146 results on '"McKain, Kathryn"'
Search Results
2. The NASA Atmospheric Tomography (ATom) Mission : Imaging the Chemistry of the Global Atmosphere
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Thompson, Chelsea R., Wofsy, Steven C., Prather, Michael J., Newman, Paul A., Hanisco, Thomas F., Ryerson, Thomas B., Fahey, David W., Apel, Eric C., Brock, Charles A., Brune, William H., Froyd, Karl, Katich, Joseph M., Nicely, Julie M., Peischl, Jeff, Ray, Eric, Veres, Patrick R., Wang, Siyuan, Allen, Hannah M., Asher, Elizabeth, Bian, Huisheng, Blake, Donald, Bourgeois, Ilann, Budney, John, Bui, T. Paul, Butler, Amy, Campuzano-Jost, Pedro, Chang, Cecilia, Chin, Mian, Commane, Róisín, Correa, Gus, Crounse, John D., Daube, Bruce, Dibb, Jack E., DiGangi, Joshua P., Diskin, Glenn S., Dollner, Maximilian, Elkins, James W., Fiore, Arlene M., Flynn, Clare M., Guo, Hao, Hall, Samuel R., Hannun, Reem A., Hills, Alan, Hintsa, Eric J., Hodzic, Alma, Hornbrook, Rebecca S., Huey, L. Greg, Jimenez, Jose L., Keeling, Ralph F., Kim, Michelle J., Kupc, Agnieszka, Lacey, Forrest, Lait, Leslie R., Lamarque, Jean-Francois, Liu, Junhua, McKain, Kathryn, Meinardi, Simone, Miller, David O., Montzka, Stephen A., Moore, Fred L., Morgan, Eric J., Murphy, Daniel M., Murray, Lee T., Nault, Benjamin A., Neuman, J. Andrew, Nguyen, Louis, Gonzalez, Yenny, Rollins, Andrew, Rosenlof, Karen, Sargent, Maryann, Schill, Gregory, Schwarz, Joshua P., St. Clair, Jason M., Steenrod, Stephen D., Stephens, Britton B., Strahan, Susan E., Strode, Sarah A., Sweeney, Colm, Thames, Alexander B., Ullmann, Kirk, Wagner, Nicholas, Weber, Rodney, Weinzierl, Bernadett, Wennberg, Paul O., Williamson, Christina J., Wolfe, Glenn M., and Zeng, Linghan
- Published
- 2022
3. Large contribution of biomass burning emissions to ozone throughout the global remote troposphere
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Bourgeois, Ilann, Peischl, Jeff, Neuman, J. Andrew, Brown, Steven S., Thompson, Chelsea R., Aikin, Kenneth C., Allen, Hannah M., Angot, Hélène, Apel, Eric C., Baublitz, Colleen B., Brewer, Jared F., Campuzano-Jost, Pedro, Commane, Róisín, Crounse, John D., Daube, Bruce C., DiGangi, Joshua P., Diskin, Glenn S., Emmons, Louisa K., Fiore, Arlene M., Gkatzelis, Georgios I., Hills, Alan, Hornbrook, Rebecca S., Huey, L. Gregory, Jimenez, Jose L., Kim, Michelle, Lacey, Forrest, McKain, Kathryn, Murray, Lee T., Nault, Benjamin A., Parrish, David D., Ray, Eric, Sweeney, Colm, Tanner, David, Wofsy, Steven C., and Ryerson, Thomas B.
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- 2021
4. Correction: COS-derived GPP relationships with temperature and light help explain high-latitude atmospheric CO₂ seasonal cycle amplification
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Hu, Lei, Montzka, Stephen A., Kaushik, Aleya, Andrews, Arlyn E., Sweeney, Colm, Miller, John, Baker, Ian T., Denning, Scott, Campbell, Elliott, Shiga, Yoichi P., Tans, Pieter, Siso, M. Carolina, Crotwell, Molly, McKain, Kathryn, Thoning, Kirk, Hall, Bradley, Vimont, Isaac, Elkins, James W., Whelan, Mary E., and Suntharalingam, Parvadha
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- 2021
5. Majority of US urban natural gas emissions unaccounted for in inventories
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Sargent, Maryann R., Floerchinger, Cody, McKain, Kathryn, Budney, John, Gottlieb, Elaine W., Hutyra, Lucy R., Rudek, Joseph, and Wofsy, Steven C.
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- 2021
6. COS-derived GPP relationships with temperature and light help explain high-latitude atmospheric CO₂ seasonal cycle amplification
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Hu, Lei, Montzka, Stephen A., Kaushik, Aleya, Andrews, Arlyn E., Sweeney, Colm, Miller, John, Baker, Ian T., Denning, Scott, Campbell, Elliott, Shiga, Yoichi P., Tans, Pieter, Siso, M. Carolina, Crotwell, Molly, McKain, Kathryn, Thoning, Kirk, Hall, Bradley, Vimont, Isaac, Elkins, James W., Whelan, Mary E., and Suntharalingam, Parvadha
- Published
- 2021
7. Methane emissions from oil and gas production on the North Slope of Alaska
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Floerchinger, Cody, McKain, Kathryn, Bonin, Timothy, Peischl, Jeff, Biraud, Sébastien C., Miller, Charles, Ryerson, Thomas B., Wofsy, Steven C., and Sweeney, Colm
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- 2019
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8. Nonlinear and Non‐Gaussian Ensemble Assimilation of MOPITT CO.
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Gaubert, Benjamin, Anderson, Jeffrey L., Trudeau, Michael, Smith, Nadia, McKain, Kathryn, Pétron, Gabrielle, Raeder, Kevin, Arellano, Avelino F., Granier, Claire, Emmons, Louisa K., Ortega, Ivan, Hannigan, James W., Tang, Wenfu, Worden, Helen M., Ziskin, Daniel, and Edwards, David P.
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KALMAN filtering ,CARBON monoxide ,ATMOSPHERIC chemistry ,ATMOSPHERIC models ,ATMOSPHERIC composition ,ATMOSPHERIC boundary layer ,CARBON cycle - Abstract
Satellite retrievals of carbon monoxide (CO) are routinely assimilated in atmospheric chemistry models to improve air quality forecasts, produce reanalyzes and to estimate emissions. This study applies the quantile‐conserving ensemble filter framework, a novel assimilation algorithm that can deal with non‐Gaussian and modestly nonlinear distributions. Instead of assuming normal distributions like the Ensemble Adjustments Kalman Filter (EAKF), we now apply a bounded normal rank histogram (BNRH) distribution for the prior. The goal is to efficiently estimate bounded quantities such as CO atmospheric mixing ratios and emission fluxes while maintaining the good performance achieved by the EAKF. We contrast assimilating meteorological and MOPITT (Measurement of Pollution in the Troposphere) observations for May 2018. We evaluate the results with the fourth deployment of the NASA Atmospheric Tomography Mission (ATom‐4) airborne field campaign. We also compare simulations with CO tropospheric columns from the network for the detection of atmospheric composition change and surface in‐situ observations from NOAA carbon cycle greenhouse gases. While the differences remain small, the BNRH approach clearly works better than the EAKF in comparison to all observation data sets. Plain Language Summary: The MOPITT instrument on the NASA/Terra satellite can detect carbon monoxide (CO) pollution in the lower and mid‐tropospheric atmosphere but cannot accurately differentiate small changes in the altitude of pollution plumes. Such satellite observations are assimilated in numerical model predictions to improve the spatial and temporal distribution of CO in the atmosphere and to estimate emission fluxes. We present a novel method that does not require assumptions about the model and the observations, leading to a more efficient and accurate assimilation of the satellite observations. Key Points: A novel non Gaussian and nonlinear ensemble data assimilation (DA) framework is applied to MOPITT joint state/flux optimizationThe new method performs better than the Ensemble Adjustment Kalman Filter in comparison to independent observationsMOPITT observations indicate that CAMS‐GLOB‐ANT_v5.3 emission fluxes are underestimated across the mid‐latitudes in May 2018 [ABSTRACT FROM AUTHOR]
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- 2024
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9. Anthropogenic and biogenic CO₂ fluxes in the Boston urban region
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Sargent, Maryann, Barrera, Yanina, Nehrkorn, Thomas, Hutyra, Lucy R., Gately, Conor K., Jones, Taylor, McKain, Kathryn, Sweeney, Colm, Hegarty, Jennifer, Hardiman, Brady, and Wofsy, Steven C.
