skip to main content


Title: Impacts of meteorology and emissions on summertime surface ozone increases over central eastern China between 2003 and 2015
Abstract. Recent studies have shown that surface ozone (O3)concentrations over central eastern China (CEC) have increased significantlyduring the past decade. We quantified the effects of changes inmeteorological conditions and O3 precursor emissions on surface O3levels over CEC between July 2003 and July 2015 using the GEOS-Chem model.The simulated monthly mean maximum daily 8 h average O3 concentration(MDA8 O3) in July increased by approximately 13.6 %, from 65.5±7.9 ppbv (2003) to 74.4±8.7 ppbv (2015), comparable to the observedresults. The change in meteorology led to an increase in MDA8 O3 of5.8±3.9 ppbv over the central part of CEC, in contrast to a decreaseof about -0.8±3.5 ppbv over the eastern part of the region. Incomparison, the MDA8 O3 over the central and eastern parts of CECincreased by 3.5±1.4 and 5.6±1.8 ppbv due to the increasedemissions. The increase in averaged O3 in the CEC region resulting fromthe emission increase (4.0±1.9 ppbv) was higher than that caused bymeteorological changes (3.1±4.9 ppbv) relative to the 2003 standardsimulation, while the regions with larger O3 increases showed a highersensitivity to meteorological conditions than to emission changes.Sensitivity tests indicate that increased levels of anthropogenic non-methanevolatile organic compounds (NMVOCs) dominate the O3 increase over theeastern part of CEC, and anthropogenic nitrogen oxides (NOx) mainly increaseMDA8 O3 over the central and western parts and decrease O3 in afew urban areas in the eastern part. Budget analysis showed that netphotochemical production and meteorological conditions (transport inparticular) are two important factors that influence O3 levels over theCEC. The results of this study suggest a need to further assess theeffectiveness of control strategies for O3 pollution in the context ofregional meteorology and anthropogenic emission changes.  more » « less
Award ID(s):
1743401
NSF-PAR ID:
10132416
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ;
Date Published:
Journal Name:
Atmospheric Chemistry and Physics
Volume:
19
Issue:
3
ISSN:
1680-7324
Page Range / eLocation ID:
1455 to 1469
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract. Our work explores the impact of two important dimensions of landsystem changes, land use and land cover change (LULCC) as well as directagricultural reactive nitrogen (Nr) emissions from soils, on ozone(O3) and fine particulate matter (PM2.5) in terms of air quality overcontemporary (1992 to 2014) timescales. We account for LULCC andagricultural Nr emissions changes with consistent remote sensingproducts and new global emission inventories respectively estimating theirimpacts on global surface O3 and PM2.5 concentrations as well as Nrdeposition using the GEOS-Chem global chemical transport model. Over thistime period, our model results show that agricultural Nr emissionchanges cause a reduction of annual mean PM2.5 levels over Europe andnorthern Asia (up to −2.1 µg m−3) while increasing PM2.5 levels in India, China and the eastern US (up to +3.5 µg m−3). Land cover changes induce small reductions in PM2.5 (up to −0.7 µg m−3) over Amazonia, China and India due to reduced biogenic volatile organic compound (BVOC) emissions and enhanced deposition of aerosol precursor gases (e.g., NO2, SO2). Agricultural Nr emissionchanges only lead to minor changes (up to ±0.6 ppbv) in annual meansurface O3 levels, mainly over China, India and Myanmar. Meanwhile, ourmodel result suggests a stronger impact of LULCC on surface O3 over the time period across South America; the combination of changes in drydeposition and isoprene emissions results in −0.8 to +1.2 ppbv surfaceozone changes. The enhancement of dry deposition reduces the surface ozone level (up to −1 ppbv) over southern China, the eastern US and central Africa. The enhancement of soil NO emission due to crop expansion also contributes to surface ozone changes (up to +0.6 ppbv) over sub-Saharan Africa. Incertain regions, the combined effects of LULCC and agricultural Nr emission changes on O3 and PM2.5 air quality can be comparable (>20 %) to anthropogenic emission changes over the same time period. Finally, we calculate that the increase in global agricultural Nr emissions leads to a net increase in global land area (+3.67×106km2) that potentially faces exceedance of the critical Nr load (>5 kg N ha−1 yr−1). Our result demonstrates the impacts of contemporary LULCC and agricultural Nr emission changes on PM2.5 and O3 in terms of air quality, as well as the importanceof land system changes for air quality over multidecadal timescales. 
    more » « less
  2. Abstract. We investigated the ozone pollution trend and its sensitivity to keyprecursors from 1990 to 2015 in the United States using long-term EPA Air Quality System (AQS)observations and mesoscale simulations. The modeling system, a coupledregional climate–air quality model (CWRF-CMAQ; Climate-Weather Research Forecast andthe Community Multiscale Air Quality), captured well the summersurface ozone pollution during the past decades, having a mean slope oflinear regression with AQS observations of ∼0.75. While theAQS network has limited spatial coverage and measures only a few keychemical species, CWRF-CMAQ provides comprehensive simulations to enablea more rigorous study of the change in ozone pollution and chemicalsensitivity. Analysis of seasonal variations and diurnal cycle of ozoneobservations showed that peak ozone concentrations in the summer afternoondecreased ubiquitously across the United States, up to 0.5 ppbv yr−1 in majornon-attainment areas such as Los Angeles, while concentrations at certainhours such as the early morning and late afternoon increased slightly.Consistent with the AQS observations, CMAQ simulated a similar decreasingtrend of peak ozone concentrations in the afternoon, up to 0.4 ppbv yr−1, andincreasing ozone trends in the early morning and late afternoon. A monotonicallydecreasing trend (up to 0.5 ppbv yr−1) in the odd oxygen (Ox=O3+NO2) concentrations are simulated by CMAQ at all daytime hours.This result suggests that the increased ozone in the early morning and lateafternoon was likely caused by reduced NO–O3 titration, driven bycontinuous anthropogenic NOx emission reductions in the past decades.Furthermore, the CMAQ simulations revealed a shift in chemical regimes ofozone photochemical production. From 1990 to 2015, surface ozone productionin some metropolitan areas, such as Baltimore, has transited from aVOC-sensitive environment (>50 % probability) to aNOx-sensitive regime. Our results demonstrated that the long-termCWRF-CMAQ simulations can provide detailed information of the ozonechemistry evolution under a changing climate and may partially explain theUS ozone pollution responses to regional and national regulations. 
    more » « less
  3. Abstract

