Abstract Trends in fossil fuel emissions are a major driver of changes in atmospheric CO, but detection of trends in CO from anthropogenic sources is complicated by the presence of large interannual variability (IAV) in biomass burning. We use a multiyear model simulation of CO with year‐specific biomass burning to predict the number of years needed to detect the impact of changes in Asian anthropogenic emissions on downwind regions. Our study includes two cases for changing anthropogenic emissions: a stepwise change of 15% and a linear trend of 3% yr −1 . We first examine how well the model reproduces the observed IAV of CO over the North Pacific, since this variability impacts the time needed to detect significant anthropogenic trends. The modeled IAV over the North Pacific correlates well with that seen from the Measurements of Pollution in the Troposphere (MOPITT) instrument but underestimates the magnitude of the variability. The model predicts that a 3% yr −1 trend in Asian anthropogenic emissions would lead to a statistically significant trend in CO surface concentration in the western United States within 12 years, and accounting for Siberian boreal biomass‐burning emissions greatly reduces the number of years needed for trend detection. Combining the modeled trend with the observed MOPITT variability at 500 hPa, we estimate that the 3% yr −1 trend could be detectable in satellite observations over Asia in approximately a decade. Our predicted timescales for trend detection highlight the importance of long‐term measurements of CO from satellites.
Abstract. Interannual variations in background tropospheric trace gases (such as carbon monoxide, CO) are largely driven by variations in emissions (especially wildfires) and transport pathways. Understanding this variability is essential to quantify the intercontinental contribution to US air quality. We investigate the interannual variability of long-range transport of Asian pollutants to the Northeast Pacific via measurements from the Mt. Bachelor Observatory (MBO: 43.98° N, 121.69° W; 2.7 km a.s.l.) and GEOS-Chem chemical transport model simulations in spring 2005 vs. the INTEX-B campaign during spring 2006. Measurements of CO at MBO were significantly enhanced during spring 2005 relative to the same time in 2006 (the INTEX-B study period); a decline in monthly mean CO of 41 ppbv was observed between April 2005 and April 2006. A backtrajectory-based meteorological index shows that long-range transport of CO from the heavily industrialized region of East Asia was significantly greater in early spring 2005 than in 2006. In addition, spring 2005 was an anomalously strong biomass burning season in Southeast Asia. Data presented by Yurganov et al. (2008) using MOPITT satellite retrievals from this area reveal an average CO burden anomaly (referenced to March 2000–February 2002 mean values) between October 2004 through April 2005 of 2.6 Tg CO vs. 0.6 Tg CO for the same period a year later. The Naval Research Laboratory's global aerosol transport model, as well as winds from NCEP reanalysis, show that emissions from these fires were efficiently transported to MBO throughout April 2005. Asian dust transport, however, was substantially greater in 2006 than 2005, particularly in May. Monthly mean aerosol light scattering coefficient at 532 nm (σsp) at MBO more than doubled from 2.7 Mm−1 in May 2005 to 6.2 Mm−1 in May 2006. We also evaluate CO interannual variability throughout the western US via Earth System Research Laboratory ground site data and throughout the Northern Hemisphere via MOPITT and TES satellite observations. Both in the Northeast Pacific and on larger scales, we reveal a significant decrease (from 2–21%) in springtime maximum CO between 2005 and 2006, evident in all platforms and the GEOS-Chem model. We attribute this to (a) anomalously strong biomass burning in Southeast Asia during winter 2004 through spring 2005, and (b) the transport pattern in March and April 2006 which limited the inflow of Asian pollution to the lower free troposphere over western North America.
Abstract The oxidizing capacity of the troposphere is controlled primarily by the abundance of hydroxyl radical (OH). The global mean concentration of tropospheric OH, [OH] TROP (the burden of OH in the global troposphere appropriate for calculating the lifetime of methane) inferred from measurements of methyl chloroform has remained relatively constant during the past several decades despite rising levels of methane that should have led to a decline. Here we examine other factors that may have affected [OH] TROP such as the changing values of stratospheric ozone, rising tropospheric H 2 O, varying burden of NO x (=NO+NO 2 ), rising temperatures, and widening of the climatological tropics due to expansion of the Hadley cell. Our analysis suggests the positive trends in [OH] TROP due to H 2 O, NO x , and overhead O 3 , and tropical expansion are large enough (Δ [OH] TROP = +0.95 ± 0.18%/decade) to counter almost all of the expected decrease in [OH] TROP due to rising methane (Δ [OH] TROP = −1.01 ± 0.05%/decade) over the period 1980 to 2015, while variations in temperature contribute almost no trend (Δ [OH] TROP = −0.02 ± 0.02%/decade) in [OH] TROP . The approximated impact of Hadley cell expansion on [OH] TROP is also a small but not insignificant factor partially responsible for the steadiness of tropospheric oxidizing capacity over the past several decades, which free‐running models likely do not capture.