- Published
- 2018
10. THE O₂/N₂ RATIO AND CO₂ AIRBORNE SOUTHERN OCEAN STUDY
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Stephens, Britton B., Long, Matthew C., Keeling, Ralph F., Kort, Eric A., Sweeney, Colm, Apel, Eric C., Atlas, Elliot L., Beaton, Stuart, Bent, Jonathan D., Blake, Nicola J., Bresch, James F., Casey, Joanna, Daube, Bruce C., Diao, Minghui, Diaz, Ernesto, Dierssen, Heidi, Donets, Valeria, Gao, Bo-Cai, Gierach, Michelle, Green, Robert, Haag, Justin, Hayman, Matthew, Hills, Alan J., Hoecker-Martínez, Martín S., Honomichl, Shawn B., Hornbrook, Rebecca S., Jensen, Jorgen B., Li, Rong-Rong, McCubbin, Ian, McKain, Kathryn, Morgan, Eric J., Nolte, Scott, Powers, Jordan G., Rainwater, Bryan, Randolph, Kaylan, Reeves, Mike, Schauffler, Sue M., Smith, Katherine, Smith, Mackenzie, Stith, Jeff, Stossmeister, Gregory, Toohey, Darin W., and Watt, Andrew S.
- Published
- 2018
11. Neutral Tropical African CO2 Exchange Estimated From Aircraft and Satellite Observations.
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Gaubert, Benjamin, Stephens, Britton B., Baker, David F., Basu, Sourish, Bertolacci, Michael, Bowman, Kevin W., Buchholz, Rebecca, Chatterjee, Abhishek, Chevallier, Frédéric, Commane, Róisín, Cressie, Noel, Deng, Feng, Jacobs, Nicole, Johnson, Matthew S., Maksyutov, Shamil S., McKain, Kathryn, Liu, Junjie, Liu, Zhiqiang, Morgan, Eric, and O'Dell, Chris
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CARBON cycle ,ATMOSPHERIC carbon dioxide ,MODEL airplanes ,ARTIFICIAL satellites ,CARBON dioxide ,MOLE fraction - Abstract
Tropical lands play an important role in the global carbon cycle yet their contribution remains uncertain owing to sparse observations. Satellite observations of atmospheric carbon dioxide (CO2) have greatly increased spatial coverage over tropical regions, providing the potential for improved estimates of terrestrial fluxes. Despite this advancement, the spread among satellite‐based and in‐situ atmospheric CO2 flux inversions over northern tropical Africa (NTA), spanning 0–24°N, remains large. Satellite‐based estimates of an annual source of 0.8–1.45 PgC yr−1 challenge our understanding of tropical and global carbon cycling. Here, we compare posterior mole fractions from the suite of inversions participating in the Orbiting Carbon Observatory 2 (OCO‐2) Version 10 Model Intercomparison Project (v10 MIP) with independent in‐situ airborne observations made over the tropical Atlantic Ocean by the National Aeronautics and Space Administration (NASA) Atmospheric Tomography (ATom) mission during four seasons. We develop emergent constraints on tropical African CO2 fluxes using flux‐concentration relationships defined by the model suite. We find an annual flux of 0.14 ± 0.39 PgC yr−1 (mean and standard deviation) for NTA, 2016–2018. The satellite‐based flux bias suggests a potential positive concentration bias in OCO‐2 B10 and earlier version retrievals over land in NTA during the dry season. Nevertheless, the OCO‐2 observations provide improved flux estimates relative to the in situ observing network at other times of year, indicating stronger uptake in NTA during the wet season than the in‐situ inversion estimates. Plain Language Summary: Satellite carbon dioxide (CO2) observations over land imply a major revision to our understanding of the global carbon cycle linked to large emissions from northern tropical Africa (NTA) during the dry season, from October to May. We use aircraft observations made over the Atlantic Ocean in four seasons to evaluate flux models driven by a range of ground and satellite observations. Our results show that models using satellite observations over land overestimate annual emissions from NTA by approximately 1 PgC yr−1, concentrated in the dry season. At other times of year, satellite CO2 observations provide improved estimates of NTA exchange, with a stronger CO2 uptake during the wet season. Key Points: Emergent constraints derived from aircraft carbon dioxide (CO2) measurements and inversions estimate a near neutral northern tropical African CO2 budgetInversions using satellite observations overestimate annual emissions from northern tropical Africa (NTA) by approximately 1 PgC yr−1Satellite CO2 observations imply a strong sink during the wet season over NTA [ABSTRACT FROM AUTHOR]
- Published
- 2023
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12. Constraining Remote Oxidation Capacity with ATom Observations
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Travis, Katherine R, Heald, Colette L, Allen, Hannah M, Apel, Eric C, Arnold, Stephen R, Blake, Donald R, Brune, William H, Chen, Xin, Commane, Róisín, Crounse, John D, Daube, Bruce C, Diskin, Glenn S, Elkins, James W, Evans, Mathew J, Hall, Samuel R, Hintsa, Eric J, Hornbrook, Rebecca S, Kasibhatla, Prasad S, Kim, Michelle J, Luo, Gan, McKain, Kathryn, Millet, Dylan B, Moore, Fred L, Peischl, Jeffrey, Ryerson, Thomas B, Sherwen, Tomás, Thames, Alexander B, Ullmann, Kirk, Wang, Xuan, Wennberg, Paul O, Wolfe, Glenn M, and Yu, Fangqun
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Geophysics ,Environment Pollution - Abstract
The global oxidation capacity, defined as the tropospheric mean concentration of the hydroxyl radical (OH), controls the lifetime of reactive trace gases in the atmosphere such as methane and carbon monoxide (CO). Models tend to underestimate the methane lifetime and CO concentrations throughout the troposphere, which is consistent with excessive OH. Approximately half the oxidation of methane and non-methane volatile organic compounds (VOCs) is thought to occur over the oceans where oxidant chemistry has received little validation due to a lack of observational constraints. We use observations from the first two deployments of the NASA ATom aircraft campaign during July–August 2016 and January–February 2017 to evaluate the oxidation capacity over the remote oceans and its representation in the GEOS-Chem chemical transport model. The model successfully simulates the magnitude and vertical profile of remote OH within the measurement uncertainties. Comparisons against the drivers of OH production (water vapor, ozone, and NOy concentrations, ozone photolysis frequencies) also show minimal bias with the exception of wintertime NOy, for which a model overestimate may indicate insufficient wet scavenging and/or missing loss on seasalt aerosol but large uncertainties remain that require further studies of NOy partitioning and removal in the troposphere. During the ATom-1 deployment, OH reactivity (OHR) below 3 km is significantly enhanced, and this is not captured by the sum of its measured components (cOHRobs) or by the model (cOHRmod). This enhancement could suggest missing reactive VOCs but cannot be explained by new estimates of ocean VOC sources and additional modeled reactivity in this region would be difficult to reconcile with the full suite of ATom measurement constraints. The model generally reproduces the magnitude and seasonality of cOHRobs but underestimates the contribution of oxygenated VOC, mainly acetaldehyde, which is severely underestimated throughout the troposphere despite its calculated lifetime of less than a day. Missing model acetaldehyde in previous studies was attributed to measurement uncertainties that have been largely resolved. Observations of peroxyacetic acid (PAA) provide new support for remote levels of acetaldehyde. The underestimate in modeled acetaldehyde and PAA is present throughout the year in both hemispheres and peaks during Northern Hemisphere summer. The addition of ocean VOC sources in the model increases annual surface cOHRmod by 10 % and improves model-measurement agreement for acetaldehyde particularly in winter but cannot resolve the model summertime bias. Doing so would require a 100 Tg yr−1 source of a long-lived unknown precursor throughout the year with significant additional emissions in the Northern Hemisphere summer. Improving the model bias for remote acetaldehyde and PAA is unlikely to fully resolve previously reported model global biases in OH and methane lifetime, suggesting that future work should examine the sources and sinks of OH over land.
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- 2020
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13. Methane emissions from natural gas infrastructure and use in the urban region of Boston, Massachusetts
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McKain, Kathryn, Down, Adrian, Racitie, Steve M., Budney, John, Hutyra, Lucy R., Floerchinger, Cody, Herndon, Scott C., Nehrkorn, Thomas, Zahniser, Mark S., Jackson, Robert B., Phillips, Nathan, and Wofsy, Steven C.
