scholarly journals The climate impact of ship NO<sub>x</sub> emissions: an improved estimate accounting for plume chemistry

2014 ◽  
Vol 14 (3) ◽  
pp. 3427-3458
Author(s):  
C. D. Holmes ◽  
M. J. Prather ◽  
G. C. M. Vinken
Keyword(s):  
Radiative Forcing ◽  
Transport Model ◽  
Parametric Representation ◽  
Climate Impact ◽  
Nox Emissions ◽  
Chemical Transport Model ◽  
Rf Components ◽  
Maritime Shipping ◽  
Sensitivity Tests ◽  
Emission Changes

Abstract. Nitrogen oxide (NOx) emissions from maritime shipping produce ozone (O3) and hydroxyl radicals (OH), which in turn destroy methane (CH4). The balance between this warming (due to O3) and cooling (due to CH4) determines the net effect of ship NOx on climate. Previous estimates of the chemical impact and radiative forcing (RF) of ship NOx have generally assumed that plumes of ship exhaust are instantly diluted into model grid cells spanning hundreds of kilometers, even though this is known to produce biased results. Here we improve the parametric representation of exhaust-gas chemistry developed in the GEOS-Chem chemical transport model (CTM) to provide the first estimate of RF from shipping that accounts for sub-grid-scale ship plume chemistry. The CTM now calculates O3 production and CH4 loss both within and outside the exhaust plumes and also accounts for the effect of wind speed. With the improved modeling of plumes, ship NOx perturbations are smaller than suggested by the ensemble of past global modeling studies, but if we assume instant dilution of ship NOx on the grid scale, the CTM reproduces previous model results. Our best estimates of the RF components from increasing ship NOx emissions by 1 Tg(N) yr−1 are smaller than given in the past literature: +3.4 ± 0.85 mW m−2 from the short-lived ozone increase, −5.0 ± 1.1 mW m−2 from the CH4 decrease, and −1.7 ± 0.7 mW m−2 from the long-lived O3 decrease that accompanies the CH4 change. The resulting net RF is −3.3 ± 1.8 mW m−2 for emissions of 1 Tg(N) yr−1. Due to non-linearity in O3 production as a function of background NOx, RF from large changes in ship NOx emissions, such as the increase since preindustrial times, is about 20% larger than this RF value for small marginal emission changes. Using sensitivity tests in one CTM, we quantify sources of uncertainty in the RF components and causes of the ±30% spread in past model results. The main source of uncertainty is the composition of the background atmosphere in the CTM, which is driven by model formulation (±10 to 20%) and the plausible range of anthropogenic emissions (±10%).

scholarly journals The climate impact of ship NO<sub>x</sub> emissions: an improved estimate accounting for plume chemistry

2014 ◽  
Vol 14 (13) ◽  
pp. 6801-6812 ◽  
Author(s):  
C. D. Holmes ◽  
M. J. Prather ◽  
G. C. M. Vinken
Keyword(s):  
Radiative Forcing ◽  
Transport Model ◽  
Parametric Representation ◽  
Climate Impact ◽  
Nox Emissions ◽  
Chemical Transport Model ◽  
Rf Components ◽  
Maritime Shipping ◽  
Sensitivity Tests ◽  
Emission Changes

Abstract. Nitrogen oxide (NOx) emissions from maritime shipping produce ozone (O3) and hydroxyl radicals (OH), which in turn destroy methane (CH4). The balance between this warming (due to O3) and cooling (due to CH4) determines the net effect of ship NOx on climate. Previous estimates of the chemical impact and radiative forcing (RF) of ship NOx have generally assumed that plumes of ship exhaust are instantly diluted into model grid cells spanning hundreds of kilometers, even though this is known to produce biased results. Here we improve the parametric representation of exhaust-gas chemistry developed in the GEOS-Chem chemical transport model (CTM) to provide the first estimate of RF from shipping that accounts for sub-grid-scale ship plume chemistry. The CTM now calculates O3 production and CH4 loss both within and outside the exhaust plumes and also accounts for the effect of wind speed. With the improved modeling of plumes, ship NOx perturbations are smaller than suggested by the ensemble of past global modeling studies, but if we assume instant dilution of ship NOx on the grid scale, the CTM reproduces previous model results. Our best estimates of the RF components from increasing ship NOx emissions by 1 Tg(N) yr−1 are smaller than that given in the past literature: + 3.4 ± 0.85 mW m−2 (1σ confidence interval) from the short-lived ozone increase, −5.7 ± 1.3 mW m−2 from the CH4 decrease, and −1.7 ± 0.7 mW m−2 from the long-lived O3 decrease that accompanies the CH4 change. The resulting net RF is −4.0 ± 2.0 mW m−2 for emissions of 1 Tg(N) yr−1. Due to non-linearity in O3 production as a function of background NOx, RF from large changes in ship NOx emissions, such as the increase since preindustrial times, is about 20% larger than this RF value for small marginal emission changes. Using sensitivity tests in one CTM, we quantify sources of uncertainty in the RF components and causes of the ±30% spread in past model results; the main source of uncertainty is the composition of the background atmosphere in the CTM, which is driven by model formulation (±10 to 20%) and the plausible range of anthropogenic emissions (±10%).

