ALBERT

Description: Many studies have shown that global land cover change can significantly affect surface ozone air quality, albeit still with great uncertainties due to the complex pathways involved. In this study, we develop a framework to systematically examine the effects of any changes in foliage density as represented by leaf area index (LAI) on surface ozone concentration. We perform a series of perturbation experiments using the GEOS‐Chem chemical transport model. The spatial variability of the simulated results is used as a proxy to build a statistical model to quantify the sensitivity of surface ozone to LAI changes, which is found to arise mostly from the associated changes in dry deposition velocity and isoprene emission rate, whereas other factors and second‐order effects are negligible. The spatial variations of ozone responses to LAI changes are found to be the most correlated with anthropogenic NOx emission, biogenic isoprene emission, wind speed, ozone concentration, baseline LAI, and changes in LAI. We also show that the sign of change in surface ozone under future LAI changes for a given location can be inferred by distinguishing between three different regimes based on local anthropogenic NOx emission and LAI. The statistical model is optimized so that it is applicable to a wide range of LAI changes and can be used as a quick assessment tool to estimate the impacts of various land use policies on ozone air quality, and a diagnostic tool to estimate the relative contribution of different pathways toward the overall ozone‐LAI relationship.

Description: Surface ozone (O3) is an important air pollutant and greenhouse gas. Land use and land cover is one of the critical factors influencing ozone, in addition to anthropogenic emissions and climate. Land use and land cover change (LULCC) can on the one hand affect ozone “biogeochemically”, i.e., via dry deposition and biogenic emissions of volatile organic compounds (VOCs). LULCC can on the other hand alter regional- to large-scale climate through modifying albedo and evapotranspiration, which can lead to changes in surface temperature, hydrometeorology, and atmospheric circulation that can ultimately impact ozone “biogeophysically”. Such biogeophysical effects of LULCC on ozone are largely understudied. This study investigates the individual and combined biogeophysical and biogeochemical effects of LULCC on ozone and explicitly examines the critical pathway for how LULCC impacts ozone pollution. A global coupled atmosphere–chemistry–land model is driven by projected LULCC from the present day (2000) to the future (2050) under RCP4.5 and RCP8.5 scenarios, focusing on the boreal summer. Results reveal that when considering biogeochemical effects only, surface ozone is predicted to have slight changes by up to 2 ppbv maximum in some areas due to LULCC. It is primarily driven by changes in isoprene emission and dry deposition counteracting each other in shaping ozone. In contrast, when considering the combined effect of LULCC, ozone is more substantially altered by up to 5 ppbv over several regions in North America and Europe under RCP4.5, reflecting the importance of biogeophysical effects on ozone changes. In boreal and temperate mixed forests with intensive reforestation, enhanced net radiation and sensible heat induce a cascade of hydrometeorological feedbacks that generate warmer and drier conditions favorable for higher ozone levels. In contrast, reforestation in subtropical broadleaf forests has minimal impacts on boundary-layer meteorology and ozone air quality. Furthermore, significant ozone changes are also found in regions with only modest LULCC, which can only be explained by “remote” biogeophysical effects. A likely mechanism is that reforestation induces a circulation response, leading to reduced moisture transport and ultimately warmer and drier conditions in the surrounding regions with limited LULCC. We conclude that the biogeophysical effects of LULCC are important pathways through which LULCC influences ozone air quality both locally and in remote regions even without significant LULCC. Overlooking the effects of hydrometeorological changes on ozone air quality may cause underestimation of the impacts of LULCC on ozone pollution.

