Abstract Reactive nitrogen (Nr) gases (NH3, N2O, and NO) emitted from agricultural fields constitute a substantial portion of the Nr flux from land to the atmosphere. Here, we coupled the Flows of Agricultural Nitrogen (FANv3) with a modified version of the Community Land Model (CLM5.1) to produce a model (CLM‐FANv3) that simulates the emissions of NH3, NO, and N2O. CLM‐FANv3 is developed under the strong observational constraints of measurements conducted in mesocosms from a US Corn‐Belt agricultural site where corn is planted subject to different fertilizer amounts and soil types. Combining measurements and models allows us to integrate disparate measurements of the mesocosm to produce more complete insights into the dynamic flow of nitrogen within the soil system. The new nitrogen dynamics in CLM‐FANv3, as constrained by the measurements, are different than CLM5.1 with much‐enhanced nitrification (2.5×), enhanced uptake of nitrate in plants (5×), increased nitrate leaching (an order of magnitude larger), and decreased denitrification (about half) at the mesocosm site. NH3 emissions are comparable to denitrification to N2, a significant term neglected in most Earth System Models. The emission factors for NO and N2O in CLM‐FANv3 (0.8%, 1.9%) are in reasonable agreement with the measured emission factor (1.7%, 1.4%), a substantial improvement over the CLM5.1 coupled with FANv2 model (0.2%, 3.5%). The strong measurement constraints have important implications for simulating expected future changes in Nr emissions. Differences in nitrogen cycling also impact projected amounts of carbon stored in agricultural soils over the long term.

Atmospheric methane is a potent greenhouse gas that is photochemically active. The addition of chlorine to the atmosphere has been proposed to mitigate global warming through methane reduction by increasing its chemical loss. However, the potential environmental impacts of such climate mitigation remain unexplored. We explore the possible effects of increasing reactive chlorine emissions on the methane budget, atmospheric composition and radiative forcing. Due to non-linear chemistry we found that achieving effective methane reduction require a minimum 3-fold increase in chlorine atoms compared to present-day levels. Our highest scenario, 50-fold present-day chlorine levels, led to a reduction of the surface temperature by 0.6°C in the year 2050. Beyond the direct effects on methane and temperature, our results show significant alterations in other climate forcers, particularly a large decrease in tropospheric ozone. This translates into a reduction in radiative forcing of a similar magnitude as of the methane removed. Additionally, the Antarctic stratosphere ozone burden during September and October was reduced by up to 40% with the highest chlorine addition. Consequently, the implementation of such strategies requires careful consideration of various factors, including the quantity and method of chlorine addition, as well as potential environmental impacts on air quality and ocean acidity.

Abstract. The escalating climate crisis requires rapid action to reduce the concentrations of atmospheric greenhouse gases and lower global surface temperatures. Methane will play a critical role in near-term warming due to its high radiative forcing and short atmospheric lifetime. Methane emissions have accelerated in recent years, and there is significant risk and uncertainty associated with the future growth in natural emissions. The largest natural sink of methane occurs through oxidation reactions with atmospheric hydroxyl and chlorine radicals. Enhanced atmospheric oxidation could be a potential approach to remove atmospheric methane. One method proposes the addition of iron salt aerosol (ISA) to the atmosphere, mimicking a natural process proposed to occur when mineral dust mixes with chloride from sea spray to form iron chlorides, which are photolyzed by sunlight to produce chlorine radicals. Under the right conditions, lofting ISA into the atmosphere could potentially reduce atmospheric methane concentrations and lower global surface temperatures. Recognizing that potential atmospheric methane removal must only be considered an additive measure – in addition to, not replacing, crucial anthropogenic greenhouse gas emission reductions and carbon dioxide removal – roadmaps can be a valuable tool to organize and streamline interdisciplinary and multifaceted research to efficiently move towards understanding whether an approach may be viable and socially acceptable or if it is nonviable and further research should be deprioritized. Here we present a 5-year research roadmap to explore whether ISA enhancement of the chlorine radical sink could be a viable and socially acceptable atmospheric methane removal approach.