scholarly journals Sulfate-nitrate-ammonium aerosols over China: response to 2000–2015 emission changes of sulfur dioxide, nitrogen oxides, and ammonia

2013 ◽  
Vol 13 (5) ◽  
pp. 2635-2652 ◽  
Author(s):  
Y. Wang ◽  
Q. Q. Zhang ◽  
K. He ◽  
Q. Zhang ◽  
L. Chai
Keyword(s):  
Emission Reduction ◽  
Transport Model ◽  
Critical Role ◽  
Sufficient Information ◽  
Nox Emissions ◽  
Chemical Transport Model ◽  
Dominant Component ◽  
Emission Changes ◽  
Emission Reduction Target

Abstract. We use a chemical transport model to examine the change of sulfate-nitrate-ammonium (SNA) aerosols over China due to anthropogenic emission changes of their precursors (SO2, NOx and NH3) from 2000 to 2015. From 2000 to 2006, annual mean SNA concentrations increased by about 60% over China as a result of the 60% and 80% increases in SO2 and NOx emissions. During this period, sulfate is the dominant component of SNA over South China (SC) and Sichuan Basin (SCB), while nitrate and sulfate contribute equally over North China (NC). Based on emission reduction targets in the 12th (2011–2015) Five-Year Plan (FYP), China's total SO2 and NOx emissions are projected to change by −16% and +16% from 2006 to 2015, respectively. The amount of NH3 emissions in 2015 is uncertain, given the lack of sufficient information on the past and present levels of NH3 emissions in China. With no change in NH3 emissions, SNA mass concentrations in 2015 will decrease over SCB and SC compared to their 2006 levels, but increase over NC where the magnitude of nitrate increase exceeds that of sulfate reduction. This suggests that the SO2 emission reduction target set by the 12th FYP, although effective in reducing SNA over SC and SCB, will not be successful over NC, for which NOx emission control needs to be strengthened. If NH3 emissions are allowed to keep their recent growth rate and increase by +16% from 2006 to 2015, the benefit of SO2 reduction will be completely offset over all of China due to the significant increase of nitrate, demonstrating the critical role of NH3 in regulating nitrate. The effective strategy to control SNA and hence PM2.5 pollution over China should thus be based on improving understanding of current NH3 emissions and putting more emphasis on controlling NH3 emissions in the future.

scholarly journals Sulfate-nitrate-ammonium aerosols over China: response to 2000–2015 emission changes of sulfur dioxide, nitrogen oxides, and ammonia

2012 ◽  
Vol 12 (9) ◽  
pp. 24243-24285 ◽  
Author(s):  
Y. Wang ◽  
Q. Q. Zhang ◽  
K. He ◽  
Q. Zhang ◽  
L. Chai
Keyword(s):  
Emission Reduction ◽  
Transport Model ◽  
Critical Role ◽  
Nox Emissions ◽  
Chemical Transport Model ◽  
So2 Emission ◽  
Dominant Component ◽  
Emission Changes ◽  
Emission Reduction Target