- Published
- 2015
14. Chapter 13 - Aircraft vertical profile measurements for evaluation of satellite retrievals of long-lived trace gases
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Kort, Eric A. and McKain, Kathryn
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- 2023
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15. Quantification of regional terrestrial biosphere CO2 flux errors in v10 OCO-2 MIP models using airborne measurements.
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Jeongmin Yun, Junjie Liu, Byrne, Brendan, Weir, Brad, Ott, Lesley E., McKain, Kathryn, Baier, Bianca, and Gatti, Luciana V.
- Abstract
Multi-inverse modeling inter-comparison projects (MIPs) provide a chance to assess the uncertainties in inversion estimates arising from various sources such as atmospheric CO
2 observations, transport models, and prior fluxes. However, accurately quantifying ensemble CO2 flux errors remains challenging, often relying on the ensemble spread as a surrogate. This study proposes a method to quantify the errors of regional terrestrial biosphere CO2 flux estimates from 10 inverse models within the Orbiting Carbon Observatory-2 (OCO-2) MIP by using independent airborne CO2 measurements for the period 2015-2017. We first calculate the root-mean-square error (RMSE) between the ensemble mean of posterior CO2 concentration estimates and airborne observations and then isolate the CO2 concentration error caused solely by the ensemble mean of posterior terrestrial biosphere CO2 flux estimates by subtracting the errors of observation and transport in seven regions. Our analysis reveals significant regional variations in the average monthly RMSE over three years, ranging from 0.90 to 2.04 ppm. The ensemble flux error projected into CO2 space is a major component that accounts for 58-84% of the mean RMSE. We further show that in five regions, the observation-based error estimates exceed the atmospheric CO2 errors computed from the ensemble spread of posterior CO2 flux estimates by 1.37-1.89 times, implying an underestimation of the actual ensemble flux error, while their magnitudes are comparable in two regions. By identifying the most sensitive areas to airborne measurements through adjoint sensitivity analysis, we find that the underestimation of flux errors is prominent in eastern parts of Australia and East Asia, western parts of Europe and Southeast Asia, and midlatitude North America, suggesting the presence of systematic biases related to anthropogenic CO2 emissions in inversion estimates. The regions with no underestimation were southeastern Alaska and northeastern South America. Our study emphasizes the value of independent airborne measurements not only for the overall evaluation of inversion performance but also for quantifying regional errors in ensemble terrestrial biosphere flux estimates. [ABSTRACT FROM AUTHOR]- Published
- 2023
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16. Quantification of regional terrestrial biosphere CO2 flux errors in v10 OCO-2 MIP models using airborne measurements.
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Yun, Jeongmin, Liu, Junjie, Byrne, Brendan, Weir, Brad, Ott, Lesley E., McKain, Kathryn, Baier, Bianca, and Gatti, Luciana V.
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MEASUREMENT errors ,BIOSPHERE ,AREA measurement ,SENSITIVITY analysis ,ORBITS (Astronomy) - Abstract
Multi-inverse modeling inter-comparison projects (MIPs) provide a chance to assess the uncertainties in inversion estimates arising from various sources such as atmospheric CO
2 observations, transport models, and prior fluxes. However, accurately quantifying ensemble CO2 flux errors remains challenging, often relying on the ensemble spread as a surrogate. This study proposes a method to quantify the errors of regional terrestrial biosphere CO2 flux estimates from 10 inverse models within the Orbiting Carbon Observatory-2 (OCO-2) MIP by using independent airborne CO2 measurements for the period 2015–2017. We first calculate the root-mean-square error (RMSE) between the ensemble mean of posterior CO2 concentration estimates and airborne observations and then isolate the CO2 concentration error caused solely by the ensemble mean of posterior terrestrial biosphere CO2 flux estimates by subtracting the errors of observation and transport in seven regions. Our analysis reveals significant regional variations in the average monthly RMSE over three years, ranging from 0.90 to 2.04 ppm. The ensemble flux error projected into CO2 space is a major component that accounts for 58–84 % of the mean RMSE. We further show that in five regions, the observation-based error estimates exceed the atmospheric CO2 errors computed from the ensemble spread of posterior CO2 flux estimates by 1.37–1.89 times, implying an underestimation of the actual ensemble flux error, while their magnitudes are comparable in two regions. By identifying the most sensitive areas to airborne measurements through adjoint sensitivity analysis, we find that the underestimation of flux errors is prominent in eastern parts of Australia and East Asia, western parts of Europe and Southeast Asia, and midlatitude North America, suggesting the presence of systematic biases related to anthropogenic CO2 emissions in inversion estimates. The regions with no underestimation were southeastern Alaska and northeastern South America. Our study emphasizes the value of independent airborne measurements not only for the overall evaluation of inversion performance but also for quantifying regional errors in ensemble terrestrial biosphere flux estimates. [ABSTRACT FROM AUTHOR]- Published
- 2023
- Full Text
- View/download PDF
17. Application of the Multi-Scale Infrastructure for Chemistry and Aerosols version 0 (MUSICAv0) for air quality research in Africa.
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Tang, Wenfu, Emmons, Louisa K., Worden, Helen M., Kumar, Rajesh, He, Cenlin, Gaubert, Benjamin, Zheng, Zhonghua, Tilmes, Simone, Buchholz, Rebecca R., Martinez-Alonso, Sara-Eva, Granier, Claire, Soulie, Antonin, McKain, Kathryn, Daube, Bruce C., Peischl, Jeff, Thompson, Chelsea, and Levelt, Pieternel
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MODIS (Spectroradiometer) ,AIR quality ,TROPOSPHERIC chemistry ,ATMOSPHERIC chemistry ,AEROSOLS ,CHEMICAL models ,TROPOSPHERIC aerosols - Abstract
The Multi-Scale Infrastructure for Chemistry and Aerosols Version 0 (MUSICAv0) is a new community modeling infrastructure that enables the study of atmospheric composition and chemistry across all relevant scales. We develop a MUSICAv0 grid with Africa refinement (∼ 28 km × 28 km over Africa). We evaluate the MUSICAv0 simulation for 2017 with in situ observations and compare the model results to satellite products over Africa. A simulation from the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), a regional model that is widely used in Africa studies, is also included in the analyses as a reference. Overall, the performance of MUSICAv0 is comparable to WRF-Chem. Both models underestimate carbon monoxide (CO) compared to in situ observations and satellite CO column retrievals from the Measurements of Pollution in the Troposphere (MOPITT) satellite instrument. MUSICAv0 tends to overestimate ozone (O3), likely due to overestimated stratosphere-to-troposphere flux of ozone. Both models significantly underestimate fine particulate matter (PM2.5) at two surface sites in East Africa. The MUSICAv0 simulation agrees better with aerosol optical depth (AOD) retrievals from the Moderate Resolution Imaging Spectroradiometer (MODIS) and tropospheric nitrogen dioxide (NO2) column retrievals from the Ozone Monitoring Instrument (OMI) than WRF-Chem. MUSICAv0 has a consistently lower tropospheric formaldehyde (HCHO) column than OMI retrievals. Based on model–satellite discrepancies between MUSICAv0 and WRF-Chem and MOPITT CO , MODIS AOD, and OMI tropospheric NO2 , we find that future field campaign(s) and more in situ observations in the East African region (5 ∘ S–5 ∘ N, 30–45 ∘ E) could substantially improve the predictive skill of atmospheric chemistry model(s). This suggested focus region exhibits the largest model–in situ observation discrepancies, as well as targets for high population density, land cover variability, and anthropogenic pollution sources. [ABSTRACT FROM AUTHOR]
