skip to main content

Title: Importance of dry deposition parameterization choice in global simulations of surface ozone
Abstract. Dry deposition is a major sink of tropospheric ozone.Increasing evidence has shown that ozone dry deposition actively linksmeteorology and hydrology with ozone air quality. However, there is littlesystematic investigation on the performance of different ozone drydeposition parameterizations at the global scale and how parameterizationchoice can impact surface ozone simulations. Here, we present the results ofthe first global, multidecadal modelling and evaluation of ozone drydeposition velocity (vd) using multiple ozone dry depositionparameterizations. We model ozone dry deposition velocities over 1982–2011using four ozone dry deposition parameterizations that are representative ofcurrent approaches in global ozone dry deposition modelling. We useconsistent assimilated meteorology, land cover, and satellite-derived leafarea index (LAI) across all four, such that the differences in simulatedvd are entirely due to differences in deposition model structures orassumptions about how land types are treated in each. In addition, we usethe surface ozone sensitivity to vd predicted by a chemical transportmodel to estimate the impact of mean and variability of ozone dry depositionvelocity on surface ozone. Our estimated vd values from four differentparameterizations are evaluated against field observations, and whileperformance varies considerably by land cover types, our results suggestthat none of the parameterizations are universally better than the others.Discrepancy in simulated mean vd more » among the parameterizations isestimated to cause 2 to 5 ppbv of discrepancy in surface ozone in theNorthern Hemisphere (NH) and up to 8 ppbv in tropical rainforests in July,and up to 8 ppbv in tropical rainforests and seasonally dry tropical forestsin Indochina in December. Parameterization-specific biases based onindividual land cover type and hydroclimate are found to be the two maindrivers of such discrepancies. We find statistically significant trends inthe multiannual time series of simulated July daytime vd in allparameterizations, driven by warming and drying (southern Amazonia, southernAfrican savannah, and Mongolia) or greening (high latitudes). The trend inJuly daytime vd is estimated to be 1 % yr−1 and leadsto up to 3 ppbv of surface ozone changes over 1982–2011. The interannual coefficient ofvariation (CV) of July daytime mean vd in NH is found to be5 %–15 %, with spatial distribution that varies with the dry depositionparameterization. Our sensitivity simulations suggest this can contributebetween 0.5 to 2 ppbv to interannual variability (IAV) in surface ozone, butall models tend to underestimate interannual CV when compared to long-termozone flux observations. We also find that IAV in some dry depositionparameterizations is more sensitive to LAI, while in others it is more sensitiveto climate. Comparisons with other published estimates of the IAV ofbackground ozone confirm that ozone dry deposition can be an important partof natural surface ozone variability. Our results demonstrate the importanceof ozone dry deposition parameterization choice on surface ozone modellingand the impact of IAV of vd on surface ozone, thus making a strong casefor further measurement, evaluation, and model–data integration of ozone drydeposition on different spatiotemporal scales. « less
Authors:
; ; ;
Award ID(s):
1750328
Publication Date:
NSF-PAR ID:
10131161
Journal Name:
Atmospheric Chemistry and Physics
Volume:
19
Issue:
22
Page Range or eLocation-ID:
14365 to 14385
ISSN:
1680-7324
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 ofmore »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.« less
  2. Fire causes abrupt changes in vegetation properties and modifies flux exchanges between land and atmosphere at subseasonal to seasonal scales. Yet these shortterm fire effects on vegetation dynamics and surface energy balance have not been comprehensively investigated in the fire-coupled vegetation model. This study applies the SSiB4/TRIFFID-Fire (the Simplified Simple Biosphere Model coupled with the Top-down Representation of Interactive Foliage and Flora Including Dynamics with fire) model to study the short-term fire impact in southern Africa. Specifically, we aim to quantify how large impacts fire exerts on surface energy through disturbances on vegetation dynamics, how fire effects evolve during themore »fire season and the subsequent rainy season, and how surface-darkening effects play a role besides the vegetation change effects. We find fire causes an annual average reduction in grass cover by 4 %–8% for widespread areas between 5–20 S and a tree cover reduction by 1% at the southern periphery of tropical rainforests. The regional fire effects accumulate during June–October and peak in November, the beginning of the rainy season. After the fire season ends, the grass cover quickly returns to unburned conditions, while the tree fraction hardly recovers in one rainy season. The vegetation removal by fire has reduced the leaf area index (LAI) and gross primary productivity (GPP) by 3 %–5% and 5 %–7% annually. The exposure of bare soil enhances surface albedo and therefore decreases the absorption of shortwave radiation. Annual mean sensible heat has dropped by 1.4Wm−2, while the latent heat reduction is small (0.1Wm−2/ due to the evaporation. Surface temperature is increased by as much as 0.33K due to the decrease of sensible heat fluxes, and the warming would be enhanced when the surface-darkening effect is incorporated. Our results suggest that fire effects in grass-dominant areas diminish within 1 year due to the high resilience of grasses after fire. Yet fire effects in the periphery of tropical forests are irreversible within one growing season and can cause large-scale deforestation if accumulated for hundreds of years.« less