Keeping global surface temperatures below international climate targets will require substantial measures to control atmospheric CO _2 and CH _4 concentrations. Recent studies have focused on interventions to decrease CH _4 through enhanced atmospheric oxidation. Here for the first time using a set of models, we evaluate the effect of adding iron aerosols to the atmosphere to enhance molecular chlorine production, and thus enhance the atmospheric oxidation of methane and reduce its concentration. Using different iron emission sensitivity scenarios, we examine the potential role and impact of enhanced iron emissions on direct interactions with solar radiation, and on the chemical and radiative response of methane. Our results show that the impact of iron emissions on CH _4 depends sensitively on the location of the iron emissions. In all emission regions there is a threshold in the amount of iron that must be added to remove methane. Below this threshold CH _4 increases. Even once that threshold is reached, the iron-aerosol driven chlorine-enhanced impacts on climate are complex. The radiative forcing of both methane and ozone are decreased in the most efficient regions but the direct effect due to the addition of absorbing iron aerosols tends to warm the planet. Adding any anthropogenic aerosol may also cool the planet due to aerosol cloud interactions, although these are very uncertain, and here we focus on the unique properties of adding iron aerosols. If the added emissions have a similar distribution as current shipping emissions, our study shows that the amount of iron aerosols that must be added before methane decreases is 2.5 times the current shipping emissions of iron aerosols, or 6 Tg Fe yr ^−1 in the most ideal case examined here. Our study suggests that the photoactive fraction of iron aerosols is a key variable controlling the impact of iron additions and poorly understood. More studies of the sensitivity of when, where and how iron aerosols are added should be conducted. Before seriously considering this method, additional impacts on the atmospheric chemistry, climate, environmental impacts and air pollution should be carefully assessed in future studies since they are likely to be important.

The role of manganese (Mn) in ecosystem carbon (C) biogeochemical cycling is gaining increasing attention. While soil Mn is mainly derived from bedrock, atmospheric deposition could be a major source of Mn to surface soils, with implications for soil C cycling. However, quantification of the atmospheric Mn cycle, which comprises emissions from natural (desert dust, sea salts, volcanoes, primary biogenic particles, and wildfires) and anthropogenic sources (e.g., industrialization and land-use change due to agriculture), transport, and deposition, remains uncertain. Here, we use compiled emission data sets for each identified source to model and quantify the atmospheric Mn cycle by combining an atmospheric model and in situ atmospheric concentration measurements. We estimated global emissions of atmospheric Mn in aerosols (<10 mu m in aerodynamic diameter) to be 1,400 Gg Mn year(-1). Approximately 31% of the emissions come from anthropogenic sources. Deposition of the anthropogenic Mn shortened Mn "pseudo" turnover times in 1-m-thick surface soils (ranging from 1,000 to over 10,000,000 years) by 1-2 orders of magnitude in industrialized regions. Such anthropogenic Mn inputs boosted the Mn-to-N ratio of the atmospheric deposition in non-desert dominated regions (between 5 x 10(-5) and 0.02) across industrialized areas, but that was still lower than soil Mn-to-N ratio by 1-3 orders of magnitude. Correlation analysis revealed a negative relationship between Mn deposition and topsoil C density across temperate and (sub)tropical forests, consisting with atmospheric Mn deposition enhancing carbon respiration as seen in in situ biogeochemical studies.