- Published
- 2023
- Full Text
- View/download PDF
18. An observation-based, reduced-form model for oxidation in the remote marine troposphere.
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Baublitz, Colleen B., Fiore, Arlene M., Ludwig, Sarah M., Nicely, Julie M., Wolfe, Glenn M., Murray, Lee T., Commane, Róisín, Prather, Michael J., Anderson, Daniel C., Correa, Gustavo, Duncan, Bryan N., Follette-Cook, Melanie, Westervelt, Daniel M., Bourgeois, Ilann, Brune, William H., Bui, T. Paul, DiGangi, Joshua P., Diskin, Glenn S., Hall, Samuel R., and McKain, Kathryn
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TROPOSPHERE ,PRODUCTION losses ,ARTIFICIAL satellite tracking ,HYDROXYL group ,SPATIAL variation - Abstract
The hydroxyl radical (OH) fuels atmospheric chemical cycling as the main sink for methane and a driver of the formation and loss of many air pollutants, but direct OH observations are sparse. We develop and evaluate an observation-based proxy for short-term, spatial variations in OH (Proxy
OH ) in the remote marine troposphere using comprehensive measurements from the NASA Atmospheric Tomography (ATom) airborne campaign. ProxyOH is a reduced form of the OH steady-state equation representing the dominant OH production and loss pathways in the remote marine troposphere, according to box model simulations of OH constrained with ATom observations. ProxyOH comprises only eight variables that are generally observed by routine ground-or satellite-based instruments. ProxyOH scales linearly with in situ [OH] spatial variations along the ATom flight tracks (median r² = 0.90, interquartile range = 0.80 to 0.94 across 2-km altitude by 20° latitudinal regions). We deconstruct spatial variations in ProxyOH as a first-order approximation of the sensitivity of OH variations to individual terms. Two terms modulate within-region ProxyOH variations--water vapor (H2O) and, to a lesser extent, nitric oxide (NO). This implies that a limited set of observations could offer an avenue for observation-based mapping of OH spatial variations over much of the remote marine troposphere. Both H2 O and NO are expected to change with climate, while NO also varies strongly with human activities. We also illustrate the utility of ProxyOH as a process-based approach for evaluating intermodel differences in remote marine tropospheric OH. [ABSTRACT FROM AUTHOR]- Published
- 2023
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- View/download PDF
19. WRF Simulations of the Urban Circulation in the Salt Lake City Area for CO₂ Modeling
- Author
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Nehrkorn, Thomas, Henderson, John, Leidner, Mark, Mountain, Marikate, Eluszkiewicz, Janusz, Mckain, Kathryn, and Wofsy, Steven
- Published
- 2013
20. Inferring the vertical distribution of CO and CO2 from TCCON total column values using the TARDISS algorithm.
- Author
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Parker, Harrison A., Laughner, Joshua L., Toon, Geoffrey C., Wunch, Debra, Roehl, Coleen M., Iraci, Laura T., Podolske, James R., McKain, Kathryn, Baier, Bianca C., and Wennberg, Paul O.
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ATMOSPHERIC carbon dioxide ,CARBON dioxide ,TRACE gases ,GAS distribution ,CARBON cycle ,CARBON monoxide - Abstract
We describe an approach for determining limited information about the vertical distribution of carbon monoxide (CO) and carbon dioxide (CO2) from total column ground-based Total Carbon Column Observation Network (TCCON) observations. For CO and CO2 , it has been difficult to retrieve information about their vertical distribution from spectral line shapes because of the errors in the spectroscopy and the atmospheric temperature profile that mask the effects of variations in their mixing ratio with altitude. For CO2 the challenge is especially difficult given that these variations are typically 2 % or less. Nevertheless, if sufficient accuracy can be obtained, such information would be highly valuable for evaluation of retrievals from satellites and more generally for improving the estimate of surface sources and sinks of these trace gases. We present here the Temporal Atmospheric Retrieval Determining Information from Secondary Scaling (TARDISS) retrieval algorithm. TARDISS uses several simultaneously obtained total column observations of the same gas from different absorption bands with distinctly different vertical averaging kernels. The different total column retrievals are combined in TARDISS using a Bayesian approach where the weights and temporal covariance applied to the different retrievals include additional constraints on the diurnal variation in the vertical distribution for these gases. We assume that the near-surface part of the column varies rapidly over the course of a day (from surface sources and sinks, for example) and that the upper part of the column has a larger temporal covariance over the course of a day. Using measurements from the five North American TCCON sites, we find that the retrieved lower partial column (between the surface and ∼ 800 hPa) of the CO and CO2 dry mole fractions (DMFs) have slopes of 0.999 ± 0.002 and 1.001 ± 0.003 with respect to lower column DMF from integrated in situ data measured directly from aircraft and in AirCores. The average error for our lower column CO retrieval is 1.51 ppb (∼ 2 %) while the average error for our CO2 retrieval is 5.09 ppm (∼ 1.25 %). Compared with classical line-shape-derived vertical profile retrievals, our algorithm reduces the influence of forward model errors such as imprecision in spectroscopy (line shapes and intensities) and in the instrument line shape. In addition, because TARDISS uses the existing retrieved column abundances from TCCON (which themselves are computationally much less intensive than profile retrieval algorithms), it is very fast and processes years of data in minutes. We anticipate that this approach will find broad application for use in carbon cycle science. [ABSTRACT FROM AUTHOR]
- Published
- 2023
- Full Text
- View/download PDF
21. Application of the Multi-Scale Infrastructure for Chemistry and Aerosols version 0 (MUSICAv0) for air quality in Africa.
- Author
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Wenfu Tang, Emmons, Louisa K., Worden, Helen M., Kumar, Rajesh, He, Cenlin, Gaubert, Benjamin, Zhonghua Zheng, Tilmes, Simone, Buchholz, Rebecca R., Martinez-Alonso, Sara-Eva, Granier, Claire, Soulie, Antonin, McKain, Kathryn, Daube, Bruce C., Peischl, Jeff, Thompson, Chelsea, and Levelt, Pieternel
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TROPOSPHERIC aerosols ,MODIS (Spectroradiometer) ,AIR quality ,ATMOSPHERIC chemistry ,AEROSOLS ,CHEMICAL models - Abstract
The Multi-Scale Infrastructure for Chemistry and Aerosols Version 0 (MUSICAv0) is a new community modeling infrastructure that enables the study of atmospheric composition and chemistry across all relevant scales. We develop a MUSICAv0 grid with Africa refinement (~28 km x 28 km over Africa). We evaluate the MUSICAv0 simulation for 2017 with in situ observations and compare the model results to satellite products over Africa. A simulation from the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), a regional model that is widely used in Africa studies, is also included in the analyses as a reference. Overall, the performance of MUSICAv0 is comparable to WRF-Chem. Both models underestimate carbon monoxide (CO) compared to in situ observations and satellite CO column retrievals from the Measurements of Pollution in the Troposphere (MOPITT) satellite instrument. MUSICAv0 tends to overestimate ozone (O
3 ), likely due to overestimated stratosphere-to-troposphere flux of ozone. Both models significantly underestimate fine particulate matter (PM2.5) at two surface sites in East Africa. The MUSICAv0 simulation agrees better with aerosol optical depth (AOD) retrievals from the Moderate Resolution Imaging Spectroradiometer (MODIS) and tropospheric nitrogen dioxide (NO2) column retrievals from the Ozone Monitoring Instrument (OMI) than WRF-Chem. MUSICAv0 has a consistently lower tropospheric formaldehyde (HCHO) column than OMI retrievals. Based on model-satellite discrepancies between MUSICAv0 and WRF-Chem and MOPITT CO, MODIS AOD, and OMI tropospheric NO2 , we find that future field campaign(s) and more in situ observations in an East African region (30°E - 45°E, 5°S - 5°N) could substantially improve the predictive skill of atmospheric chemistry model(s). This suggested focus region exhibits the largest model-in situ observation discrepancies, as well as targets for high population density, land cover variability, and anthropogenic pollution sources. [ABSTRACT FROM AUTHOR]- Published
- 2023
- Full Text
- View/download PDF
22. Assessment of ground-based atmospheric observations for verification of greenhouse gas emissions from an urban region
- Author
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McKain, Kathryn, Wofsy, Steven C., Nehrkorn, Thomas, Eluszkiewicz, Janusz, Ehleringer, James R., and Stephens, Britton B.
- Published
- 2012
23. H₂O₂ and CH₃OOH (MHP) in the Remote Atmosphere: 1. Global Distribution and Regional Influences
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Allen, Hannah M., Crounse, John D., Kim, Michelle J., Teng, Alexander P., Ray, Eric A., McKain, Kathryn, Sweeney, Colm, and Wennberg, Paul O.
