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Henze, Daven K.

Publications and source records attributed to Henze, Daven K..

AMORE-Isoprene v1.0: a new reduced mechanism for gas-phase isoprene oxidation

Abstract. Gas-phase oxidation of isoprene by ozone (O3) and the hydroxyl (OH) and nitrate (NO3) radicals significantly impacts tropospheric oxidant levels and secondary organic aerosol formation. The most comprehensive and up-to-date chemical mechanism for isoprene oxidation consists of several hundred species and over 800 reactions. Therefore, the computational expense of including the entire mechanism in large-scale atmospheric chemical transport models is usually prohibitive, and most models employ reduced isoprene mechanisms ranging in size from ∼ 10 to ∼ 200 species. We have developed a new reduced isoprene oxidation mechanism using a directed-graph path-based automated model reduction approach, with minimal manual adjustment of the output mechanism. The approach takes as inputs a full isoprene oxidation mechanism, the environmental parameter space, and a list of priority species which are protected from elimination during the reduction process. Our reduced mechanism, AMORE-Isoprene (where AMORE stands for Automated Model Reduction), consists of 12 species which are unique to the isoprene mechanism as well as 22 reactions. We demonstrate its performance in a box model in comparison with experimental data from the literature and other current isoprene oxidation mechanisms. AMORE-Isoprene's performance with respect to predicting the time evolution of isoprene oxidation products, including isoprene epoxydiols (IEPOX) and formaldehyde, is favorable compared with other similarly sized mechanisms. When AMORE-Isoprene is included in the Community Regional Atmospheric Chemistry Multiphase Mechanism 1.0 (CRACMM1AMORE) in the Community Multiscale Air Quality Model (CMAQ, v5.3.3), O3 and formaldehyde agreement with Environmental Protection Agency (EPA) Air Quality System observations is improved. O3 bias is reduced by 3.4 ppb under daytime conditions for O3 concentrations over 50 ppb. Formaldehyde bias is reduced by 0.26 ppb on average for all formaldehyde measurements compared with the base CRACMM1. There was no significant change in computation time between CRACMM1AMORE and the base CRACMM. AMORE-Isoprene shows a 35 % improvement in agreement between simulated IEPOX concentrations and chamber data over the base CRACMM1 mechanism when compared in the Framework for 0-D Atmospheric Modeling (F0AM) box model framework. This work demonstrates a new highly reduced isoprene mechanism and shows the potential value of automated model reduction for complex reaction systems.

58 GEOSCIENCES↗

Improvement of aerosol optical depth data for localized solar resource assessment

Solar irradiance, especially for direct normal irradiance (DNI), is sensitive to the atmospheric aerosols, which can strongly extinguish DNI over areas with elevated aerosol loadings. The National Solar Radiation Database (NSRDB), developed by the National Renewable Energy Laboratory (NREL), uses AOD from MERRA-2 reanalysis and is further downscaled from 0.5° to 2-km based on elevation. However, the elevation-based downscaling may not accurately represent AOD, especially over the areas with large AOD gradients. This study examined whether the 1-km MODIS MAIAC satellite-retrieved AOD product can better represent the AOD distribution and be used to improve solar irradiance assessment. We focused on areas with relatively high AOD over North America (California, and New York City, US, and Mexico City in Mexico, in particular). The evaluation of MAIAC AOD and MERRA-2 AOD against ground-truth AERONET AOD shows that MAIAC AOD exhibits smaller RMSE by about 0.05 and higher correlation coefficient by 0.1-0.6 than MERRA-2 AOD. In addition, MERRA-2 AOD shows larger negative bias. The simulated DNI using MAIAC AOD (DNIMAIAC) and using MERRA-2 AOD (DNINSRDB) were evaluated with DNI observations. The results show the performance of DNIMAIAC is better than that of DNINSRDB with smaller RMSE by 0.5-1.5%, smaller positive mean bias by 0.8-3.1% and comparable correlation for the 3 sites analyzed. Overall, 1-km MAIAC AOD shows higher accuracy than 2-km elevation-based MERRA-2 AOD, leading to better performance of the simulated DNI using MAIAC AOD. Therefore, 1-km MAIAC AOD can be used to improve the accuracy of solar resource assessment.