In 2019, the Government of India launched the National Clean Air Program to address the pervasive problem of poor air quality and the adverse effect on public health. Coordinated efforts to prevent agricultural burning of crop residues in Northwestern IGP (Indo-Gangetic Plain) have been implemented, but the practice is rapidly expanding into the populous Eastern IGP states, including Bihar, with uncertain consequences for regional air quality. This research has three objectives: (1) characterize historical rice residue burning trends since 2002 over space and time in Bihar State, (2) project future burning trajectories to 2050 under ‘business as usual’ and alternative scenarios of change, and (3) simulate air quality outcomes under each scenario to describe implications for public health. Six future burning scenarios were defined as maintenance of the ‘status quo’ fire extent, area expansion of burning at ‘business as usual’ rates, and a Northwest IGP analogue, of which both current rice yields and plausible yield intensification were considered for each case. The Community Earth System Model (CESM v2.1.0) was used to characterize the mid-century air quality impacts under each scenario. These analyses suggest that contemporary Bihar State burning levels contribute a small daily average proportion (8.1%) of the fine particle pollution load (i.e. PM _2.5 , particles ⩽2.5 μ m) during the burning months, but up to as much as 62% on the worst of winter days in Bihar’s capital region. With a projected 142% ‘business as usual’ increase in burned area extent anticipated for 2050, Bihar’s capital region may experience the equivalent of 30 PM _2.5 additional exceedance days, according to the WHO standard (24 h; exceedance level: 15 µ g m ^−3 ), due to rice residue burning alone in the October to December period. If historical burning trends intensify and Bihar resembles the Northwest States of Punjab and Haryana by 2050, 46 d would exceed the WHO standard for PM _2.5 in Bihar’s capital region.

Manganese (Mn) is a key cofactor in enzymes responsible for lignin decay (mainly Mn peroxidase), regulating the rate of litter degradation and carbon (C) turnover in temperate and boreal forest biomes.While soil Mn is mainly derived from bedrock, atmospheric Mn could also contribute to soil Mn cycling, especially within the surficial horizon, with implications for soil C cycling. However, quantification of the atmospheric Mn cycle, which comprises emissions from natural (desert dust, sea salts, volcanoes, primary biogenic particles, and wildfires) and anthropogenic sources (e.g. industrialization and land-use change due to agriculture) transport, and deposition into the terrestrial and marine ecosystem, remains uncertain. Here, we use compiled emission datasets for each identified source to model and quantify the atmospheric Mn cycle with observational constraints. We estimated global emissions of atmospheric Mn in aerosols (<10 µm in aerodynamic diameter) to be 1500 Gg Mn yr-1. Approximately 32% of the emissions come from anthropogenic sources. Deposition of the anthropogenic Mn shortened soil Mn “pseudo” turnover times in surficial soils about 1-m depth (ranging from 1,000 to over 10,000,000 years) by 1-2 orders of magnitude in industrialized regions. Such anthropogenic Mn inputs boosted the Mn-to-N ratio of the atmospheric deposition in non-desert dominated regions (between 5×10-5 and 0.02) across industrialized areas, but still lower than soil Mn-to-N ratio by 1-3 orders of magnitude. Correlation analysis revealed a negative relationship between Mn deposition and topsoil C density across temperate and (sub)tropical forests, illuminating the role of Mn deposition in these ecosystems.

Active chlorine in the atmosphere is poorly constrained and so is its role in the oxidation of the potent greenhouse gas methane, causing uncertainty in global methane budgets. We propose a photocatalytic mechanism for chlorine atom production that occurs when Sahara dust mixes with sea spray aerosol. The mechanism is validated by implementation in a global atmospheric model and thereby explaining the episodic, seasonal, and location-dependent 13C depletion in CO in air samples from Barbados [J.E. Mak, G. Kra, T. Sandomenico, P. Bergamaschi, J. Geophys. Res. Atmos.108 (2003)], which remained unexplained for decades. The production of Cl can also explain the anomaly in the CO:ethane ratio found at Cape Verde [K. A. Read et al., J. Geophys. Res. Atmos.114 (2009)], in addition to explaining the observation of elevated HOCl [M. J. Lawler et al., Atmos. Chem. Phys.11, 7617-7628 (2011)]. Our model finds that 3.8 Tg(Cl) y-1 is produced over the North Atlantic, making it the dominant source of chlorine in the region; globally, chlorine production increases by 41%. The shift in the methane sink budget due to the increased role of Cl means that isotope-constrained top-down models fail to allocate 12 Tg y-1 (2% of total methane emissions) to 13C-depleted biological sources such as agriculture and wetlands. Since 2014, an increase in North African dust emissions has increased the 13C isotope of atmospheric CH4, thereby partially masking a much greater decline in this isotope, which has implications for the interpretation of the drivers behind the recent increase of methane in the atmosphere.