    This study examines the benefit of using a dynamical ensemble for 48 hr deterministic and probabilistic predictions of near‐surface fine particulate matter (PM2.5) over the contiguous United States (CONUS). Our ensemble design captures three key sources of uncertainties in PM2.5modeling including meteorology, emissions, and secondary organic aerosol (SOA) formation. Twenty‐four ensemble members were simulated using the Community Multiscale Air Quality (CMAQ) model during January, April, July, and October 2016. The raw ensemble mean performed better than most of the ensemble members but underestimated the observed PM2.5over the CONUS with the largest underestimation over the western CONUS owing to negative PM2.5bias in nearly all the members. To improve the ensemble performance, we calibrated the raw ensemble using model output statistics (MOS) and variance deficit methods. The calibrated ensemble captured the diurnal and day‐to‐day variability in observed PM2.5very well and exhibited almost zero mean bias. The mean bias in the calibrated ensemble was reduced by 90–100% in the western CONUS and by 40–100% in other parts of the CONUS, compared to the raw ensemble in all months. The corresponding reduction in root‐mean‐square error (RMSE) was 13–40%. The calibrated ensemble also showed 30% improvement in the RMSE and spread matching compared to the raw ensemble. We have also shown that a nine‐member ensemble based on combinations of three meteorological and three anthropogenic emission scenarios can be used as a smaller subset of the full ensemble when sufficient computational resources are not available in the operational setting.