Abstract. We use a chemical transport model to examine the change of sulfate-nitrate-ammonium (SNA) aerosols over China due to anthropogenic emission changes of their precursors (SO2, NOx and NH3) from 2000 to 2015. From 2000 to 2006, annual mean SNA concentrations increased by about 60% over China as a result of the 60%~80% increases in SO2 and NOx emissions. During this period, sulfate is the dominant component of SNA over South China (SC) and Sichuan Basin (SCB), while nitrate makes equal contribution as sulfate over North China (NC). Based on emission reduction targets in the 12th (2011–2015) Five Year Plan (FYP), China's total SO2 and NOx emissions are projected to change by −16% and +16% from 2006 to 2015, respectively. However, the amount of NH3 emissions in 2015 is uncertain, given our finding that bottom-up inventories tend to overestimate China's ammonia emissions during the 2000–2006 period. With no change in NH3 emissions, SNA mass concentrations in 2015 will decrease over SCB and SC compared to their levels in 2006, but increase over NC where the magnitude of nitrate increase exceeds that of sulfate reduction. This suggests that the SO2 emission reduction target set by the 12th FYP, although effective in reducing SNA over SC and SCB, will not be successful over NC for which NOx emission control needs to be strengthened. If NH3 emissions are allowed to keep their recent growth rate and increase by +16% from 2006 to 2015, the benefit of SO2 reduction will be completely offset over all of China due to the significant increase of nitrate, demonstrating the critical role of NH3 in regulating nitrate. The effective strategy to control SNA and hence PM2.5 pollution over China should thus be based on improving understanding of current NH3 emissions and putting more emphasis on controlling NH3 emissions in the future.

scholarly journals Concentrations and radiative forcing of anthropogenic aerosols from 1750–2014 simulated with the OsloCTM3 and CEDS emission inventory

2018 ◽  
Author(s):  
Marianne T. Lund ◽  
Gunnar Myhre ◽  
Amund S. Haslerud ◽  
Ragnhild B. Skeie ◽  
Jan Griesfeller ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
Emission Inventory ◽  
Transport Model ◽  
Model Performance ◽  
Anthropogenic Aerosols ◽  
Anthropogenic Aerosol ◽  
Emission Data ◽  
Sensitivity Tests ◽  
Emission Changes ◽  
New Community

Abstract. We document the ability of the new generation Oslo chemistry-transport model, OsloCTM3, to accurately simulate present-day aerosol distributions. The model is then used with the new Community Emission Data System (CEDS) historical emission inventory to provide updated time series of anthropogenic aerosol concentrations and consequent direct radiative forcing (RFari) from 1750 to 2014. Overall, the OsloCTM3 performs well compared with measurements of surface concentrations and remotely sensed aerosol optical depth. Concentrations are underestimated in Asia, but the higher emissions in CEDS than previous inventories result in improvements compared to observations. The black carbon (BC) treatment in OsloCTM3 gives better agreement with observed vertical BC profiles relative to the predecessor OsloCTM2. However, Arctic wintertime BC concentrations remain underestimated, and a range of sensitivity tests indicate that better physical understanding of processes associated with atmospheric BC processing is required to simultaneously reproduce both the observed features. Uncertainties in model input data, resolution and scavenging affects the distribution of all aerosols species, especially at high latitudes and altitudes. However, we find no evidence of consistently better model performance across all observables and regions in the sensitivity tests than in the baseline configuration. Using CEDS, we estimate a total net RFari in 2014 relative to 1750 of −0.17 W m−2, significantly weaker than the IPCC AR5 2010–1750 estimate. Differences are attributable to several factors, including stronger absorption by organic aerosol, updated parameterization of BC absorption, and reduced sulfate cooling. The trend towards a weaker RFari over recent years is more pronounced than in the IPCC AR5, illustrating the importance of capturing recent regional emission changes.

scholarly journals Concentrations and radiative forcing of anthropogenic aerosols from 1750 to 2014 simulated with the Oslo CTM3 and CEDS emission inventory

2018 ◽  
Vol 11 (12) ◽  
pp. 4909-4931 ◽  
Author(s):  
Marianne Tronstad Lund ◽  
Gunnar Myhre ◽  
Amund Søvde Haslerud ◽  
Ragnhild Bieltvedt Skeie ◽  
Jan Griesfeller ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
Emission Inventory ◽  
Transport Model ◽  
Model Performance ◽  
Anthropogenic Aerosols ◽  
Anthropogenic Aerosol ◽  
Emission Data ◽  
Sensitivity Tests ◽  
Emission Changes ◽  
New Community