Abstract. Measurements from actinic flux spectroradiometers on board the NASA DC-8 during the Atmospheric Tomography (ATom) mission provide an extensive set of statistics on how clouds alter photolysis rates (J-values) throughout the remote Pacific and Atlantic Ocean basins. ATom made profiling circumnavigations of the troposphere over four seasons during 2016–2018. J-values are a primary chemical control over tropospheric ozone and methane abundances and their greenhouse effects. Clouds have been recognized for more than three decades as being an important factor in tropospheric chemistry. The ATom climatology of J-values is a unique test of how the chemistry models treat clouds. This work focuses on measurements over the Pacific during the first deployment (ATom-1) in August 2016. Nine global chemistry–climate or –transport models provide J-values for the domains measured in ATom-1. We compare mean profiles over a range of cloudy and clear conditions; but, more importantly, we build a statistical picture of the impact of clouds on J-values through the distribution of the ratio of J-cloudy to J-clear. In detail, the models show largely disparate patterns. When compared with measurements, there is some limited, broad agreement. Models here have resolutions of 50–200 km and thus reduce the occurrence of clear sky when averaging over grid cells. In situ measurements also average the scattered sunlight, but only out to scales of 10 s of km. A primary uncertainty remains in the role of clouds in chemistry, in particular, how models average over cloud fields, and how such averages can simulate measurements.
Abstract. An approach for analysis and modeling of global atmospheric chemistry is developed for application to measurements that provide a tropospheric climatology of those heterogeneously distributed, reactive species that control the loss of methane and the production and loss of ozone. We identify key species (e.g., O3, NOx, HNO3, HNO4, C2H3NO5, H2O, HOOH, CH3OOH, HCHO, CO, CH4, C2H6, acetaldehyde, acetone), and presume that they can be measured simultaneously in air parcels on the scale of a few km horizontally and a few tenths vertically. Six global models have prepared such climatologies (at model resolution) for August with emphasis on the vast central Pacific and Atlantic Ocean basins. We show clear differences in model generated reactivities as well as species covariances that could readily be discriminated with an unbiased climatology. A primary tool is comparison of multi-dimensional probability densities of key species weighted by frequency of occurrence as well as by the reactivity of the parcels with respect to methane and ozone. The reactivity-weighted probabilities tell us which parcels matter in this case. Testing 100-km scale models with 2-km measurements using these tools also addresses a core question about model resolution and whether fine-scale atmospheric structures matter to the overall ozone and methane budget. A new method enabling these six global chemistry-climate models to ingest an externally-sourced climatology and then compute air parcel reactivity is demonstrated. Such an observed climatology is anticipated from the NASA Atmospheric Tomography (ATom) aircraft mission (2015–2020), measuring the key species, executing profiles over the Pacific and Atlantic Ocean basins. This work is a core part of the design of ATom.
Abstract. The NASA Atmospheric Tomography (ATom) mission built a photochemical climatology of air parcels based on in situ measurements with the NASA DC-8 aircraft along objectively planned profiling transects through the middle of the Pacific and Atlantic oceans. In this paper we present and analyze a data set of 10 s (2 km) merged and gap-filled observations of the key reactive species driving the chemical budgets of O3 and CH4 (O3, CH4, CO, H2O, HCHO, H2O2, CH3OOH, C2H6, higher alkanes, alkenes, aromatics, NOx, HNO3, HNO4, peroxyacetyl nitrate, and other organic nitrates), consisting of 146 494 distinct air parcels from ATom deployments 1 through 4. Six models calculated the O3 and CH4 photochemical tendencies from this modeling data stream for ATom 1. We find that 80 %–90 % of the total reactivity lies in the top 50 % of the parcels and 25 %–35 % in the top 10 %, supporting previous model-only studies that tropospheric chemistry is driven by a fraction of all the air. Surprisingly, the probability densities of species and reactivities averaged on a model scale (100 km) differ only slightly from the 2 km ATom 10 s data, indicating that much of the heterogeneity in tropospheric chemistry can be captured with current global chemistry models. Comparing the ATom reactivities over the tropical oceans with climatological statistics from six global chemistry models, we find generally good agreement with the reactivity rates for O3 and CH4. Models distinctly underestimate O3 production below 2 km relative to the mid-troposphere, and this can be traced to lower NOx levels than observed. Attaching photochemical reactivities to measurements of chemical species allows for a richer, yet more constrained-to-what-matters, set of metrics for model evaluation. This paper presents a corrected version of the paper published under the same authors and title (sans “corrected”) as https://doi.org/10.5194/acp-21-13729-2021.