  3. To simulate global mercury (Hg) dynamics in chemical transport models (CTMs), surface-atmosphere exchange of gaseous elemental mercury, Hg 0 , is often parameterized based on resistance-based dry deposition schemes coupled with a re-emission function, mainly from soils. Despite extensive use of this approach, direct evaluations of this implementation against field observations of net Hg 0 exchange are lacking. In this study, we evaluate an existing net exchange parameterization (referred to here as the base model) by comparing modeled fluxes of Hg 0 to fluxes measured in the field using micrometeorological techniques. Comparisons were performed in two terrestrial ecosystems: a grasslandmore »site in Switzerland and an Arctic tundra site in Alaska, U.S., each including summer and winter seasons. The base model included the dry deposition and soil re-emission parameterizations from Zhang et al. (2003) and the global CTM GEOS-Chem, respectively. Comparisons of modeled and measured Hg 0 fluxes showed large discrepancies, particularly in the summer months when the base model overestimated daytime net deposition by approximately 9 and 2 ng m −2 h −1 at the grassland and tundra sites, respectively. In addition, the base model was unable to capture a measured nighttime net Hg 0 deposition and wintertime deposition. We conducted a series of sensitivity analyses and recommend that Hg simulations using CTMs: (i) reduce stomatal uptake of Hg 0 over grassland and tundra in models by a factor 5–7; (ii) increase nighttime net Hg 0 deposition, e.g. , by increasing ground and cuticular uptake by reducing the respective resistance terms by factors of 3–4 and 2–4, respectively; and (iii) implement a new soil re-emission parameterization to produce larger daytime emissions and lower nighttime emissions. We also compared leaf Hg 0 uptake over the growing season estimated by the dry deposition model against foliar Hg measurements, which revealed good agreement with the measured leaf Hg concentrations after adjusting the base model as suggested above. We conclude that the use of resistance-based models combined with the new soil re-emission flux parameterization is able to reproduce observed diel and seasonal patterns of Hg 0 exchange in these ecosystems. This approach can be used to improve model parameterizations for other ecosystems if flux measurements become available.« less
  4. Abstract. Fire causes abrupt changes in vegetation properties and modifies fluxexchanges between land and atmosphere at subseasonal to seasonal scales. Yetthese short-term fire effects on vegetation dynamics and surface energybalance have not been comprehensively investigated in the fire-coupledvegetation model. This study applies the SSiB4/TRIFFID-Fire (the SimplifiedSimple Biosphere Model coupled with the Top-down Representation of InteractiveFoliage and Flora Including Dynamics with fire) model to studythe short-term fire impact in southern Africa. Specifically, we aim toquantify how large impacts fire exerts on surface energy throughdisturbances on vegetation dynamics, how fire effects evolve during the fireseason and the subsequent rainy season, and howmore »surface-darkening effectsplay a role besides the vegetation change effects. We find fire causes an annual average reduction in grass cover by 4 %–8 %for widespread areas between 5–20∘ S and a tree cover reductionby 1 % at the southern periphery of tropical rainforests. The regionalfire effects accumulate during June–October and peak in November, thebeginning of the rainy season. After the fire season ends, the grass coverquickly returns to unburned conditions, while the tree fraction hardlyrecovers in one rainy season. The vegetation removal by fire has reduced theleaf area index (LAI) and gross primary productivity (GPP) by 3 %–5 % and5 %–7 % annually. The exposure of bare soil enhances surface albedo andtherefore decreases the absorption of shortwave radiation. Annual meansensible heat has dropped by 1.4 W m−2, while the latent heat reductionis small (0.1 W m−2) due to the compensating effects between canopytranspiration and soil evaporation. Surface temperature is increased by asmuch as 0.33 K due to the decrease of sensible heat fluxes, and the warmingwould be enhanced when the surface-darkening effect is incorporated. Ourresults suggest that fire effects in grass-dominant areas diminish within1 year due to the high resilience of grasses after fire. Yet fire effectsin the periphery of tropical forests are irreversible within one growingseason and can cause large-scale deforestation if accumulated for hundredsof years.« less
  5. Convective parameterization is the long-lasting bottleneck of global climate modelling and one of the most difficult problems in atmospheric sciences. Uncertainty in convective parameterization is the leading cause of the widespread climate sensitivity in IPCC global warming projections. This paper reviews the observations and parameterizations of atmospheric convection with emphasis on the cloud structure, bulk effects, and closure assumption. The representative state-of-the-art convection schemes are presented, including the ECMWF convection scheme, the Grell scheme used in NCEP model and WRF model, the Zhang-MacFarlane scheme used in NCAR and DOE models, and parameterizations of shallow moist convection. The observed convection hasmore »self-suppression mechanisms caused by entrainment in convective updrafts, surface cold pool generated by unsaturated convective downdrafts, and warm and dry lower troposphere created by mesoscale downdrafts. The post-convection environment is often characterized by “diamond sounding” suggesting an over-stabilization rather than barely returning to neutral state. Then the pre-convection environment is characterized by slow moistening of lower troposphere triggered by surface moisture convergence and other mechanisms. The over-stabilization and slow moistening make the convection events episodic and decouple the middle/upper troposphere from the boundary layer, making the state-type quasi-equilibrium hypothesis invalid. Right now, unsaturated convective downdrafts and especially mesoscale downdrafts are missing in most convection schemes, while some schemes are using undiluted convective updrafts, all of which favour easily turned-on convection linked to double-ITCZ (inter-tropical convergence zone), overly weak MJO (Madden-Julian Oscillation) and precocious diurnal precipitation maximum. We propose a new strategy for convection scheme development using reanalysis-driven model experiments such as the assimilation runs in weather prediction centres and the decadal prediction runs in climate modelling centres, aided by satellite simulators evaluating key characteristics such as the lifecycle of convective cloud-top distribution and stratiform precipitation fraction.« less