14 SOLAR ENERGY↗

Aircraft-based inversions quantify the importance of wetlands and livestock for Upper Midwest methane emissions

Abstract. We apply airborne measurements across three seasons (summer, winter and spring 2017–2018) in a multi-inversion framework to quantify methane emissions from the US Corn Belt and Upper Midwest, a key agricultural and wetland source region. Combing our seasonal results with prior fall values we find that wetlands are the largest regional methane source (32 %, 20 [16–23] Gg/d), while livestock (enteric/manure; 25 %, 15 [14–17] Gg/d) are the largest anthropogenic source. Natural gas/petroleum, waste/landfills, and coal mines collectively make up the remainder. Optimized fluxes improve model agreement with independent datasets within and beyond the study timeframe. Inversions reveal coherent and seasonally dependent spatial errors in the WetCHARTs ensemble mean wetland emissions, with an underestimate for the Prairie Pothole region but an overestimate for Great Lakes coastal wetlands. Wetland extent and emission temperature dependence have the largest influence on prediction accuracy; better representation of coupled soil temperature–hydrology effects is therefore needed. Our optimized regional livestock emissions agree well with the Gridded EPA estimates during spring (to within 7 %) but are ∼ 25 % higher during summer and winter. Spatial analysis further shows good top-down and bottom-up agreement for beef facilities (with mainly enteric emissions) but larger (∼ 30 %) seasonal discrepancies for dairies and hog farms (with > 40 % manure emissions). Findings thus support bottom-up enteric emission estimates but suggest errors for manure; we propose that the latter reflects inadequate treatment of management factors including field application. Overall, our results confirm the importance of intensive animal agriculture for regional methane emissions, implying substantial mitigation opportunities through improved management.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

What Factors Control the Trend of Increasing AAOD Over the United States in the Last Decade?

We examine the spatial and temporal trends of absorbing aerosol optical depth (AAOD) in the last decade over the United States (U.S.) observed by the Ozone Monitoring Instrument (OMI). Monthly average OMI AAOD has increased over broad areas of the central U.S. from 2005 to 2015, by up to a factor of 4 in some grid cells (~60 km resolution). The AAOD increases in all seasons, although the percentage increases are larger in summer (June-July-August) than in winter (December-January-February) by a factor of 3. Despite enhancements in AAOD, OMI AOD exhibits insignificant trend over most of the U.S. except parts of the central and western U.S., the latter which may partly be due to decreases in precipitation. Trends in AAOD contrast with declining trends in surface concentrations of black carbon (BC) aerosol. Interannual variability of local biomass burning emissions of BC may contribute to the positive trend in AAOD over the western U.S. Changes in both dust aerosol measured at the surface (in terms of concentration and size) and dust AAOD indicate distinct enhancements, especially over the central U.S. by 50-100%, which appears to be one of the major factors that impacts positive trends in AAOD.

Satellite retrieval↗

Satellite Data of Atmospheric Pollution for U.S. Air Quality Applications: Examples of Applications, Summary of Data End-User Resources, Answers to FAQs, and Common Mistakes to Avoid

Satellite data of atmospheric pollutants are becoming more widely used in the decision-making and environmental management activities of public, private sector and non-profit organizations. They are employed for estimating emissions, tracking pollutant plumes, supporting air quality forecasting activities, providing evidence for "exceptional event" declarations, monitoring regional long-term trends, and evaluating air quality model output. However, many air quality managers are not taking full advantage of the data for these applications nor has the full potential of satellite data for air quality applications been realized. A key barrier is the inherent difficulties associated with accessing, processing, and properly interpreting observational data. A degree of technical skill is required on the part of the data end-user, which is often problematic for air quality agencies with limited resources. Therefore, we 1) review the primary uses of satellite data for air quality applications, 2) provide some background information on satellite capabilities for measuring pollutants, 3) discuss the many resources available to the end-user for accessing, processing, and visualizing the data, and 4) provide answers to common questions in plain language.