- Abstract
Atmospheric hydroperoxides are a significant component of the atmosphere's oxidizing capacity. Two of the most abundant hydroperoxides, hydrogen peroxide (H₂O₂) and methyl hydroperoxide (MHP, CH₃OOH), were measured in the remote atmosphere using chemical ionization mass spectrometry aboard the NASA DC-8 aircraft during the Atmospheric Tomography Mission. These measurements present a seasonal investigation into the global distribution of these two hydroperoxides, with near pole-to-pole coverage across the Pacific and Atlantic Ocean basins and from the marine boundary layer to the upper troposphere and lower stratosphere. H₂O₂ mixing ratios are highest between 2 and 4 km altitude in the equatorial region of the Atlantic Ocean basin, where they reach global maximums of 3.6–6.5 ppbv depending on season. MHP mixing ratios reach global maximums of 4.3–8.6 ppbv and are highest between 1 and 3 km altitude, but peak in different regions depending on season. A major factor contributing to the global H₂O₂ distribution is the influence of biomass burning emissions in the Atlantic Ocean basin, encountered in all four seasons, where the highest H₂O₂ mixing ratios were found to correlate strongly with increased mixing ratios of the biomass burning tracers hydrogen cyanide (HCN) and carbon monoxide (CO). This biomass burning enhanced H₂O₂ by a factor of 1.3–2.2, on average, in the Atlantic compared with the Pacific Ocean basin.
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- 2022
24. A new algorithm to generate a priori trace gas profiles for the GGG2020 retrieval algorithm.
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Laughner, Joshua L., Roche, Sébastien, Kiel, Matthäus, Toon, Geoffrey C., Wunch, Debra, Baier, Bianca C., Biraud, Sébastien, Chen, Huilin, Kivi, Rigel, Laemmel, Thomas, McKain, Kathryn, Quéhé, Pierre-Yves, Rousogenous, Constantina, Stephens, Britton B., Walker, Kaley, and Wennberg, Paul O.
- Subjects
TRACE gases ,APRIORI algorithm ,FOURIER transform spectrometers ,ATMOSPHERIC transport ,ALGORITHMS ,TIME series analysis - Abstract
Optimal estimation retrievals of trace gas total columns require prior vertical profiles of the gases retrieved to drive the forward model and ensure the retrieval problem is mathematically well posed. For well-mixed gases, it is possible to derive accurate prior profiles using an algorithm that accounts for general patterns of atmospheric transport coupled with measured time series of the gases in questions. Here we describe the algorithm used to generate the prior profiles for GGG2020, a new version of the GGG retrieval that is used to analyze spectra from solar-viewing Fourier transform spectrometers, including the Total Carbon Column Observing Network (TCCON). A particular focus of this work is improving the accuracy of CO2 , CH4 , N2O , HF , and CO across the tropopause and into the lower stratosphere. We show that the revised priors agree well with independent in situ and space-based measurements and discuss the impact on the total column retrievals. [ABSTRACT FROM AUTHOR]
- Published
- 2023
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25. Evaluating Northern Hemisphere Growing Season Net Carbon Flux in Climate Models Using Aircraft Observations.
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Loechli, Morgan, Stephens, Britton B., Commane, Roisin, Chevallier, Frédéric, McKain, Kathryn, Keeling, Ralph F., Morgan, Eric J., Patra, Prabir K., Sargent, Maryann R., Sweeney, Colm, and Keppel‐Aleks, Gretchen
- Subjects
GROWING season ,ATMOSPHERIC models ,CARBON cycle ,ATMOSPHERIC carbon dioxide ,MODEL airplanes ,EFFECT of human beings on climate change ,HETEROTROPHIC respiration - Abstract
Understanding terrestrial ecosystems and their response to anthropogenic climate change requires quantification of land‐atmosphere carbon exchange. However, top‐down and bottom‐up estimates of large‐scale land‐atmosphere fluxes, including the northern extratropical growing season net flux (GSNF), show significant discrepancies. We developed a data‐driven metric for the GSNF using atmospheric carbon dioxide concentration observations collected during the High‐Performance Instrumented Airborne Platform for Environmental Research Pole‐to‐Pole Observations and Atmospheric Tomography Mission flight campaigns. This aircraft‐derived metric is bias‐corrected using three independent atmospheric inversion systems. We estimate the northern extratropical GSNF to be 5.7 ± 0.3 Pg C and use it to evaluate net biosphere productivity from the Coupled Model Intercomparison Project phase 5 and 6 (CMIP5 and CMIP6) models. While the model‐to‐model spread in the GSNF has decreased in the CMIP6 models relative to that of the CMIP5 models, there is still disagreement on the magnitude and timing of seasonal carbon uptake with most models underestimating the GSNF and overestimating the length of the growing season relative to the observations. We also use an emergent constraint approach to estimate annual northern extratropical gross primary productivity to be 56 ± 17 Pg C, heterotrophic respiration to be 25 ± 13 Pg C, and net primary productivity to be 28 ± 12 Pg C. The flux inferred from these aircraft observations provides an additional constraint on large‐scale gross fluxes in prognostic Earth system models that may ultimately improve our ability to accurately predict carbon‐climate feedbacks. Plain Language Summary: The exchange of carbon between the land and atmosphere is an important part of the Earth's climate, and this exchange might change due to human‐caused climate change. However, estimates of land‐atmosphere carbon fluxes made using different techniques do not agree with each other. We use atmospheric carbon dioxide observations collected during two flight campaigns to show that 5.7 Pg C is exchanged between the atmosphere and the land in the northern hemisphere during the summer growing season. This estimate is used to evaluate the performance of two generations of climate prediction models. The newer generation of models show less spread than the older generation, but there is still significant disagreement on the magnitude and timing of land‐atmosphere carbon exchange among models. Most models underestimate the growing season net flux and overestimate the length of the growing season. We also use our observational estimate to reduce the spread on component fluxes of carbon exchange, namely uptake by photosynthesis and release by respiration. Key Points: Aircraft observations of atmospheric carbon dioxide concentrations are used to infer the net flux of the northern extratropical growing season net fluxThe observations suggest a larger net flux and shorter growing season than those simulated in Earth system modelsAn emergent constraint approach is used to estimate productivity and respiration fluxes [ABSTRACT FROM AUTHOR]
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- 2023
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26. Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements – corrected.
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Guo, Hao, Flynn, Clare M., Prather, Michael J., Strode, Sarah A., Steenrod, Stephen D., Emmons, Louisa, Lacey, Forrest, Lamarque, Jean-Francois, Fiore, Arlene M., Correa, Gus, Murray, Lee T., Wolfe, Glenn M., St. Clair, Jason M., Kim, Michelle, Crounse, John, Diskin, Glenn, DiGangi, Joshua, Daube, Bruce C., Commane, Roisin, and McKain, Kathryn
- Subjects
TROPOSPHERIC aerosols ,CHEMICAL models ,TROPOSPHERIC chemistry ,TROPOSPHERE ,PEROXYACETYL nitrate ,CHEMICAL species ,HETEROGENEITY - 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 O 3 and CH 4 (O 3 , CH 4 , CO, H 2 O, HCHO, H 2 O 2 , CH 3 OOH, C 2 H 6 , higher alkanes, alkenes, aromatics, NO x , HNO 3 , HNO 4 , peroxyacetyl nitrate, and other organic nitrates), consisting of 146 494 distinct air parcels from ATom deployments 1 through 4. Six models calculated the O 3 and CH 4 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 O 3 and CH 4. Models distinctly underestimate O 3 production below 2 km relative to the mid-troposphere, and this can be traced to lower NO x 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 10.5194/acp-21-13729-2021. [ABSTRACT FROM AUTHOR]
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- 2023
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27. TROPESS/CrIS carbon monoxide profile validation with NOAA GML and ATom in situ aircraft observations.