The escalating climate crisis requires rapid action to reduce the concentrations of atmospheric greenhouse gases and lower global surface temperatures. Methane will play a critical role in near-term warming due to its high radiative forcing and short atmospheric lifetime. Methane emissions have accelerated in recent years and there is significant risk and uncertainty associated with the future growth in natural emissions. The largest natural sink of methane occurs through oxidation reactions with atmospheric hydroxyl and chlorine radicals. Enhanced atmospheric oxidation could be a potential approach to remove atmospheric methane. One method proposes the addition of iron salt aerosols (ISA) to the atmosphere, mimicking a natural process that is proposed to occur when mineral dust mixes with chloride from sea spray to form iron chlorides, which are photolyzed by sunlight to produce chlorine radicals. Under the right conditions, lofting ISA into the atmosphere could potentially reduce atmospheric methane concentrations and lower global surface temperatures. Recognizing that potential atmospheric methane removal must only be considered as an additive measure-in addition to, not replacing, crucial anthropogenic greenhouse gas emission reductions and carbon dioxide removal-roadmaps can be a valuable tool to organize and streamline interdisciplinary and multifaceted research to efficiently move towards an understanding of whether an approach may be viable and socially acceptable, or if it is nonviable and further research should be deprioritized. Here we present an example of a five-year research roadmap to explore whether ISA enhancement of the chlorine radical sink could be a viable and socially acceptable atmospheric methane removal approach.

Global food loss and waste (FLW) undermines the resilience and sustainability of food systems and is closely tied to the United Nation’s Sustainable Development Goals on climate, resource use and food security. Here we reveal strong yet under-discussed interconnections between FLW and two other Sustainable Development Goals of Human Health and Life on Land via the nitrogen cycle. We find that eliminating global FLW in 2015 would have reduced anthropogenic NH 3 emissions associated with food production by 11.4 Tg (16%), decreased local PM 2.5 concentrations by up to 5 μg m −3 and PM 2.5 -related years of life lost by 1.5 million years, and mitigated nitrogen critical load exceedances in global biodiversity hotspots by up to 19%. Halving FLW in 2030 will reduce years of life lost by 0.5–0.8 million years and nitrogen deposition by 4.7–6.0 Tg N per year (4%) (range for socioeconomic pathways). Complementary to near-term NH 3 mitigation potential via technological measures, our study emphasizes incentivizing FLW reduction efforts from air quality and ecosystem health perspectives.

Atmospheric methane is both a potent greenhouse gas and photochemically active, with approximately equal anthropogenic and natural sources. The addition of chlorine to the atmosphere has been proposed to mitigate global warming through methane reduction by increasing its chemical loss. However, the potential environmental impacts of such climate mitigation remain unexplored. Here, sensitivity studies are conducted to evaluate the possible effects of increasing reactive chlorine emissions on the methane budget, atmospheric composition and radiative forcing. Because of non-linear chemistry, in order to achieve a reduction in methane burden (instead of an increase), the chlorine atom burden needs to be a minimum of three times the estimated present-day burden. If the methane removal target is set to 20%, 45%, or 70% less global methane by 2050 compared to the levels in the Representative Concentration Pathway 8.5 scenario (RCP8.5), our modeling results suggest that additional chlorine fluxes of 630, 1250, and 1880 Tg Cl/year, respectively, are needed. The results show that increasing chlorine emissions also induces significant changes in other important climate forcers. Remarkably, the tropospheric ozone decrease is large enough that the magnitude of radiative forcing decrease is similar to that of methane. Adding 630, 1250, and 1880 Tg Cl/year to the RCP8.5 scenario, chosen to have the most consistent current-day trends of methane, will decrease the surface temperature by 0.2, 0.4, and 0.6 °C by 2050, respectively. The quantity and method in which the chlorine is added, its interactions with climate pathways, and the potential environmental impacts on air quality and ocean acidity, must be carefully considered before any action is taken.