Description: Tropospheric ozone is an air pollutant that substantially harms vegetation and is also strongly dependent on various vegetation-mediated processes. The interdependence between ozone and vegetation may constitute feedback mechanisms that can alter ozone concentration itself but have not been considered in most studies to date. In this study we examine the importance of dynamic coupling between surface ozone and leaf area index (LAI) in shaping ozone air quality and vegetation. We first implement an empirical scheme for ozone damage on vegetation in the Community Land Model (CLM) and simulate the steady-state responses of LAI to long-term exposure to a range of prescribed ozone levels (from 0 to 100 ppb). We find that most plant functional types suffer a substantial decline in LAI as ozone level increases. Based on the CLM-simulated results, we develop and implement in the GEOS-Chem chemical transport model a parameterization that computes fractional changes in monthly LAI as a function of local mean ozone levels. By forcing LAI to respond to ozone concentrations on a monthly timescale, the model simulates ozone–LAI coupling dynamically via biogeochemical processes including biogenic volatile organic compound (VOC) emissions and dry deposition, without the complication from meteorological changes. We find that ozone-induced damage on LAI can lead to changes in ozone concentrations by −1.8 to +3 ppb in boreal summer, with a corresponding ozone feedback factor of −0.1 to +0.6 that represents an overall self-amplifying effect from ozone–LAI coupling. Substantially higher simulated ozone due to strong positive feedbacks is found in most tropical forests, mainly due to the ozone-induced reductions in LAI and dry deposition velocity, whereas reduced isoprene emission plays a lesser role in these low-NOx environments. In high-NOx regions such as the eastern US, Europe, and China, however, the feedback effect is much weaker and even negative in some regions, reflecting the compensating effects of reduced dry deposition and reduced isoprene emission (which reduces ozone in high-NOx environments). In remote, low-LAI regions, including most of the Southern Hemisphere, the ozone feedback is generally slightly negative due to the reduced transport of NOx–VOC reaction products that serve as NOx reservoirs. This study represents the first step to accounting for dynamic ozone–vegetation coupling in a chemical transport model with ramifications for a more realistic joint assessment of ozone air quality and ecosystem health.

Description: In his study, we use a combination of multivariate statistical methods to understand the relationships of PM2.5 with local meteorology and synoptic weather patterns in different regions of China across various timescales. Using June 2014 to May 2017 daily total PM2.5 observations from ∼ 1500 monitors, all deseasonalized and detrended to focus on synoptic-scale variations, we find strong correlations of daily PM2.5 with all selected meteorological variables (e.g., positive correlation with temperature but negative correlation with sea-level pressure throughout China; positive and negative correlation with relative humidity in northern and southern China, respectively). The spatial patterns suggest that the apparent correlations with individual meteorological variables may arise from common association with synoptic systems. Based on a principal component analysis of 1998–2017 meteorological data to diagnose distinct meteorological modes that dominate synoptic weather in four major regions of China, we find strong correlations of PM2.5 with several synoptic modes that explain 10 to 40 % of daily PM2.5 variability. These modes include monsoonal flows and cold frontal passages in northern and central China associated with the Siberian High, onshore flows in eastern China, and frontal rainstorms in southern China. Using the Beijing–Tianjin–Hebei (BTH) region as a case study, we further find strong interannual correlations of regionally averaged satellite-derived annual mean PM2.5 with annual mean relative humidity (RH; positive) and springtime fluctuation frequency of the Siberian High (negative). We apply the resulting PM2.5-to-climate sensitivities to the Intergovernmental Panel on Climate Change (IPCC) Coupled Model Intercomparison Project Phase 5 (CMIP5) climate projections to predict future PM2.5 by the 2050s due to climate change, and find a modest decrease of ∼ 0.5 µg m−3 in annual mean PM2.5 in the BTH region due to more frequent cold frontal ventilation under the RCP8.5 future, representing a small “climate benefit”, but the RH-induced PM2.5 change is inconclusive due to the large inter-model differences in RH projections.

Description: Tropospheric ozone is one of the most hazardous air pollutants as it harms both human health and plant productivity. Foliage uptake of ozone via dry deposition damages photosynthesis and causes stomatal closure. These foliage changes could lead to a cascade of biogeochemical and biogeophysical effects that not only modulate the carbon cycle, regional hydrometeorology and climate, but also cause feedbacks onto surface ozone concentration itself. In this study, we implement a semi-empirical parameterization of ozone damage on vegetation in the Community Earth System Model to enable online ozone–vegetation coupling, so that for the first time ecosystem structure and ozone concentration can coevolve in fully coupled land–atmosphere simulations. With ozone–vegetation coupling, present-day surface ozone is simulated to be higher by up to 4–6 ppbv over Europe, North America and China. Reduced dry deposition velocity following ozone damage contributes to ∼ 40–100 % of those increases, constituting a significant positive biogeochemical feedback on ozone air quality. Enhanced biogenic isoprene emission is found to contribute to most of the remaining increases, and is driven mainly by higher vegetation temperature that results from lower transpiration rate. This isoprene-driven pathway represents an indirect, positive meteorological feedback. The reduction in both dry deposition and transpiration is mostly associated with reduced stomatal conductance following ozone damage, whereas the modification of photosynthesis and further changes in ecosystem productivity are found to play a smaller role in contributing to the ozone–vegetation feedbacks. Our results highlight the need to consider two-way ozone–vegetation coupling in Earth system models to derive a more complete understanding and yield more reliable future predictions of ozone air quality.