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Worden, Helen M., Francis, Gene L., Kulawik, Susan S., Bowman, Kevin W., Cady-Pereira, Karen, Fu, Dejian, Hegarty, Jennifer D., Kantchev, Valentin, Luo, Ming, Payne, Vivienne H., Worden, John R., Commane, Róisín, and McKain, Kathryn
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CARBON monoxide ,TROPOSPHERIC ozone ,COLUMNS ,STANDARD deviations ,WATER vapor ,ATOMS - Abstract
The new single-pixel TROPESS (TRopospheric Ozone and its Precursors from Earth System Sounding) profile retrievals of carbon monoxide (CO) from the Cross-track Infrared Sounder (CrIS) are evaluated using vertical profiles of in situ observations from the National Oceanic and Atmospheric Administration (NOAA) Global Monitoring Laboratory (GML) aircraft program and from the Atmospheric Tomography Mission (ATom) campaigns. The TROPESS optimal estimation retrievals are produced using the MUSES (MUlti-SpEctra, MUlti-SpEcies, MUlti-Sensors) algorithm, which has heritage from retrieval algorithms developed for the EOS/Aura Tropospheric Emission Spectrometer (TES). TROPESS products provide retrieval diagnostics and error covariance matrices that propagate instrument noise as well as the uncertainties from sequential retrievals of parameters such as temperature and water vapor that are required to estimate the carbon monoxide profiles. The validation approach used here evaluates biases in column and profile values as well as the validity of the retrieval error estimates using the mean and variance of the compared satellite and aircraft observations. CrIS–NOAA GML comparisons had biases of 0.6 % for partial column average volume mixing ratios (VMRs) and (2.3, 0.9, -4.5) % for VMRs at (750, 511, 287) hPa vertical levels, respectively, with standard deviations from 9 % to 14 %. CrIS–ATom comparisons had biases of -0.04 % for partial column and (2.2, 0.5, -3.0) % for (750, 511, 287) hPa vertical levels, respectively, with standard deviations from 6 % to 10 %. The reported observational errors for TROPESS/CrIS CO profiles have the expected behavior with respect to the vertical pattern in standard deviation of the comparisons. These comparison results give us confidence in the use of TROPESS/CrIS CO profiles and error characterization for continuing the multi-decadal record of satellite CO observations. [ABSTRACT FROM AUTHOR]
- Published
- 2022
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28. Evaluation of MOPITT and TROPOMI carbon monoxide retrievals using AirCore in situ vertical profiles.
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Martínez-Alonso, Sara, Deeter, Merritt N., Baier, Bianca C., McKain, Kathryn, Worden, Helen, Borsdorff, Tobias, Sweeney, Colm, and Aben, Ilse
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TRACE gases ,CARBON monoxide ,POLLUTION measurement ,COLUMNS ,STRATOSPHERE ,TROPOSPHERE - Abstract
AirCore in situ vertical profiles sample the atmosphere from near the surface to the lower stratosphere, making them ideal for the validation of satellite tropospheric trace gas data. Here we present intercomparison results of AirCore carbon monoxide (CO) measurements with respect to retrievals from MOPITT (Measurements of Pollution In The Troposphere; version 8) and TROPOMI (TROPOspheric Monitoring Instrument), on board the NASA Terra and ESA Sentinel 5-Precursor satellites, respectively. Mean MOPITT/AirCore total column bias values and their standard deviation (0.4 ± 5.5, 1.7 ± 5.6, and 0.7 ± 6.0 for MOPITT thermal-infrared, near-infrared, and multispectral retrievals, respectively; all in %) are similar to results obtained in MOPITT/NOAA aircraft flask data comparisons from this study and from previous validation efforts. MOPITT CO retrievals are systematically validated using in situ vertical profiles from a variety of aircraft campaigns. Because most aircraft vertical profiles do not sample the troposphere's entire vertical extent, they must be extended upwards in order to be usable in validation. Here we quantify, for the first time, the error introduced in MOPITT CO validation by the use of shorter aircraft vertical profiles extended upwards by analyzing validation results of MOPITT with respect to full and truncated AirCore CO vertical profiles. Our results indicate that the error is small, affects mostly upper tropospheric retrievals (at 300 hPa: ∼ 2.6, 0.8, and 3.2 percent points for MOPITT thermal-infrared, near-infrared, and multispectral, respectively), and may have resulted in the overestimation of MOPITT retrieval biases in that region. TROPOMI can retrieve CO under both clear and cloudy conditions. The latter is achieved by quantifying interfering trace gases and parameters describing the cloud contamination of the measurements together with the CO column; then, the reference CO profiles used in the retrieval are scaled based on estimated above-cloud CO rather than on estimated total CO. We use AirCore measurements as the reference to evaluate the error introduced by this approach in cloudy TROPOMI retrievals over land after accounting for TROPOMI's vertical sensitivity to CO (relative bias and its standard deviation = 2.02 % ± 11.13 %). We also quantify the null-space error, which accounts for differences between the shape of TROPOMI reference profiles and that of AirCore measured profiles (for TROPOMI cloudy enull=0.98 % ± 2.32 %). [ABSTRACT FROM AUTHOR]
- Published
- 2022
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29. Using atmospheric observations to quantify annual biogenic carbon dioxide fluxes on the Alaska North Slope.
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Schiferl, Luke D., Watts, Jennifer D., Larson, Erik J. L., Arndt, Kyle A., Biraud, Sébastien C., Euskirchen, Eugénie S., Goodrich, Jordan P., Henderson, John M., Kalhori, Aram, McKain, Kathryn, Mountain, Marikate E., Munger, J. William, Oechel, Walter C., Sweeney, Colm, Yi, Yonghong, Zona, Donatella, and Commane, Róisín
- Subjects
ATMOSPHERIC carbon dioxide ,CARBON dioxide ,CARBON emissions ,GROWING season ,TUNDRAS ,PERMAFROST - Abstract
The continued warming of the Arctic could release vast stores of carbon into the atmosphere from high-latitude ecosystems, especially from thawing permafrost. Increasing uptake of carbon dioxide (CO2) by vegetation during longer growing seasons may partially offset such release of carbon. However, evidence of significant net annual release of carbon from site-level observations and model simulations across tundra ecosystems has been inconclusive. To address this knowledge gap, we combined top-down observations of atmospheric CO2 concentration enhancements from aircraft and a tall tower, which integrate ecosystem exchange over large regions, with bottom-up observed CO2 fluxes from tundra environments and found that the Alaska North Slope is not a consistent net source nor net sink of CO2 to the atmosphere (ranging from -6 to +6 TgCyr-1 for 2012–2017). Our analysis suggests that significant biogenic CO2 fluxes from unfrozen terrestrial soils, and likely inland waters, during the early cold season (September–December) are major factors in determining the net annual carbon balance of the North Slope, implying strong sensitivity to the rapidly warming freeze-up period. At the regional level, we find no evidence of the previously reported large late-cold-season (January–April) CO2 emissions to the atmosphere during the study period. Despite the importance of the cold-season CO2 emissions to the annual total, the interannual variability in the net CO2 flux is driven by the variability in growing season fluxes. During the growing season, the regional net CO2 flux is also highly sensitive to the distribution of tundra vegetation types throughout the North Slope. This study shows that quantification and characterization of year-round CO2 fluxes from the heterogeneous terrestrial and aquatic ecosystems in the Arctic using both site-level and atmospheric observations are important to accurately project the Earth system response to future warming. [ABSTRACT FROM AUTHOR]
- Published
- 2022
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30. Inferring the vertical distribution of CO and CO2 from TCCON total column values using the TARDISS algorithm.
- Author
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Parker, Harrison A., Laughner, Joshua L., Toon, Geoffrey C., Wunch, Debra, Roehl, Coleen M., Iraci, Laura T., Podolske, James R., McKain, Kathryn, Baier, Bianca, and Wennberg, Paul O.