Earth System Models (ESMs) have implemented nitrogen (N) cycles to account for N limitation on terrestrial carbon uptake. However, representing inputs, losses, and recycling of N in ESMs is challenging. Here, we use global rates and ratios of key soil N fluxes, including nitrification, denitrification, mineralization, leaching, immobilization, and plant uptake (both NH4 + and NO3 - ), from the literature to evaluate the N cycles in the land model components of two ESMs. The two land models evaluated here, E3SM Land Model version 1 (ELMv1)-ECA and CLM5.0, originated from a common model but have diverged in their representation of plant-microbe competition for soil N. The models predict similar global rates of gross primary productivity (GPP) but have approximately two-fold to three-fold differences in their underlying global mineralization, immobilization, plant N uptake, nitrification, and denitrification fluxes. Both models dramatically underestimate the immobilization of NO3 - by soil bacteria compared with literature values and predict dominance of plant uptake by a single form of mineral nitrogen (NO3 - for ELM, with regional exceptions, and NH4 + for CLM5.0). CLM5.0 strongly underestimates the global ratio of gross nitrification:gross mineralization and both models are likely to substantially underestimate the ratio of nitrification:denitrification. Few experimental data exist to evaluate this last ratio, in part because nitrification and denitrification are quantified using different techniques and because denitrification fluxes are difficult to measure at all. More observational constraints on soil nitrogen fluxes such as nitrification and denitrification, as well as greater scrutiny of the functional impact of introducing separate NH4 + and NO3 - pools into ESMs, could help to improve confidence in present and future simulations of N limitation on the carbon cycle.

Ammonia (NH3) plays a central role in the chemistry of inorganic secondary aerosols in the atmosphere. The largest emission sector for NH3 is agriculture, where NH3 is volatilized from livestock wastes and fertilized soils. Although the NH3 volatilization from soils is driven by the soil temperature and moisture, many atmospheric chemistry models prescribe the emission using yearly emission inventories and climatological seasonal variations. Here we evaluate an alternative approach where the NH3 emissions from agriculture are simulated interactively using the process model FANv2 (Flow of Agricultural Nitrogen, version 2) coupled to the Community Atmospheric Model with Chemistry (CAM-chem). We run a set of 6-year global simulations using the NH3 emission from FANv2 and three global emission inventories (EDGAR, CEDS and HTAP) and evaluate the model performance using a global set of multi-component (atmospheric NH3 and NH4+, and NH4+ wet deposition) in situ observations. Over East Asia, Europe and North America, the simulations with different emissions perform similarly when compared with the observed geographical patterns. The seasonal distributions of NH3 emissions differ between the inventories, and the comparison to observations suggests that both FANv2 and the inventories would benefit from more realistic timing of fertilizer applications. The largest differences between the simulations occur over data-scarce regions. In Africa, the emissions simulated by FANv2 are 200 %–300 % higher than in the inventories, and the available in situ observations from western and central Africa, as well as NH3 retrievals from the Infrared Atmospheric Sounding Interferometer (IASI) instrument, are consistent with the higher NH3 emissions as simulated by FANv2. Overall, in simulating ammonia and ammonium concentrations over regions with detailed regional emission inventories, the inventories based on these details (HTAP, CEDS) capture the atmospheric concentrations and their seasonal variability the best. However these inventories cannot capture the impact of meteorological variability on the emissions, nor can these inventories couple the emissions to the biogeochemical cycles and their changes with climate drivers. Finally, we show with sensitivity experiments that the simulated time-averaged nitrate concentration in air is sensitive to the temporal resolution of the NH3 emissions. Over the CASTNET monitoring network covering the US, resolving the NH3 emissions hourly instead monthly reduced the positive model bias from approximately 80 % to 60 % of the observed yearly mean nitrate concentration. This suggests that some of the commonly reported overestimation of aerosol nitrate over the US may be related to unresolved temporal variability in the NH3 emissions.