Description: Human activities have substantially increased atmospheric deposition of reactive nitrogen to the Earth's surface, inducing unintentional effects on ecosystems with complex environmental and climate consequences. One consequence remaining unexplored is how surface air quality might respond to the enhanced nitrogen deposition through surface–atmosphere exchange. Here we combine a chemical transport model (GEOS-Chem) and a global land model (Community Land Model, CLM) to address this issue with a focus on ozone pollution in the Northern Hemisphere. We consider three processes that are important for surface ozone and can be perturbed by the addition of atmospheric deposited nitrogen – namely, emissions of biogenic volatile organic compounds (VOCs), ozone dry deposition, and soil nitrogen oxide (NOx) emissions. We find that present-day anthropogenic nitrogen deposition (65 Tg N a−1 to the land), through enhancing plant growth (represented as increases in vegetation leaf area index, LAI, in the model), could increase surface ozone from increased biogenic VOC emissions (e.g., a 6.6 Tg increase in isoprene emission), but it could also decrease ozone due to higher ozone dry deposition velocities (up to 0.02–0.04 cm s−1 increases). Meanwhile, deposited anthropogenic nitrogen to soil enhances soil NOx emissions. The overall effect on summer mean surface ozone concentrations shows general increases over the globe (up to 1.5–2.3 ppbv over the western US and South Asia), except for some regions with high anthropogenic NOx emissions (0.5–1.0 ppbv decreases over the eastern US, western Europe, and North China). We compare the surface ozone changes with those driven by the past 20-year climate and historical land use changes. We find that the impacts from anthropogenic nitrogen deposition can be comparable to the climate- and land-use-driven surface ozone changes at regional scales and partly offset the surface ozone reductions due to land use changes reported in previous studies. Our study emphasizes the complexity of biosphere–atmosphere interactions, which can have important implications for future air quality prediction.

Description: Dry deposition is a major sink of tropospheric ozone. Increasing evidence has shown that ozone dry deposition actively links meteorology and hydrology with ozone air quality. However, there is little systematic investigation on the performance of different ozone dry deposition parameterizations at the global scale and how parameterization choice can impact surface ozone simulations. Here, we present the results of the first global, multidecadal modelling and evaluation of ozone dry deposition velocity (vd) using multiple ozone dry deposition parameterizations. We model ozone dry deposition velocities over 1982–2011 using four ozone dry deposition parameterizations that are representative of current approaches in global ozone dry deposition modelling. We use consistent assimilated meteorology, land cover, and satellite-derived leaf area index (LAI) across all four, such that the differences in simulated vd are entirely due to differences in deposition model structures or assumptions about how land types are treated in each. In addition, we use the surface ozone sensitivity to vd predicted by a chemical transport model to estimate the impact of mean and variability of ozone dry deposition velocity on surface ozone. Our estimated vd values from four different parameterizations are evaluated against field observations, and while performance varies considerably by land cover types, our results suggest that none of the parameterizations are universally better than the others. Discrepancy in simulated mean vd among the parameterizations is estimated to cause 2 to 5 ppbv of discrepancy in surface ozone in the Northern Hemisphere (NH) and up to 8 ppbv in tropical rainforests in July, and up to 8 ppbv in tropical rainforests and seasonally dry tropical forests in Indochina in December. Parameterization-specific biases based on individual land cover type and hydroclimate are found to be the two main drivers of such discrepancies. We find statistically significant trends in the multiannual time series of simulated July daytime vd in all parameterizations, driven by warming and drying (southern Amazonia, southern African savannah, and Mongolia) or greening (high latitudes). The trend in July daytime vd is estimated to be 1 % yr−1 and leads to up to 3 ppbv of surface ozone changes over 1982–2011. The interannual coefficient of variation (CV) of July daytime mean vd in NH is found to be 5 %–15 %, with spatial distribution that varies with the dry deposition parameterization. Our sensitivity simulations suggest this can contribute between 0.5 to 2 ppbv to interannual variability (IAV) in surface ozone, but all models tend to underestimate interannual CV when compared to long-term ozone flux observations. We also find that IAV in some dry deposition parameterizations is more sensitive to LAI, while in others it is more sensitive to climate. Comparisons with other published estimates of the IAV of background ozone confirm that ozone dry deposition can be an important part of natural surface ozone variability. Our results demonstrate the importance of ozone dry deposition parameterization choice on surface ozone modelling and the impact of IAV of vd on surface ozone, thus making a strong case for further measurement, evaluation, and model–data integration of ozone dry deposition on different spatiotemporal scales.