Existing descriptions of bi-directional ammonia (NH ₃ ) land–atmosphere exchange incorporate temperature and moisture controls, and are beginning to be used in regional chemical transport models. However, such models have typically applied simpler emission factors to upscale the main NH ₃ emission terms. While this approach has successfully simulated the main spatial patterns on local to global scales, it fails to address the environment- and climate-dependence of emissions. To handle these issues, we outline the basis for a new modelling paradigm where both NH ₃ emissions and deposition are calculated online according to diurnal, seasonal and spatial differences in meteorology. We show how measurements reveal a strong, but complex pattern of climatic dependence, which is increasingly being characterized using ground-based NH ₃ monitoring and satellite observations, while advances in process-based modelling are illustrated for agricultural and natural sources, including a global application for seabird colonies. A future architecture for NH ₃ emission–deposition modelling is proposed that integrates the spatio-temporal interactions, and provides the necessary foundation to assess the consequences of climate change. Based on available measurements, a first empirical estimate suggests that 5°C warming would increase emissions by 42 per cent (28–67%). Together with increased anthropogenic activity, global NH ₃ emissions may increase from 65 (45–85) Tg N in 2008 to reach 132 (89–179) Tg by 2100.

Significance: Human activities have greatly increased emissions of reactive forms of nitrogen to the atmosphere. This perturbation to the nitrogen cycle has produced large increases of nitrogen deposition to sensitive ecosystems. Over recent decades, attention has focused on wet and dry deposition of nitrate stemming from fossil fuel combustion emissions of nitrogen oxides. Successful decreases in nitrogen oxides emissions in the United States have substantially decreased nitrate deposition. By contrast, emissions of ammonia, an unregulated air pollutant, and resulting deposition of ammonium have grown. Expanded observations demonstrate that deposition of reactive nitrogen in the United States has shifted from a nitrate-dominated to an ammonium-dominated condition. Recognition of this shift is critical to formulating effective future policies to protect ecosystems from excess nitrogen deposition.

Disjunct eddy covariance in conjunction with continuous in‐canopy gradient measurements allowed for the first time to quantify the fine‐scale source and sink distribution of some of the most abundant biogenic (isoprene, monoterpenes, methanol, acetaldehyde, and acetone) and photooxidized (MVK+MAC, acetone, acetaldehyde, acetic, and formic acid) VOCs in an old growth tropical rain forest. Our measurements revealed substantial isoprene emissions (up to 2.50 mg m⁻² h⁻¹) and light‐dependent monoterpene emissions (up to 0.33 mg m⁻² h⁻¹) at the peak of the dry season (April and May 2003). Oxygenated species such as methanol, acetone, and acetaldehyde were typically emitted during daytime with net fluxes up to 0.50, 0.36, and 0.20 mg m⁻² h⁻¹, respectively. When generalized for tropical rain forests, these fluxes would add up to a total emission of 36, 16, 19, 106, and 7.2 Tg/yr for methanol, acetaldehyde, acetone, isoprene, and monoterpenes, respectively. During nighttime we observed strong sinks for oxygenated and nitrogen‐containing compounds such as methanol, acetone, acetaldehyde, MVK+MAC, and acetonitrile with deposition velocities close to the aerodynamic limit. This suggests that the canopy resistance (R_c) is very small and not the rate‐limiting step for the nighttime deposition of many VOCs. Our measured mean dry deposition velocities of methanol, acetone, acetaldehyde, MVK+MAC, and acetonitrile were a factor 10–20 higher than estimated from traditional deposition models. If our measurements are generalized, this could have important implications for the redistribution of VOCs in atmospheric chemistry models. Our observations indicate that the current understanding of reactive carbon exchange can only be seen as a first‐order approximation.

Atmospheric ammonia (NH₃) is the primary atmospheric base and an important precursor for inorganic particulate matter and when deposited NH₃ contributes to surface water eutrophication, soil acidification and decline in species biodiversity. Flux measurements indicate that the air–surface exchange of NH₃ is bidirectional. However, the effects of bidirectional exchange, soil biogeochemistry and human activity are not parameterized in air quality models. The US Environmental Protection Agency's (EPA) Community Multiscale Air-Quality (CMAQ) model with bidirectional NH₃ exchange has been coupled with the United States Department of Agriculture's (USDA) Environmental Policy Integrated Climate (EPIC) agroecosystem model. The coupled CMAQ-EPIC model relies on EPIC fertilization timing, rate and composition while CMAQ models the soil ammonium (NH₄^+) pool by conserving the ammonium mass due to fertilization, evasion, deposition, and nitrification processes. This mechanistically coupled modeling system reduced the biases and error in NH_x (NH₃ + NH₄^+) wet deposition and in ambient aerosol concentrations in an annual 2002 Continental US (CONUS) domain simulation when compared to a 2002 annual simulation of CMAQ without bidirectional exchange. Fertilizer emissions estimated in CMAQ 5.0 with bidirectional exchange exhibits markedly different seasonal dynamics than the US EPA's National Emissions Inventory (NEI), with lower emissions in the spring and fall and higher emissions in July.

Presently only limited sets of tropospheric ammonia (NH₃) measurements in the Earth's atmosphere have been reported from satellite and surface station measurements, despite the well-documented negative impact of NH₃ on the environment and human health. Presented here is a detailed description of the satellite retrieval strategy and analysis for the Tropospheric Emission Spectrometer (TES) using simulations and measurements. These results show that: (i) the level of detectability for a representative boundary layer TES NH₃ mixing ratio value is ~0.4 ppbv, which typically corresponds to a profile that contains a maximum level value of ~1 ppbv; (ii) TES NH₃ retrievals generally provide at most one degree of freedom for signal (DOFS), with peak sensitivity between 700 and 900 mbar; (iii) TES NH₃ retrievals show significant spatial and seasonal variability of NH₃ globally; (iv) initial comparisons of TES observations with GEOS-CHEM estimates show TES values being higher overall. Important differences and similarities between modeled and observed seasonal and spatial trends are noted, with discrepancies indicating areas where the timing and magnitude of modeled NH₃ emissions from agricultural sources, and to lesser extent biomass burning sources, need further study.