To better understand the role of atmospheric dynamics in modulating surface concentrations of fine particulate matter (PM2.5), we relate the anticyclonic wave activity (AWA) metric and PM2.5 data from the Interagency Monitoring of Protected Visual Environment (IMPROVE) data for the period of 1988–2014 over the US. The observational results are compared with hindcast simulations over the past 2 decades using the National Center for Atmospheric Research–Community Earth System Model (NCAR CESM). We find that PM2.5 is positively correlated (up to R=0.65) with AWA changes close to the observing sites using regression analysis. The composite AWA for high-aerosol days (all daily PM2.5 above the 90th percentile) shows a similarly strong correlation between PM2.5 and AWA. The most prominent correlation occurs in the Midwestern US. Furthermore, the higher quantiles of PM2.5 levels are more sensitive to the changes in AWA. For example, we find that the averaged sensitivity of the 90th-percentile PM2.5 to changes in AWA is approximately 3 times as strong as the sensitivity of 10th-percentile PM2.5 at one site (Arendtsville, Pennsylvania; 39.92∘ N, 77.31∘ W). The higher values of the 90th percentile compared to the 50th percentile in quantile regression slopes are most prominent over the northeastern US. In addition, future changes in US PM2.5 based only on changes in climate are estimated to increase PM2.5 concentrations due to increased AWA in summer over areas where PM2.5 variations are dominated by meteorological changes, especially over the western US. Changes between current and future climates in AWA can explain up to 75 % of PM2.5 variability using a linear regression model. Our analysis indicates that higher PM2.5 concentrations occur when a positive AWA anomaly is prominent, which could be critical for understanding how pollutants respond to changing atmospheric circulation as well as for developing robust pollution projections.

Models of terrestrial system dynamics often include nitrogen (N) cycles to better represent N limitations on terrestrial carbon (C) uptake, but simulating the fate of N in ecosystems has proven challenging. Here, key soil N fluxes and flux ratios from the Community Land Model version 5.0 (CLM5.0) are compared with an extensive set of observations from the Hubbard Brook Forest Long-Term Ecological Research site in New Hampshire. Simulated fluxes include microbial immobilization and plant uptake, which compete with nitrification and denitrification, respectively, for available soil ammonium (NH4 + ) and nitrate (NO3 - ). In its default configuration, CLM5.0 predicts that both plant uptake and immobilization are strongly dominated by NH4 + over NO3 - , and that the model ratio of nitrification:denitrification is ~1:1. In contrast, Hubbard Brook observations suggest that NO3 - plays a more significant role in plant uptake and that nitrification could exceed denitrification by an order of magnitude. Modifications to the standard CLM5.0 at Hubbard Brook indicate that a simultaneous increase in the competitiveness of nitrifying microbes for NH4 + and reduction in the competitiveness of denitrifying bacteria for NO3 - are needed to bring soil N flux ratios into better agreement with observations. Such adjustments, combined with evaluation against observations, may help to improve confidence in present and future simulations of N limitation on the C cycle, although C fluxes, such as gross primary productivity and net primary productivity, are less sensitive to the model modifications than soil N fluxes.

Western North American fires have been increasing in magnitude and severity over the last few decades. The complex coupling of fires with the atmospheric energy budget and meteorology creates short-term feedbacks on regional weather altering the amount of pollution to which Americans are exposed. Using a combination of model simulations and observations, this study shows that the severe fires in the summer of 2017 increased atmospheric aerosol concentrations leading to a cooling of the air at the surface, reductions in sensible heat fluxes, and a lowering of the planetary boundary layer height over land. This combination of lower-boundary layer height and increased aerosol pollution from the fires reduces air quality. We estimate that from start of August to end of October 2017, ∼400 premature deaths occurred within the western US as a result of short-term exposure to elevated PM2.5 from fire smoke. As North America confronts a warming climate with more fires the short-term climate and pollution impacts of increased fire activity should be assessed within policy aimed to minimize impacts of climate change on society.

