Effects of ozone-vegetation coupling on surface ozone air quality via biogeochemical and meteorological feedbacks

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 4-6ĝ€ppbv over Europe, North America and China. Reduced dry deposition velocity following ozone damage contributes to ĝ1/4 40-100ĝ€% 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

Modeling the interinfluence of fertilizer-induced NH3 emission, nitrogen deposition, and aerosol radiative effects using modified CESM2

Global ammonia (NH3) emission is expected to continue to rise due to intensified fertilization for growing food to satisfy the increasing demand worldwide. Previous studies have focused mainly on estimating the land-to-atmosphere NH3 injection but seldom addressed the other side of the bidirectional nitrogen exchange – deposition. Ignoring this significant input source of soil mineral nitrogen may lead to an underestimation of NH3 emissions from natural sources. Here, we used an Earth system model to quantify NH3-induced changes in atmospheric composition and the consequent impacts on the Earth's radiative budget and biosphere as well as the impacts of deposition on NH3 emissions from the land surface. We implemented a new scheme into the Community Land Model version 5 (CLM5) of the Community Earth System Model version 2 (CESM2) to estimate the volatilization of ammonium salt (NH+4) associated with synthetic and manure fertilizers into gaseous NH3. We further parameterized the amount of emitted NH3 captured in the plant canopy to derive a more accurate quantity of NH3 that escapes to the atmosphere. Our modified CLM5 estimated that 14 Tg N yr−1 of global NH3 emission is attributable to fertilizers. Interactively coupling terrestrial NH3 emissions to atmospheric chemistry simulations by the Community Atmospheric Model version 4 with chemistry (CAM4-chem), we found that such emissions favor the formation and deposition of NH aerosol+4, which in turn influences the aerosol radiative effect and enhances soil NH3 volatilization in regions downwind of fertilized croplands. Our fully coupled simulations showed that global-total NH3 emission is enhanced by 3.3 Tg N yr−1 when 30 % more synthetic fertilizer is used compared to the 2000-level fertilization. In synergy with observations and emission inventories, our work provides a useful tool for stakeholders to evaluate the intertwined relations between agricultural trends, fertilizer use, NH3 emission, atmospheric aerosols, and climate so as to derive optimal strategies for securing both food production and environmental sustainability

Improving nitrogen cycling in a land surface model (CLM5) to quantify soil N2O, NO, and NH3 emissions from enhanced rock weathering with croplands

Surficial enhanced rock weathering (ERW) is a land-based carbon dioxide removal (CDR) strategy that involves applying crushed silicate rock (e.g., basalt) to agricultural soils. However, unintended biogeochemical interactions with the nitrogen cycle may arise through ERW increasing soil pH as basalt grains undergo dissolution that may reinforce, counteract, or even offset the climate benefits from carbon sequestration. Increases in soil pH could drive changes in the soil emissions of key non-CO2 greenhouse gases, e.g., nitrous oxide (N2O), and trace gases, e.g., nitric oxide (NO) and ammonia (NH3), that affect air quality and crop and human health. We present the development and implementation of a new improved nitrogen cycling scheme for the Community Land Model v5 (CLM5), the land component of the Community Earth System Model, allowing evaluation of ERW effects on soil gas emissions. We base the new parameterizations on datasets derived from soil pH responses of N2O, NO, and NH3 in ERW field trial and mesocosm experiments with crushed basalt. These new capabilities involve the direct implementation of routines within the CLM5 N cycle framework, along with asynchronous coupling of soil pH changes estimated through an ERW model. We successfully validated simulated “control” (i.e., no ERW) seasonal cycles of soil N2O, NO, and NH3 emissions against a wide range of global emission inventories. We benchmark simulated mitigation of soil N2O fluxes in response to ERW against a subset of data from ERW field trials in the US Corn Belt. Using the new scheme, we provide a specific example of the effect of large-scale ERW deployment with croplands on soil nitrogen fluxes across five key regions with high potential for CDR with ERW (North America, Brazil, Europe, India, and China). Across these regions, ERW implementation led to marked reductions in N2O and NO (both 18 %), with moderate increases in NH3 (2 %). While further developments are still required in our implementations when additional ERW data become available, our improved N cycle scheme within CLM5 has utility for investigating the potential of ERW point-source and regional effects of soil N2O, NO, and NH3 fluxes in response to current and future climates. This framework also provides the basis for assessing the implications of ERW for air quality given the role of NO in tropospheric ozone formation, as well as both NO and NH3 in inorganic aerosol formation