Duncan, Bryan↗

Emissions Estimation from Satellite Retrievals: a Review of Current Capability

Since the mid-1990s a new generation of Earth-observing satellites has been able to detect tropospheric air pollution at increasingly high spatial and temporal resolution. Most primary emitted species can be measured by one or more of the instruments. This review article addresses the question of how well we can relate the satellite measurements to quantification of primary emissions and what advances are needed to improve the usability of the measurements by U.S. air quality managers. Built on a comprehensive literature review and comprising input by both satellite experts and emission inventory specialists, the review identifies several targets that seem promising: large point sources of NOx and SO2, species that are difficult to measure by other means (NH3 and CH4, for example), area sources that cannot easily be quantified by traditional bottom-up methods (such as unconventional oil and gas extraction, shipping, biomass burning, and biogenic sources), and the temporal variation of emissions (seasonal, diurnal, episodic). Techniques that enhance the usefulness of current retrievals (data assimilation, oversampling, multi-species retrievals, improved vertical profiles, etc.) are discussed. Finally, we point out the value of having new geostationary satellites like GEO-CAPE and TEMPO over North America that could provide measurements at high spatial (few km) and temporal (hourly) resolution.

air quality↗

Spatially Refined Aerosol Direct Radiative Forcing Efficiencies

Global aerosol direct radiative forcing (DRF) is an important metric for assessing potential climate impacts of future emissions changes. However, the radiative consequences of emissions perturbations are not readily quantified nor well understood at the level of detail necessary to assess realistic policy options. To address this challenge, here we show how adjoint model sensitivities can be used to provide highly spatially resolved estimates of the DRF from emissions of black carbon (BC), primary organic carbon (OC), sulfur dioxide (SO2), and ammonia (NH3), using the example of emissions from each sector and country following multiple Representative Concentration Pathway (RCPs). The radiative forcing efficiencies of many individual emissions are found to differ considerably from regional or sectoral averages for NH3, SO2 from the power sector, and BC from domestic, industrial, transportation and biomass burning sources. Consequently, the amount of emissions controls required to attain a specific DRF varies at intracontinental scales by up to a factor of 4. These results thus demonstrate both a need and means for incorporating spatially refined aerosol DRF into analysis of future emissions scenario and design of air quality and climate change mitigation policies.

Climate↗

Top-down Estimate of Dust Emissions Through Integration of MODIS and MISR Aerosol Retrievals With the Geos-chem Adjoint Model

Predicting the influences of dust on atmospheric composition, climate, and human health requires accurate knowledge of dust emissions, but large uncertainties persist in quantifying mineral sources. This study presents a new method for combined use of satellite-measured radiances and inverse modeling to spatially constrain the amount and location of dust emissions. The technique is illustrated with a case study in May 2008; the dust emissions in Taklimakan and Gobi deserts are spatially optimized using the GEOSChem chemical transport model and its adjoint constrained by aerosol optical depth (AOD) that are derived over the downwind dark-surface region in China from MODIS (Moderate Resolution Imaging Spectroradiometer) reflectance with the aerosol single scattering properties consistent with GEOS-chem. The adjoint inverse modeling yields an overall 51% decrease in prior dust emissions estimated by GEOS-Chem over the Taklimakan-Gobi area, with more significant reductions south of the Gobi Desert. The model simulation with optimized dust emissions shows much better agreement with independent observations from MISR (Multi-angle Imaging SpectroRadiometer) AOD and MODIS Deep Blue AOD over the dust source region and surface PM10 concentrations. The technique of this study can be applied to global multi-sensor remote sensing data for constraining dust emissions at various temporal and spatial scales, and hence improving the quantification of dust effects on climate, air quality, and human health.

MODIS aerosol retrievals↗

Quantifying Spatial and Seasonal Variability in Atmospheric Ammonia with In Situ and Space-Based Observations

Ammonia plays an important role in many biogeochemical processes, yet atmospheric mixing ratios are not well known. Recently, methods have been developed for retrieving NH3 from space-based observations, but they have not been compared to in situ measurements. We have conducted a field campaign combining co-located surface measurements and satellite special observations from the Tropospheric Emission Spectrometer (TES). Our study includes 25 surface monitoring sites spanning 350 km across eastern North Carolina, a region with large seasonal and spatial variability in NH3. From the TES spectra, we retrieve a NH3 representative volume mixing ratio (RVMR), and we restrict our analysis to times when the region of the atmosphere observed by TES is representative of the surface measurement. We find that the TES NH3 RVMR qualitatively captures the seasonal and spatial variability found in eastern North Carolina. Both surface measurements and TES NH3 show a strong correspondence with the number of livestock facilities within 10 km of the observation. Furthermore, we find that TES H3 RVMR captures the month-to-month variability present in the surface observations. The high correspondence with in situ measurements and vast spatial coverage make TES NH3 RVMR a valuable tool for understanding regional and global NH3 fluxes.

Pinder, Robert W.↗