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COLUMNS ,TRACE gases ,TROPOSPHERIC ozone ,ATMOSPHERIC temperature ,GAS distribution ,CARBON monoxide ,CARBON cycle - Abstract
We describe an approach for determining limited information about the vertical distribution of carbon monoxide (CO) and carbon dioxide (CO
2 ) from total column observations from ground-based TCCON observations. For long-lived trace gases, such as CO and CO2 , it has been difficult to retrieve information about their vertical distribution from spectral line shapes in the shortwave infrared (SWIR) spectra because of the large doppler widths at 6000 cm-1, and errors in the spectroscopy and in the atmospheric temperature profile which mask the effects of variations in their mixing ratio with altitude in the troposphere. For CO2 the challenge is especially difficult given that these variations are typically 2% or less. Nevertheless, if sufficient accuracy can be obtained, such information would be highly valuable for evaluation of retrievals from satellites and more generally for improving the estimate of surface sources and sinks of these trace gases. We present here the Temporal Atmospheric Retrieval Determining Information from Secondary Scaling (TARDISS) retrieval algorithm. TARDISS uses several simultaneously obtained total column observations of the same gas from different absorption bands with distinctly different vertical averaging kernels. Since TARDISS avoids spectral re-fitting by ingesting retrieved column abundances, it is very fast and processes years of data in minutes. The different total column retrievals are combined using a Bayesian approach where the weights and temporal covariance applied to the different retrievals include additional constraints on the diurnal variation in the vertical distribution for these gases. We assume that only the near surface is influenced by local sources and sinks, while variations in the distribution in the middle and upper troposphere result primarily from advection that can be independently constrained using reanalysis data about the variation in mid-tropospheric potential temperature. Using measurements from five North American TCCON sites, we find that the retrieved lower partial column (between the surface and ~800 hPa) of the CO and CO2 dry mole fractions (DMF) have slopes of 1.001±0.002 and 1.007±0.002 with respect to lower column DMF from integrated in situ data measured by aircraft and AirCore. The average error for our CO retrieval is 0.857 ppb (~1%) while the average error for our CO2 retrieval is 3.55 ppm (~0.8%). We calculate degrees of freedom from signal of 0.218 per measurement for lower partial column CO on average and of 0.353 per measurement for lower partial column CO2 on average. Compared with classical line-shape-derived vertical profile retrievals, our algorithm reduces the influence of forward model errors such as imprecision in spectroscopy (line shapes and intensities) and in the instrument line shape. We anticipate that this approach will find broad application for use in carbon cycle science. [ABSTRACT FROM AUTHOR]- Published
- 2022
- Full Text
- View/download PDF
31. Evaluation of single-footprint AIRS CH4 profile retrieval uncertainties using aircraft profile measurements
- Author
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Kulawik, Susan S., Worden, John R., Payne, Vivienne H., Fu, Dejian, Wofsy, Steve C., McKain, Kathryn, Sweeney, Colm, Daube Jr., Bruce C., Lipton, Alan, Polonsky, Igor, He, Yuguang, Cady-Pereira, Karen E., Dlugokencky, Edward J., Jacob, Daniel J., and Yin, Yi
- Subjects
TheoryofComputation_MATHEMATICALLOGICANDFORMALLANGUAGES - Abstract
We evaluate the uncertainties of methane optimal estimation retrievals from single-footprint thermal infrared observations from the Atmospheric Infrared Sounder (AIRS). These retrievals are primarily sensitive to atmospheric methane in the mid-troposphere through the lower stratosphere (∼2 to ∼17 km). We compare them to in situ observations made from aircraft during the HIAPER Pole to Pole Observations (HIPPO) and Atmospheric Tomography Mission (ATom) campaigns, and from the NOAA GML aircraft network, between the surface and 5–13 km, across a range of years, latitudes between 60∘ S to 80∘ N, and over land and ocean. After a global, pressure-dependent bias correction, we find that the land and ocean have similar biases and that the reported observation error (combined measurement and interference errors) of ∼27 ppb is consistent with the SD between aircraft and individual AIRS observations. A single observation has measurement (noise related) uncertainty of ∼17 ppb, a ∼20 ppb uncertainty from radiative interferences (e.g., from water or temperature), and ∼30 ppb due to “smoothing error”, which is partially removed when making comparisons to in situ measurements or models in a way that accounts for this regularization. We estimate a 10 ppb validation uncertainty because the aircraft typically did not measure methane at altitudes where the AIRS measurements have some sensitivity, e.g., the stratosphere, and there is uncertainty in the truth that we validate against. Daily averaging only partly reduces the difference between aircraft and satellite observation, likely because of correlated errors introduced into the retrieval from temperature and water vapor. For example, averaging nine observations only reduces the aircraft–model difference to ∼17 ppb vs. the expected ∼10 ppb. Seasonal averages can reduce this ∼17 ppb uncertainty further to ∼10 ppb, as determined through comparison with NOAA aircraft, likely because uncertainties related to radiative effects of temperature and water vapor are reduced when averaged over a season.
- Published
- 2021
32. A new algorithm to generate a priori trace gas pro?les for the GGG2020 retrieval algorithm.
- Author
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Laughner, Joshua L., Roche, Sébastien, Kiel, Matthäus, Toon, Geoffrey C., Wunch, Debra, Baier, Bianca C., Biraud, Sébastien, Chen, Huilin, Kivi, Rigel, Laemmel, Thomas, McKain, Kathryn, Quéhé, Pierre-Yves, Rousogenous, Constantina, Stephens, Britton B., Walker, Kaley, and Wennberg, Paul O.
- Subjects
TRACE gases ,APRIORI algorithm ,FOURIER transform spectrometers ,ATMOSPHERIC transport ,COLUMNS ,ALGORITHMS ,FOURIER transforms - Abstract
Optimal estimation retrievals of trace gas total columns require prior vertical profiles of the gases retrieved to drive the forward model and ensure the retrieval problem is mathematically well-posed. For well-mixed gases, it is possible to derive accurate prior profiles using an algorithm that accounts for general patterns of atmospheric transport coupled with measured time series of the gases in questions. Here we describe the algorithm used to generate the prior profiles for GGG2020, a new version of the GGG retrieval that is used to analyze spectra from solar-viewing Fourier transform spectrometers, including the Total Carbon Column Observing Network (TCCON). A particular focus of this work is improving the description of CO
2 , CH4 , N2 O, HF, and CO in the stratosphere. We show that the revised priors agree well with independent in situ and space-based measurements and improve the total column retrievals. [ABSTRACT FROM AUTHOR]- Published
- 2022
- Full Text
- View/download PDF
33. The MOPITT Version 9 CO product: sampling enhancements and validation.
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Deeter, Merritt, Francis, Gene, Gille, John, Mao, Debbie, Martínez-Alonso, Sara, Worden, Helen, Ziskin, Dan, Drummond, James, Commane, Róisín, Diskin, Glenn, and McKain, Kathryn
- Subjects
CARBON monoxide ,POLLUTION measurement ,TROPOSPHERIC aerosols ,TROPOSPHERE ,NEW product development ,AEROSOLS - Abstract
Characteristics of the Version 9 (V9) MOPITT (Measurements of Pollution in the Troposphere) satellite retrieval product for tropospheric carbon monoxide (CO) are described. The new V9 product includes many CO retrievals over land which, in previous MOPITT product versions, would have been discarded by the cloud detection algorithm. Globally, the number of daytime MOPITT retrievals over land has increased by 30 %–40 % relative to the Version 8 product, although the increase in retrieval coverage exhibits significant geographical variability. Areas benefiting from the improved cloud detection performance include (but are not limited to) source regions often characterized by high aerosol concentrations. The V9 MOPITT product also incorporates a modified calibration strategy for the MOPITT near-infrared (NIR) CO channels, resulting in greater temporal consistency for the NIR-only and thermal-infrared–near-infrared (TIR–NIR) retrieval variants. Validation results based on in situ CO profiles acquired from aircraft in a variety of contexts indicate that retrieval biases for V9 are typically within the range of ± 5 % and are generally comparable to results for the V8 product. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
34. Using atmospheric trace gas vertical profiles to evaluate model fluxes: a case study of Arctic-CAP observations and GEOS simulations for the ABoVE domain.
- Author
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Sweeney, Colm, Chatterjee, Abhishek, Wolter, Sonja, McKain, Kathryn, Bogue, Robert, Conley, Stephen, Newberger, Tim, Hu, Lei, Ott, Lesley, Poulter, Benjamin, Schiferl, Luke, Weir, Brad, Zhang, Zhen, and Miller, Charles E.