     
    more » « less
  4. Abstract

    Lightning occurring with less than 2.5 mm of rainfall—typically referred to as ‘dry lightning’—is a major source of wildfire ignition in central and northern California. Despite being rare, dry lightning outbreaks have resulted in destructive fires in this region due to the intersection of dense, dry vegetation and a large population living adjacent to fire-prone lands. Since thunderstorms are much less common in this region relative to the interior West, the climatology and drivers of dry lightning have not been widely investigated in central and northern California. Using daily gridded lightning and precipitation observations (1987–2020) in combination with atmospheric reanalyses, we characterize the climatology of dry lightning and the associated meteorological conditions during the warm season (May–October) when wildfire risk is highest. Across the domain, nearly half (∼46%) of all cloud-to-ground lightning flashes occurred as dry lightning during the study period. We find that higher elevations (>2000 m) receive more dry lightning compared to lower elevations (<1000 m) with activity concentrated in July-August. Although local meteorological conditions show substantial spatial variation, we find regionwide enhancements in mid-tropospheric moisture and instability on dry lightning days relative to background climatology. Additionally, surface temperatures, lower-tropospheric dryness, and mid-tropospheric instability are increased across the region on dry versus wet lightning days. We also identify widespread dry lightning outbreaks in the historical record, quantify their seasonality and spatial extent, and analyze associated large-scale atmospheric patterns. Three of these four atmospheric patterns are characterized by different configurations of ridging over the continental interior and offshore troughing. Understanding the meteorology of dry lightning across this region can inform forecasting of possible wildfire ignitions and is relevant for assessing changes in dry lightning and wildfire risk in climate projections.

     
    more » « less
  5. Abstract. Ground-level ozone (O3) is a major air pollutant that adversely affects human health and ecosystem productivity. Removal of troposphericO3 by plant stomatal uptake can in turn cause damage to plant tissues with ramifications for ecosystem and crop health. In manyatmospheric and land surface models, the functionality of stomata opening is represented by a bulk stomatal conductance, which is oftensemi-empirically parameterized and highly fitted to historical observations. A lack of mechanistic linkage to ecophysiological processes such asphotosynthesis may render models inadequate to represent plant-mediated responses of atmospheric chemistry to long-term changes in CO2,climate, and short-lived air pollutant concentrations. A new ecophysiology module was thus developed to mechanistically simulate land−atmosphereexchange of important gas species in GEOS-Chem, a chemical transport model widely used in atmospheric chemistry studies. The implementation not onlyallows for dry deposition to be coupled with plant ecophysiology but also enables plant and crop productivity and functions to respond dynamically toatmospheric chemical changes. We conduct simulations to evaluate the effects of the ecophysiology module on simulated dry deposition velocity andconcentration of surface O3 against an observation-derived dataset known as SynFlux. Our estimated stomatal conductance and dry depositionvelocity of O3 are close to SynFlux with root-mean-squared errors (RMSEs) below 0.3 cm s−1 across different plant functionaltypes (PFTs), despite an overall positive bias in surface O3 concentration (by up to 16 ppbv). Representing ecophysiology wasfound to reduce the simulated biases in deposition fluxes from the prior model but worsen the positive biases in simulated O3concentrations. The increase in positive concentration biases is mostly attributable to the ecophysiology-based stomatal conductance being generallysmaller (and closer to SynFlux values) than that estimated by the prior semi-empirical formulation, calling for further improvements in non-stomataldepositional and non-depositional processes relevant for O3 simulations. The estimated global O3 deposition flux is864 Tg O3 yr−1 with GEOS-Chem, and the new module decreases this estimate by 92 Tg O3 yr−1. Estimated global grossprimary production (GPP) without O3 damage is 119 Pg C yr−1. O3-induced reduction in GPP is 4.2 Pg C yr−1(3.5 %). An elevated CO2 scenario (580 ppm) yields higher global GPP (+16.8 %) and lower global O3depositional sink (−3.3 %). Global isoprene emission simulated with a photosynthesis-based scheme is 317.9 Tg C yr−1, which is31.2 Tg C yr−1 (−8.9 %) less than that calculated using the MEGAN(Model of Emissions of Gases and Aerosols from Nature) emission algorithm. This new model development dynamicallyrepresents the two-way interactions between vegetation and air pollutants and thus provides a unique capability in evaluating vegetation-mediatedprocesses and feedbacks that can shape atmospheric chemistry and air quality, as well as pollutant impacts on vegetation health, especially for anytimescales shorter than the multidecadal timescale. 
    more » « less