Atmospheric deposition of inorganic nitrogen is critical to the function of ecosystems and elemental cycles. During the industrial period, humans have doubled the amount of inorganic nitrogen in the biosphere and radically altered rates of atmospheric nitrogen deposition. Despite this rapid change, estimates of global nitrogen deposition patterns generally have low, centennial‐scale temporal resolution. Lack of information on annual‐ to decadal‐scale changes in global nitrogen deposition makes it difficult for scientists researching questions on these finer timescales to contextualize their work within the global nitrogen cycle. Here we use the GEOS‐Chem Chemical Transport Model to estimate wet and dry deposition of inorganic nitrogen globally at a spatial resolution of 2° × 2.5° for 12 individual years in the period from 1984 to 2016. During this time, we found an 8% increase in global inorganic nitrogen deposition from 86.6 to 93.6 TgN/year, a trend that comprised a balance of variable regional patterns. For example, inorganic nitrogen deposition increased in areas including East Asia and Southern Brazil, while inorganic nitrogen deposition declined in areas including Europe. Further, we found a global increase in the percentage of inorganic nitrogen deposited in chemically reduced forms from 30% to 35%, and this trend was largely driven by strong regional increases in the proportion of chemically reduced nitrogen deposited over the United States. This study provides spatially explicit estimates of inorganic nitrogen deposition over the last four decades and improves our understanding of short‐term human impacts on the global nitrogen cycle.

Peroxyacetyl nitrate (PAN) formed in the atmospheric oxidation of non-methane volatile organic compounds (NMVOCs) is the principal tropospheric reservoir for nitrogen oxide radicals (NO_x = NO + NO₂). PAN enables the transport and release of NO_x to the remote troposphere with major implications for the global distributions of ozone and OH, the main tropospheric oxidants. Simulation of PAN is a challenge for global models because of the dependence of PAN on vertical transport as well as complex and uncertain NMVOC sources and chemistry. Here we use an improved representation of NMVOCs in a global 3-D chemical transport model (GEOS-Chem) and show that it can simulate PAN observations from aircraft campaigns worldwide. The immediate carbonyl precursors for PAN formation include acetaldehyde (44% of the global source), methylglyoxal (30%), acetone (7%), and a suite of other isoprene and terpene oxidation products (19%). A diversity of NMVOC emissions is responsible for PAN formation globally including isoprene (37%) and alkanes (14%). Anthropogenic sources are dominant in the extratropical Northern Hemisphere outside the growing season. Open fires appear to play little role except at high northern latitudes in spring, although results are very sensitive to plume chemistry and plume rise. Lightning NO_x is the dominant contributor to the observed PAN maximum in the free troposphere over the South Atlantic.

We construct a global atmospheric budget for acetaldehyde using a 3-D model of atmospheric chemistry (GEOS-Chem), and use an ensemble of observations to evaluate present understanding of its sources and sinks. Hydrocarbon oxidation provides the largest acetaldehyde source in the model (128 Tg a⁻¹, a factor of 4 greater than the previous estimate), with alkanes, alkenes, and ethanol the main precursors. There is also a minor source from isoprene oxidation. We use an updated chemical mechanism for GEOS-Chem, and photochemical acetaldehyde yields are consistent with the Master Chemical Mechanism. We present a new approach to quantifying the acetaldehyde air-sea flux based on the global distribution of light absorption due to colored dissolved organic matter (CDOM) derived from satellite ocean color observations. The resulting net ocean emission is 57 Tg a⁻¹, the second largest global source of acetaldehyde. A key uncertainty is the acetaldehyde turnover time in the ocean mixed layer, with quantitative model evaluation over the ocean complicated by known measurement artifacts in clean air. Simulated concentrations in surface air over the ocean generally agree well with aircraft measurements, though the model tends to overestimate the vertical gradient. PAN:NO_x ratios are well-simulated in the marine boundary layer, providing some support for the modeled ocean source. We introduce the Model of Emissions of Gases and Aerosols from Nature (MEGANv2.1) for acetaldehyde and ethanol and use it to quantify their net flux from living terrestrial plants. Including emissions from decaying plants the total direct acetaldehyde source from the land biosphere is 23 Tg a⁻¹. Other terrestrial acetaldehyde sources include biomass burning (3 Tg a⁻¹) and anthropogenic emissions (2 Tg a⁻¹). Simulated concentrations in the continental boundary layer are generally unbiased and capture the spatial gradients seen in observations over North America, Europe, and tropical South America. However, the model underestimates acetaldehyde levels in urban outflow, suggesting a missing source in polluted air. Ubiquitous high measured concentrations in the free troposphere are not captured by the model, and based on present understanding are not consistent with concurrent measurements of PAN and NO_x: we find no compelling evidence for a widespread missing acetaldehyde source in the free troposphere. We estimate the current US source of ethanol and acetaldehyde (primary + secondary) at 1.3 Tg a⁻¹ and 7.8 Tg a⁻¹, approximately 60{%} and 480% of the corresponding increases expected for a national transition from gasoline to ethanol fuel.