Abstract. We document the ability of the new-generation Oslo chemistry-transport model, Oslo CTM3, to accurately simulate present-day aerosol distributions. The model is then used with the new Community Emission Data System (CEDS) historical emission inventory to provide updated time series of anthropogenic aerosol concentrations and consequent direct radiative forcing (RFari) from 1750 to 2014. Overall, Oslo CTM3 performs well compared with measurements of surface concentrations and remotely sensed aerosol optical depth. Concentrations are underestimated in Asia, but the higher emissions in CEDS than previous inventories result in improvements compared to observations. The treatment of black carbon (BC) scavenging in Oslo CTM3 gives better agreement with observed vertical BC profiles relative to the predecessor Oslo CTM2. However, Arctic wintertime BC concentrations remain underestimated, and a range of sensitivity tests indicate that better physical understanding of processes associated with atmospheric BC processing is required to simultaneously reproduce both the observed features. Uncertainties in model input data, resolution, and scavenging affect the distribution of all aerosols species, especially at high latitudes and altitudes. However, we find no evidence of consistently better model performance across all observables and regions in the sensitivity tests than in the baseline configuration. Using CEDS, we estimate a net RFari in 2014 relative to 1750 of −0.17 W m−2, significantly weaker than the IPCC AR5 2011–1750 estimate. Differences are attributable to several factors, including stronger absorption by organic aerosol, updated parameterization of BC absorption, and reduced sulfate cooling. The trend towards a weaker RFari over recent years is more pronounced than in the IPCC AR5, illustrating the importance of capturing recent regional emission changes.

scholarly journals Key factors affecting single scattering albedo calculation: Implications for aerosol climate forcing

2017 ◽  
Author(s):  
Duseong S. Jo ◽  
Rokjin J. Park ◽  
Jaein I. Jeong ◽  
Gabriele Curci ◽  
Hyung-Min Lee ◽  
...  
Keyword(s):  
Particulate Matter ◽  
Radiative Forcing ◽  
Transport Model ◽  
Geometric Mean ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
Geometric Standard Deviation ◽  
Physical Parameters ◽  
Chemical Transport Model ◽  
Aerosol Mass

Abstract. Single Scattering Albedo (SSA), the ratio of scattering efficiency to total extinction efficiency, is an essential parameter used to estimate the Direct Radiative Forcing (DRF) of aerosols. However, SSA is one of the large contributors to the uncertainty of DRF estimations. In this study, we examined the sensitivity of SSA calculations to the physical properties of absorbing aerosols, in particular, Black Carbon (BC), Brown Carbon (BrC), and dust. We used GEOS-Chem 3-D global chemical transport model (CTM) simulations and a post-processing tool for the aerosol optical properties (FlexAOD). The model and input parameters were evaluated by comparison against the observed aerosol mass concentrations and the Aerosol Optical Depth (AOD) values obtained from global surface observation networks such as the global Aerosol Mass Spectrometer (AMS) dataset, the Surface Particulate Matter Network (SPARTAN), and the Aerosol Robotic Network (AERONET). The model was generally successful in reproducing the observed variability of both the Particulate Matter 2.5 μm (PM2.5) and AOD (R ~ 0.76) values, although it underestimated the magnitudes by approximately 20 %. Our sensitivity tests of the SSA calculation revealed that the aerosol physical parameters, which have generally received less attention than the aerosol mass loadings, can cause large uncertainties in the resulting DRF estimation. For example, large variations in the calculated BC absorption may result from slight changes of the geometric mean radius, geometric standard deviation, real and imaginary refractive indices, and density. The inclusion of BrC and observationally-constrained dust size distributions also significantly affected the SSA, and resulted in a remarkable improvement for the simulated SSA at 440 nm (bias was reduced by 44–49 %) compared with the AERONET observations. Based on the simulations performed during this study, we found that the global aerosol direct radiative effect was increased by 10 % after the SSA bias was reduced.

scholarly journals Concentrations and source regions of light absorbing impurities in snow/ice in northern Pakistan and their impact on snow albedo

2017 ◽  
Author(s):  
Chaman Gul ◽  
Siva Praveen Puppala ◽  
Shichang Kang ◽  
Bhupesh Adhikary ◽  
Yulan Zhang ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
Transport Model ◽  
Chemical Transport ◽  
Small Contribution ◽  
Northern Pakistan ◽  
Chemical Transport Model ◽  
Transport Modelling ◽  
Snow Albedo ◽  
Source Regions ◽  
Snow And Ice

