scarce or entirely absent.

Coupling of organic and inorganic aerosol systems and the effect on gas-particle partitioning in the southeastern US.

Several models were used to describe the partitioning of ammonia, water, and organic compounds between the gas and particle phases for conditions in the southeastern US during summer 2013. Existing equilibrium models and frameworks were found to be sufficient, although additional improvements in terms of estimating pure-species vapor pressures are needed. Thermodynamic model predictions were consistent, to first order, with a molar ratio of ammonium to sulfate of approximately 1.6 to 1.8 (ratio of ammonium to 2× sulfate, RN/2S ≈ 0.8 to 0.9) with approximately 70% of total ammonia and ammonium (NH x ) in the particle. Southeastern Aerosol Research and Characterization Network (SEARCH) gas and aerosol and Southern Oxidant and Aerosol Study (SOAS) Monitor for AeRosols and Gases in Ambient air (MARGA) aerosol measurements were consistent with these conditions. CMAQv5.2 regional chemical transport model predictions did not reflect these conditions due to a factor of 3 overestimate of the nonvolatile cations. In addition, gas-phase ammonia was overestimated in the CMAQ model leading to an even lower fraction of total ammonia in the particle. Chemical Speciation Network (CSN) and aerosol mass spectrometer (AMS) measurements indicated less ammonium per sulfate than SEARCH and MARGA measurements and were inconsistent with thermodynamic model predictions. Organic compounds were predicted to be present to some extent in the same phase as inorganic constituents, modifying their activity and resulting in a decrease in [H+]air (H+ in µgm-3 air), increase in ammonia partitioning to the gas phase, and increase in pH compared to complete organic vs. inorganic liquid-liquid phase separation. In addition, accounting for nonideal mixing modified the pH such that a fully interactive inorganic-organic system had a pH roughly 0.7 units higher than predicted using traditional methods (pH = 1.5 vs. 0.7). Particle-phase interactions of organic and inorganic compounds were found to increase partitioning towards the particle phase (vs. gas phase) for highly oxygenated (O : C≥0.6) compounds including several isoprene-derived tracers as well as levoglu-cosan but decrease particle-phase partitioning for low O: C, monoterpene-derived species.

A sensitive EUV Schwarzschild microscope for plasma studies with sub-micrometer resolution.

We present an extreme ultraviolet (EUV) microscope using a Schwarzschild objective which is optimized for single-shot sub-micrometer imaging of laser-plasma targets. The microscope has been designed and constructed for imaging the scattering from an EUV-heated solid-density hydrogen jet. Imaging of a cryogenic hydrogen target was demonstrated using single pulses of the free-electron laser in Hamburg (FLASH) free-electron laser at a wavelength of 13.5 nm. In a single exposure, we observe a hydrogen jet with ice fragments with a spatial resolution in the sub-micrometer range. In situ EUV imaging is expected to enable novel experimental capabilities for warm dense matter studies of micrometer-sized samples in laser-plasma experiments.

Development and evaluation of a physics-based windblown dust emission scheme implemented in the CMAQ modeling system.

A new windblown dust emission treatment was incorporated in the Community Multiscale Air Quality (CMAQ) modeling system. This new model treatment has been built upon previously developed physics-based parameterization schemes from the literature. A distinct and novel feature of this scheme, however, is the incorporation of a newly developed dynamic relation for the surface roughness length relevant to small-scale dust generation processes. Through this implementation, the effect of nonerodible elements on the local flow acceleration, drag partitioning, and surface coverage protection is modeled in a physically based and consistent manner. Careful attention is paid in integrating the new windblown dust treatment in the CMAQ model to ensure that the required input parameters are correctly configured. To test the performance of the new dust module in CMAQ, the entire year 2011 is simulated for the continental United States, with particular emphasis on the southwestern United States (SWUS) where windblown dust concentrations are relatively large. Overall, the model shows good performance with the daily mean bias of soil concentrations fluctuating in the range of ±1 µg m-3 for the entire year. Springtime soil concentrations are in quite good agreement (normalized mean bias of 8.3%) with observations, while moderate to high underestimation of soil concentration is seen in the summertime. The latter is attributed to the issue of representing the convective dust storms in summertime. Evaluations against observations for seven elevated dust events in the SWUS indicate that the new windblown dust treatment is capable of capturing spatial and temporal characteristics of dust outbreaks.

On the implications of aerosol liquid water and phase separation for organic aerosol mass.

Organic compounds and liquid water are major aerosol constituents in the southeast United States (SE US). Water associated with inorganic constituents (inorganic water) can contribute to the partitioning medium for organic aerosol when relative humidities or organic matter to organic carbon (OM/OC) ratios are high such that separation relative humidities (SRH) are below the ambient relative humidity (RH). As OM/OC ratios in the SE US are often between 1.8 and 2.2, organic aerosol experiences both mixing with inorganic water and separation from it. Regional chemical transport model simulations including inorganic water (but excluding water uptake by organic compounds) in the partitioning medium for secondary organic aerosol (SOA) when RH > SRH led to increased SOA concentrations,· particularly at night. Water uptake to the organic phase resulted in even greater SOA concentrations as a result of a positive feedback in which water uptake increased SOA, which further increased aerosol water and organic aerosol. Aerosol properties· such as the OM/OC and hygroscopicity parameter (κorg), were captured well by the model compared with measurements during the Southern Oxidant and Aerosol Study (SOAS) 2013. Organic nitrates from monoterpene oxidation were predicted to be the least water-soluble semivolatile species in the model, but most biogenically derived semivolatile species in the Community Multiscale Air Quality (CMAQ) model were highly water soluble and expected to contribute to water-soluble organic carbon (WSOC). Organic aerosol and SOA precursors were abundant at night, but additional improvements in daytime organic aerosol are needed to close the model-measurement gap. When taking into account deviations from ideality, including both inorganic (when RH > SRH) and organic water in the organic partitioning medium reduced the mean bias in SOA for routine monitoring networks and improved model performance compared to observations from SOAS. Property updates from this work will be released in CMAQ v5.2.