Nitrous oxide (N₂O) is a long-lived potent greenhouse gas and stratospheric ozone-depleting substance that has been accumulating in the atmosphere since the preindustrial period. The mole fraction of atmospheric N₂O has increased by nearly 25 % from 270 ppb (parts per billion) in 1750 to 336 ppb in 2022, with the fastest annual growth rate since 1980 of more than 1.3 ppb yr⁻¹ in both 2020 and 2021. According to the Sixth Assessment Report of the Intergovernmental Panel on Climate Change (IPCC AR6), the relative contribution of N₂O to the total enhanced effective radiative forcing of greenhouse gases was 6.4 % for 1750–2022. As a core component of our global greenhouse gas assessments coordinated by the Global Carbon Project (GCP), our global N₂O budget incorporates both natural and anthropogenic sources and sinks and accounts for the interactions between nitrogen additions and the biogeochemical processes that control N₂O emissions. We use bottom-up (BU: inventory, statistical extrapolation of flux measurements, and process-based land and ocean modeling) and top-down (TD: atmospheric measurement-based inversion) approaches. We provide a comprehensive quantification of global N₂O sources and sinks in 21 natural and anthropogenic categories in 18 regions between 1980 and 2020. We estimate that total annual anthropogenic N₂O emissions have increased 40 % (or 1.9 Tg N yr⁻¹) in the past 4 decades (1980–2020). Direct agricultural emissions in 2020 (3.9 Tg N yr⁻¹, best estimate) represent the large majority of anthropogenic emissions, followed by other direct anthropogenic sources, including fossil fuel and industry, waste and wastewater, and biomass burning (2.1 Tg N yr⁻¹), and indirect anthropogenic sources (1.3 Tg N yr⁻¹) . For the year 2020, our best estimate of total BU emissions for natural and anthropogenic sources was 18.5 (lower–upper bounds: 10.6–27.0) Tg N yr⁻¹, close to our TD estimate of 17.0 (16.6–17.4) Tg N yr⁻¹. For the 2010–2019 period, the annual BU decadal-average emissions for both natural and anthropogenic sources were 18.2 (10.6–25.9) Tg N yr⁻¹ and TD emissions were 17.4 (15.8–19.20) Tg N yr⁻¹. The once top emitter Europe has reduced its emissions by 31 % since the 1980s, while those of emerging economies have grown, making China the top emitter since the 2010s. The observed atmospheric N₂O concentrations in recent years have exceeded projected levels under all scenarios in the Coupled Model Intercomparison Project Phase 6 (CMIP6), underscoring the importance of reducing anthropogenic N₂O emissions. To evaluate mitigation efforts and contribute to the Global Stocktake of the United Nations Framework Convention on Climate Change, we propose the establishment of a global network for monitoring and modeling N₂O from the surface through to the stratosphere. The data presented in this work can be downloaded from https://doi.org/10.18160/RQ8P-2Z4R (Tian et al., 2023).

Space‐borne formaldehyde (HCHO) column measurements from the Ozone Monitoring Instrument (OMI), with 13 × 24 km² nadir footprint and daily global coverage, provide new constraints on the spatial distribution of biogenic isoprene emission from North America. OMI HCHO columns for June‐August 2006 are consistent with measurements from the earlier GOME satellite sensor (1996–2001) but OMI is 2–14% lower. The spatial distribution of OMI HCHO columns follows that of isoprene emission; anthropogenic hydrocarbon emissions are undetectable except in Houston. We develop updated relationships between HCHO columns and isoprene emission from a chemical transport model (GEOS‐Chem), and use these to infer top‐down constraints on isoprene emissions from the OMI data. We compare the OMI‐derived emissions to a state‐of‐science bottom‐up isoprene emission inventory (MEGAN) driven by two land cover databases, and use the results to optimize the MEGAN emission factors (EFs) for broadleaf trees (the main isoprene source). The OMI‐derived isoprene emissions in North America (June–August 2006) with 1° × 1° resolution are spatially consistent with MEGAN (R² = 0.48–0.68) but are lower (by 4–25% on average). MEGAN overestimates emissions in the Ozarks and the Upper South. A better fit to OMI (R² = 0.73) is obtained in MEGAN by using a uniform isoprene EF from broadleaf trees rather than variable EFs. Thus MEGAN may overestimate emissions in areas where it specifies particularly high EFs. Within‐canopy isoprene oxidation may also lead to significant differences between the effective isoprene emission to the atmosphere seen by OMI and the actual isoprene emission determined by MEGAN.