Despite strong impacts that aerosols have on climate and air quality, significant gaps remain in our knowledge concerning their long‐range transport, especially extreme transport events. With this consideration in mind and by leveraging the “atmospheric river” concept, this work develops an objective global algorithm for detecting aerosol atmospheric rivers (AARs), shows a climatology of AARs, elucidates their contributions to major global aerosol transport pathways, and illustrates how AARs can drive extreme cases of poor air quality conditions. Our methodology separately accounts for dust, carbonaceous (accounting for organic and black carbon separately where appropriate), sea salt, and sulfate aerosols. Findings show there are a number of long‐range regional transport pathways where AARs account for a sizable fraction (40% to >100%) of the total transport in relatively few events (20–40 AAR days/year). This study highlights the role of AARs in establishing source‐receptor relationships that can drive regional air‐quality and extremes.

Ratios of key soil nitrogen fluxes from two terrestrial ecosystem models (TEMs) are compared to observational values in the literature. The fluxes included nitrification, denitrification, mineralization, immobilization and plant uptake, with the latter two fluxes partitioned into NH4+ and NO3-. The two TEMs, ELMv1-ECA and CLM5.0, originated from a common model but have diverged in their handling of plant/microbe competition for soil mineral N. Both models predict unrealistically low assimilation (i.e, immobilization) of NO3- by soil bacteria compared to literature values and unrealistic dominance of plant uptake by a single form of mineral nitrogen (NO3- for ELM, NH4+ for CLM5.0). Global ratios of net mineralization (i.e., gross mineralization – gross immobilization) appear unrealistically high in both models compared to literature values while rates of nitrification/gross mineralization appear unrealistically high (ELM) and low (CLM5.0). The ratio of denitrification/nitrification is likely high in both models (3:1 ELM; 2:1 CLM5.0), but few experimental data exist to evaluate these ratios, in part because nitrification and denitrification are quantified with different techniques and generally are not measured simultaneously. The same is true of plant N uptake and microbial N assimilation. Single grid point experiments with CLM5.0 at the Hubbard Brook long-term ecological research site in New Hampshire indicate that the parameterization of nitrification is a potentially important focus area that can bring soil nitrogen flux ratios into better agreement with observations. The current flux ratios raise questions about the credibility of present and future simulations of mineral N limitation on the carbon cycle.

Local finite-amplitude wave activity (LWA) measures the waviness of the local flow. In this work we relate the anticyclonic part of LWA, AWA (anticyclonic wave activity), to surface ozone in summertime over the US on interannual to decadal timescales. Interannual covariance between AWA diagnosed from the European Centre for Medium-Range Weather Forecast Era-Interim reanalysis and ozone measured at EPA Clean Air Status and Trends Network (CASTNET) stations is analyzed using maximum covariance analysis (MCA). The first two modes in the MCA analysis explain 84 % of the covariance between the AWA and MDA8 (maximum daily 8 h average ozone), explaining 29 % and 14 % of the MDA8 ozone variance, respectively. Over most of the US we find a significant relationship between ozone at most locations and AWA over the analysis domain (24–53∘ N and 130–65∘ W) using a linear regression model. This relationship is diagnosed (i) using reanalysis meteorology and measured ozone from CASTNET, or (ii) using meteorology and ozone simulated by the Community Atmospheric Model version 4 with chemistry (CAM4-chem) within the Community Earth System Model (CESM1). Using the linear regression model we find that meteorological biases in AWA in CAM4-chem, as compared to the reanalysis meteorology, induce ozone changes between −4 and +8 ppb in CAM4-chem. Future changes (ca. 2100) in AWA are diagnosed in different climate change simulations in CAM4-chem, simulations which differ in their initial conditions and in one case differ in their reactive species emissions. All future simulations have enhanced AWA over the US, with the maximum enhancement in the southwest. As diagnosed using the linear regression model, the future change in AWA is predicted to cause a corresponding change in ozone ranging between −6 and 6 ppb. The location of this change depends on subtle features of the change in AWA. In a number of locations this change is consistent with the magnitude and the sign of the overall simulated future ozone change.