Abstract. Results from simulations performed for the Atmospheric Chemistry and Climate Modeling Intercomparison Project (ACCMIP) are analysed to examine how OH and methane lifetime may change from present day to the future, under different climate and emissions scenarios. Present day (2000) mean tropospheric chemical lifetime derived from the ACCMIP multi-model mean is 9.8 ± 1.6 yr (9.3 ± 0.9 yr when only including selected models), lower than a recent observationally-based estimate, but with a similar range to previous multi-model estimates. Future model projections are based on the four Representative Concentration Pathways (RCPs), and the results also exhibit a large range. Decreases in global methane lifetime of 4.5 ± 9.1% are simulated for the scenario with lowest radiative forcing by 2100 (RCP 2.6), while increases of 8.5 ± 10.4% are simulated for the scenario with highest radiative forcing (RCP 8.5). In this scenario, the key driver of the evolution of OH and methane lifetime is methane itself, since its concentration more than doubles by 2100 and it consumes much of the OH that exists in the troposphere. Stratospheric ozone recovery, which drives tropospheric OH decreases through photolysis modifications, also plays a partial role. In the other scenarios, where methane changes are less drastic, the interplay between various competing drivers leads to smaller and more diverse OH and methane lifetime responses, which are difficult to attribute. For all scenarios, regional OH changes are even more variable, with the most robust feature being the large decreases over the remote oceans in RCP8.5. Through a regression analysis, we suggest that differences in emissions of non-methane volatile organic compounds and in the simulation of photolysis rates may be the main factors causing the differences in simulated present day OH and methane lifetime. Diversity in predicted changes between present day and future OH was found to be associated more strongly with differences in modelled temperature and stratospheric ozone changes. Finally, through perturbation experiments we calculated an OH feedback factor (F) of 1.24 from present day conditions (1.50 from 2100 RCP8.5 conditions) and a climate feedback on methane lifetime of 0.33 ± 0.13 yr K−1, on average. Models that did not include interactive stratospheric ozone effects on photolysis showed a stronger sensitivity to climate, as they did not account for negative effects of climate-driven stratospheric ozone recovery on tropospheric OH, which would have partly offset the overall OH/methane lifetime response to climate change.
We investigate the relationships among summertime ozone (O3), temperature, and humidity on daily timescales across the Northern Hemisphere using observations and model simulations. Temperature and humidity are significantly positively correlated with O3 across continental regions in the mid-latitudes (~35-60N). Over the oceans, the relationships are consistently negative. For continental regions outside the mid-latitudes, the O3-meteorology correlations are mixed in strength and sign but generally weak. Over some high latitude, low latitude, and marine regions, temperature and humidity are significantly anticorrelated with O3. Daily variations in transport patterns linked to the position and meridional movement of the jet stream drive the relationships among O3, temperature, and humidity. Within the latitudinal range of the jet, there is an increase (decrease) in O3, temperature, and humidity over land with poleward (equatorward) movement of the jet, while over the oceans poleward movement of the jet results in decreases of these fields. Beyond the latitudes where the jet traverses, the meridional movement of the jet stream has variable or negligible effects on surface-level O3, temperature, and humidity. The O3-meteorology relationships are largely the product of the jet-induced changes in the surface-level meridional flow acting on the background meridional O3 gradient. Our results underscore the importance of considering the role of the jet stream and surface-level flow for the O3-meteorology relationships, especially in light of expected changes to these features under climate change.
Abstract This article provides an overview of the NASA Atmospheric Tomography (ATom) mission and a summary of selected scientific findings to date. ATom was an airborne measurements and modeling campaign aimed at characterizing the composition and chemistry of the troposphere over the most remote regions of the Pacific, Southern, Atlantic, and Arctic Oceans, and examining the impact of anthropogenic and natural emissions on a global scale. These remote regions dominate global chemical reactivity and are exceptionally important for global air quality and climate. ATom data provide the in situ measurements needed to understand the range of chemical species and their reactions, and to test satellite remote sensing observations and global models over large regions of the remote atmosphere. Lack of data in these regions, particularly over the oceans, has limited our understanding of how atmospheric composition is changing in response to shifting anthropogenic emissions and physical climate change. ATom was designed as a global-scale tomographic sampling mission with extensive geographic and seasonal coverage, tropospheric vertical profiling, and detailed speciation of reactive compounds and pollution tracers. ATom flew the NASA DC-8 research aircraft over four seasons to collect a comprehensive suite of measurements of gases, aerosols, and radical species from the remote troposphere and lower stratosphere on four global circuits from 2016 to 2018. Flights maintained near-continuous vertical profiling of 0.15–13-km altitudes on long meridional transects of the Pacific and Atlantic Ocean basins. Analysis and modeling of ATom data have led to the significant early findings highlighted here.