Abstract. Black carbon (BC), water-insoluble organic carbon (OC), and mineral dust are important particulate impurities in snow and ice, which significantly reduce albedo and accelerate melting. Surface snow and ice samples were collected from the Karakoram–Himalayan region of northern Pakistan during 2015 and 2016 in summer (six glaciers), autumn (two glaciers), and winter (six mountain valleys). The average BC concentration overall was 2130 ± 1560 ngg−1 in summer samples, 2883 ± 3439 ngg−1 in autumn samples, and 992 ± 883 ngg−1 in winter samples. The average water insoluble OC concentration overall was 1839 ± 1108 ngg−1 in summer samples, 1423 ± 208 ngg−1 in autumn samples, and 1342 ± 672 ngg−1 in winter samples. The overall concentration of BC, OC, and dust in aged snow samples collected during the summer campaign was higher than the concentration in ice samples. The values are relatively high compared to reports by others for the Himalayas and Tibetan Plateau. This is probably the result of taking more representative samples at lower elevation where deposition is higher and the effects of ageing and enrichment more marked. A reduction in snow albedo of 0.1–8.3 % for fresh snow and 0.9–32.5 % for aged snow was calculated for selected solar zenith angles during day time using the Snow, Ice, and Aerosol Radiation (SNICAR) model. Daily mean albedo was reduced by 0.07–12.0 %. The calculated radiative forcing ranged from 0.16 to 43.45 Wm−2 depending on snow type, solar zenith angle, and location. The potential source regions of the deposited pollutants were identified using spatial variance in wind vector maps, emission inventories coupled with backward air trajectories, and simple region tagged chemical transport modelling. Central, South, and West Asia were the major sources of pollutants during the sampling months, with only a small contribution from East Asia. Analysis based on the Weather Research and Forecasting (WRF-STEM) chemical transport model identified a significant contribution (more than 70 %) from South Asia at selected sites. Research into the presence and effect of pollutants in the glaciated areas of Pakistan is economically significant because the surface water resources in the country mainly depend on the rivers (the Indus and its tributaries) that flow from this glaciated area.

scholarly journals Contrasting the direct radiative effect and direct radiative forcing of aerosols

2014 ◽  
Vol 14 (11) ◽  
pp. 5513-5527 ◽  
Author(s):  
C. L. Heald ◽  
D. A. Ridley ◽  
J. H. Kroll ◽  
S. R. H. Barrett ◽  
K. E. Cady-Pereira ◽  
...  
Keyword(s):  
Energy Balance ◽  
Radiative Forcing ◽  
Transport Model ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Radiative Effect ◽  
Chemical Transport Model ◽  
Anthropogenic Aerosols ◽  
Anthropogenic Aerosol ◽  
Direct Radiative Forcing

Abstract. The direct radiative effect (DRE) of aerosols, which is the instantaneous radiative impact of all atmospheric particles on the Earth's energy balance, is sometimes confused with the direct radiative forcing (DRF), which is the change in DRE from pre-industrial to present-day (not including climate feedbacks). In this study we couple a global chemical transport model (GEOS-Chem) with a radiative transfer model (RRTMG) to contrast these concepts. We estimate a global mean all-sky aerosol DRF of −0.36 Wm−2 and a DRE of −1.83 Wm−2 for 2010. Therefore, natural sources of aerosol (here including fire) affect the global energy balance over four times more than do present-day anthropogenic aerosols. If global anthropogenic emissions of aerosols and their precursors continue to decline as projected in recent scenarios due to effective pollution emission controls, the DRF will shrink (−0.22 Wm−2 for 2100). Secondary metrics, like DRE, that quantify temporal changes in both natural and anthropogenic aerosol burdens are therefore needed to quantify the total effect of aerosols on climate.

scholarly journals Do contemporary (1980–2015) emissions determine the elemental carbon deposition trend at Holtedahlfonna glacier, Svalbard?