Impacts of ozone air pollution and temperature extremes on crop yields: Spatial variability, adaptation and implications for future food security

Ozone air pollution and climate change pose major threats to global crop production, with ramifications for future food security. Previous studies of ozone and warming impacts on crops typically do not account for the strong ozone-temperature correlation when interpreting crop-ozone or crop-temperature relationships, or the spatial variability of crop-to-ozone sensitivity arising from varietal and environmental differences, leading to potential biases in their estimated crop losses. Here we develop an empirical model, called the partial derivative-linear regression (PDLR) model, to estimate the spatial variations in the sensitivities of wheat, maize and soybean yields to ozone exposures and temperature extremes in the US and Europe using a composite of multidecadal datasets, fully correcting for ozone-temperature covariation. We find generally larger and more spatially varying sensitivities of all three crops to ozone exposures than are implied by experimentally derived concentration-response functions used in most previous studies. Stronger ozone tolerance is found in regions with high ozone levels and high consumptive crop water use, reflecting the existence of spatial adaptation and effect of water constraints. The spatially varying sensitivities to temperature extremes also indicate stronger heat tolerance in crops grown in warmer regions. The spatial adaptation of crops to ozone and temperature we find can serve as a surrogate for future adaptation. Using the PDLR-derived sensitivities and 2000–2050 ozone and temperature projections by the Community Earth System Model, we estimate that future warming and unmitigated ozone pollution can combine to cause an average decline in US wheat, maize and soybean production by 13%, 43% and 28%, respectively, and a smaller decline for European crops. Aggressive ozone regulation is shown to offset such decline to various extents, especially for wheat. Our findings demonstrate the importance of considering ozone regulation as well as ozone and climate change adaptation (e.g., selecting heat- and ozone-tolerant cultivars, irrigation) as possible strategies to enhance future food security in response to imminent environmental threats

Uncertainties in Isoprene Photochemistry and Emissions: Implications for the Oxidative Capacity of Past and Present Atmospheres and for Climate Forcing Agents

Current understanding of the factors controlling biogenic isoprene emissions and of the fate of isoprene oxidation products in the atmosphere has been evolving rapidly. We use a climate-biosphere-chemistry modeling framework to evaluate the sensitivity of estimates of the tropospheric oxidative capacity to uncertainties in isoprene emissions and photochemistry. Our work focuses on trends across two time horizons: from the Last Glacial Maximum (LGM, 21 000 years BP) to the preindustrial (1770s); and from the preindustrial to the present day (1990s). We find that different oxidants have different sensitivities to the uncertainties tested in this study, with OH being the most sensitive: changes in the global mean OH levels for the LGM-to-preindustrial transition range between -29 and +7, and those for the preindustrial-to-present day transition range between -8 and +17, across our simulations. Our results suggest that the observed glacial-interglacial variability in atmospheric methane concentrations is predominantly driven by changes in methane sources as opposed to changes in OH, the primary methane sink. However, the magnitudes of change are subject to uncertainties in the past isoprene global burdens, as are estimates of the change in the global burden of secondary organic aerosol (SOA) relative to the preindustrial. We show that the linear relationship between tropospheric mean OH and tropospheric mean ozone photolysis rates, water vapor, and total emissions of NOx and reactive carbon first reported in Murray et al. (2014) does not hold across all periods with the new isoprene photochemistry mechanism. Our results demonstrate that inadequacies in our understanding of present-day OH and its controlling factors must be addressed in order to improve model estimates of the oxidative capacity of past and present atmospheres