2017 ◽  
Vol 17 (20) ◽  
pp. 12779-12795 ◽  
Author(s):  
Meri M. Ruppel ◽  
Joana Soares ◽  
Jean-Charles Gallet ◽  
Elisabeth Isaksson ◽  
Tõnu Martma ◽  
...  
Keyword(s):  
Elemental Carbon ◽  
Transport Model ◽  
Ice Core ◽  
Climate Impact ◽  
The Arctic ◽  
Chemical Transport Model ◽  
Atmospheric Measurements ◽  
Atmospheric Concentration ◽  
Scavenging Efficiency ◽  
Firn Core

Abstract. The climate impact of black carbon (BC) is notably amplified in the Arctic by its deposition, which causes albedo decrease and subsequent earlier snow and ice spring melt. To comprehensively assess the climate impact of BC in the Arctic, information on both atmospheric BC concentrations and deposition is essential. Currently, Arctic BC deposition data are very scarce, while atmospheric BC concentrations have been shown to generally decrease since the 1990s. However, a 300-year Svalbard ice core showed a distinct increase in EC (elemental carbon, proxy for BC) deposition from 1970 to 2004 contradicting atmospheric measurements and modelling studies. Here, our objective was to decipher whether this increase has continued in the 21st century and to investigate the drivers of the observed EC deposition trends. For this, a shallow firn core was collected from the same Svalbard glacier, and a regional-to-meso-scale chemical transport model (SILAM) was run from 1980 to 2015. The ice and firn core data indicate peaking EC deposition values at the end of the 1990s and lower values thereafter. The modelled BC deposition results generally support the observed glacier EC variations. However, the ice and firn core results clearly deviate from both measured and modelled atmospheric BC concentration trends, and the modelled BC deposition trend shows variations seemingly independent from BC emission or atmospheric BC concentration trends. Furthermore, according to the model ca. 99 % BC mass is wet-deposited at this Svalbard glacier, indicating that meteorological processes such as precipitation and scavenging efficiency have most likely a stronger influence on the BC deposition trend than BC emission or atmospheric concentration trends. BC emission source sectors contribute differently to the modelled atmospheric BC concentrations and BC deposition, which further supports our conclusion that different processes affect atmospheric BC concentration and deposition trends. Consequently, Arctic BC deposition trends should not directly be inferred based on atmospheric BC measurements, and more observational BC deposition data are required to assess the climate impact of BC in Arctic snow.

scholarly journals Organic nitrate chemistry and its implications for nitrogen budgets in an isoprene- and monoterpene-rich atmosphere: constraints from aircraft (SEAC<sup>4</sup>RS) and ground-based (SOAS) observations in the Southeast US

2016 ◽  
Vol 16 (9) ◽  
pp. 5969-5991 ◽  
Author(s):  
Jenny A. Fisher ◽  
Daniel J. Jacob ◽  
Katherine R. Travis ◽  
Patrick S. Kim ◽  
Eloise A. Marais ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Gas Phase ◽  
Transport Model ◽  
Oxidation Mechanism ◽  
Organic Nitrate ◽  
Organic Nitrates ◽  
Nox Emissions ◽  
Particle Phase ◽  
Chemical Transport Model ◽  
Southeast Us

Abstract. Formation of organic nitrates (RONO2) during oxidation of biogenic volatile organic compounds (BVOCs: isoprene, monoterpenes) is a significant loss pathway for atmospheric nitrogen oxide radicals (NOx), but the chemistry of RONO2 formation and degradation remains uncertain. Here we implement a new BVOC oxidation mechanism (including updated isoprene chemistry, new monoterpene chemistry, and particle uptake of RONO2) in the GEOS-Chem global chemical transport model with  ∼  25  ×  25 km2 resolution over North America. We evaluate the model using aircraft (SEAC4RS) and ground-based (SOAS) observations of NOx, BVOCs, and RONO2 from the Southeast US in summer 2013. The updated simulation successfully reproduces the concentrations of individual gas- and particle-phase RONO2 species measured during the campaigns. Gas-phase isoprene nitrates account for 25–50 % of observed RONO2 in surface air, and we find that another 10 % is contributed by gas-phase monoterpene nitrates. Observations in the free troposphere show an important contribution from long-lived nitrates derived from anthropogenic VOCs. During both campaigns, at least 10 % of observed boundary layer RONO2 were in the particle phase. We find that aerosol uptake followed by hydrolysis to HNO3 accounts for 60 % of simulated gas-phase RONO2 loss in the boundary layer. Other losses are 20 % by photolysis to recycle NOx and 15 % by dry deposition. RONO2 production accounts for 20 % of the net regional NOx sink in the Southeast US in summer, limited by the spatial segregation between BVOC and NOx emissions. This segregation implies that RONO2 production will remain a minor sink for NOx in the Southeast US in the future even as NOx emissions continue to decline.

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