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TRACE gases ,ATMOSPHERIC carbon dioxide ,CARBON monoxide ,CARBON dioxide ,MOLE fraction - Abstract
Accurate estimates of carbon–climate feedbacks require an independent means for evaluating surface flux models at regional scales. The altitude-integrated enhancement (AIE) derived from the Arctic Carbon Atmospheric Profiles (Arctic-CAP) project demonstrates the utility of this bulk quantity for surface flux model evaluation. This bulk quantity leverages background mole fraction values from the middle free troposphere, is agnostic to uncertainties in boundary layer height, and can be derived from model estimates of mole fractions and vertical gradients. To demonstrate the utility of the bulk quantity, six airborne profiling surveys of atmospheric carbon dioxide (CO 2), methane (CH 4), and carbon monoxide (CO) throughout Alaska and northwestern Canada between April and November 2017 were completed as part of NASA's Arctic–Boreal Vulnerability Experiment (ABoVE). The Arctic-CAP sampling strategy involved acquiring vertical profiles of CO 2 , CH 4 , and CO from the surface to 5 km altitude at 25 sites around the ABoVE domain on a 4- to 6-week time interval. All Arctic-CAP measurements were compared to a global simulation using the Goddard Earth Observing System (GEOS) modeling system. Comparisons of the AIE bulk quantity from aircraft observations and GEOS simulations of atmospheric CO 2 , CH 4 , and CO highlight the fidelity of the modeled surface fluxes. The model–data comparison over the ABoVE domain reveals that while current state-of-the-art models and flux estimates are able to capture broad-scale spatial and temporal patterns in near-surface CO 2 and CH 4 concentrations, more work is needed to resolve fine-scale flux features that are captured in CO observations. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
35. Contributors
- Author
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Baier, Bianca C., Barnet, Christopher D., Best, Fred A., Blonski, Slawomir, Borg, Lori A., Bourassa, Mark A., Brown, Charlie, Cachorro, Victoria E., Cao, Changyong, Chen, Huilin, Choi, Taeyoung, Ciren, Pubu, Dirksen, Ruud J., Dunion, Jason, Embury, Owen, Esmaili, Rebekah, Foltz, Gregory R., Fujiwara, Masatomo, Garcia, Raymond K., Gentemann, Chelle, Gero, Jonathan, Gibson, Laura, Gilerson, Alexander, Goes, Joaquim, González, Ramiro, Grassotti, Christopher, Gröbner, Julian, Hu, Chuanmin, Hurst, Dale F., Ingleby, Bruce, Kalluri, Satya, Kazadzis, Stelios, Kennedy, John J., Kent, Elizabeth C., Knuteson, Robert O., Kollonige, Debra E., Kondragunta, Shobha, Kort, Eric A., Kouremeti, Natalia, Ladner, Sherwin, Lance, Veronica P., Lee, Yong-Keun, Lee, Zhongping, Liu, Quanhua, Liu, Shuyan, Liu, Yuling, Loveless, Michelle L., Lumpkin, Rick, Mateos, David, McKain, Kathryn, Merchant, Christopher J., Minnett, Peter J., Morris, Vernon R., Nalli, Nicholas R., Oltmans, Samuel, Ondrusek, Michael, Perez, Renellys C., Pettey, Michael, Pryor, Kenneth L., Reale, Anthony, Revercomb, Henry E., Román, Roberto, Shao, Xi, Smirnov, Alexander, Smit, Herman G.J., Smith, Nadia, Smith, Ryan, Smith, William L., Sr., Stauffer, Ryan M., Sun, Bomin, Sweeney, Colm, Taylor, Joseph K., Thompson, Anne M., Tobin, David C., Toledano, Carlos, Tufillaro, Nicholas, Uprety, Sirish, Vömel, Holger, Voss, Kenneth J., Wang, Heshun, Wang, Menghua, Wang, Wenhui, Wei, Jianwei, While, James, Yu, Peng, Yu, Yunyue, and Zhou, Yan
- Published
- 2023
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36. H2O2 and CH3OOH (MHP) in the Remote Atmosphere: 1. Global Distribution and Regional Influences.
- Author
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Allen, Hannah M., Crounse, John D., Kim, Michelle J., Teng, Alexander P., Ray, Eric A., McKain, Kathryn, Sweeney, Colm, and Wennberg, Paul O.
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CHEMICAL ionization mass spectrometry ,SMOKE ,BIOMASS burning ,ATMOSPHERE ,HYDROGEN peroxide - Abstract
Atmospheric hydroperoxides are a significant component of the atmosphere's oxidizing capacity. Two of the most abundant hydroperoxides, hydrogen peroxide (H2O2) and methyl hydroperoxide (MHP, CH3OOH), were measured in the remote atmosphere using chemical ionization mass spectrometry aboard the NASA DC‐8 aircraft during the Atmospheric Tomography Mission. These measurements present a seasonal investigation into the global distribution of these two hydroperoxides, with near pole‐to‐pole coverage across the Pacific and Atlantic Ocean basins and from the marine boundary layer to the upper troposphere and lower stratosphere. H2O2 mixing ratios are highest between 2 and 4 km altitude in the equatorial region of the Atlantic Ocean basin, where they reach global maximums of 3.6–6.5 ppbv depending on season. MHP mixing ratios reach global maximums of 4.3–8.6 ppbv and are highest between 1 and 3 km altitude, but peak in different regions depending on season. A major factor contributing to the global H2O2 distribution is the influence of biomass burning emissions in the Atlantic Ocean basin, encountered in all four seasons, where the highest H2O2 mixing ratios were found to correlate strongly with increased mixing ratios of the biomass burning tracers hydrogen cyanide (HCN) and carbon monoxide (CO). This biomass burning enhanced H2O2 by a factor of 1.3–2.2, on average, in the Atlantic compared with the Pacific Ocean basin. Plain Language Summary: Hydroperoxides, a large class of compounds that contain the R–OOH chemical structure, exist in the gas phase in the atmosphere. These compounds are key to the chemistry of the atmosphere because of the role they play in the atmosphere's ability to process and ultimately remove chemical species. Two of the most abundant atmospheric hydroperoxides were measured as part of the Atmospheric Tomography Mission, which collected samples of the atmosphere over the Pacific and Atlantic Ocean basins far from human influences. This paper presents a summary of the global distribution of these hydroperoxides across the four different seasons (winter, spring, summer, fall) and investigates the role that smoke from large‐scale fires on the continents plays in altering the amount of atmospheric hydroperoxides above the Atlantic Ocean. Key Points: The Atmospheric Tomography Mission provides an unprecedented investigation into the global seasonal distribution of hydroperoxidesChemical Ionization Mass Spectrometry is a sensitive technique for studying hydroperoxides in the remote atmosphereBiomass burning emissions increase H2O2 mixing ratios in the Atlantic Ocean compared to corresponding latitudes in the Pacific Ocean basin [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
37. Carbon Monoxide Emissions from the Washington, DC, and Baltimore Metropolitan Area: Recent Trend and COVID-19 Anomaly.
- Author
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Lopez-Coto, Israel, Xinrong Ren, Karion, Anna, McKain, Kathryn, Sweeney, Colm, Dickerson, Russell R., McDonald, Brian C., Ahn, Doyeon Y., Salawitch, Ross J., Hao He, Shepson, Paul B., and Whetstone, James R.
- Published
- 2022
- Full Text
- View/download PDF
38. Continental-scale contributions to the global CFC-11 emission increase between 2012 and 2017.
- Author
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Hu, Lei, Montzka, Stephen A., Moore, Fred, Hintsa, Eric, Dutton, Geoff, Siso, M. Carolina, Thoning, Kirk, Portmann, Robert W., McKain, Kathryn, Sweeney, Colm, Vimont, Isaac, Nance, David, Hall, Bradley, and Wofsy, Steven
- Subjects
OZONE layer ,VIENNA Convention for the Protection of the Ozone Layer (1985). Protocols, etc., 1987 Sept. 15 ,MOLE fraction ,ATMOSPHERIC methane - Abstract
The detection of increasing global CFC-11 emissions after 2012 alerted society to a possible violation of the Montreal Protocol on Substances that Deplete the Ozone Layer (MP). This alert resulted in parties to the MP taking urgent actions. As a result, atmospheric measurements made in 2019 suggest a sharp decline in global CFC-11 emissions. Despite the success in the detection and mitigation of part of this problem, regions fully responsible for the recent global emission changes in CFC-11 have not yet been identified. Roughly two thirds (60 ± 40 %) of the emission increase between 2008–2012 and 2014–2017 and two thirds (60 ± 30 %) of the decline between 2014–2017 and 2019 were explained by regional emission changes in eastern mainland China. Here, we used atmospheric CFC-11 measurements made from two global aircraft surveys – the HIAPER (High-performance Instrumented Airborne Platform for Environmental Research) Pole-to-Pole Observations (HIPPO) in November 2009–September 2011 and the Atmospheric Tomography Mission (ATom) in August 2016–May 2018, in combination with the global CFC-11 measurements made by the US National Oceanic and Atmospheric Administration during these two periods – to derive global and regional emission changes in CFC-11. Our results suggest Asia accounted for the largest fractions of global CFC-11 emissions in both periods: 43 (37–52) % during November 2009–September 2011 and 57 (49–62) % during August 2016–May 2018. Asia was also primarily responsible for the emission increase between these two periods, accounting for 86 (59–115) % of the global CFC-11 emission rise between the two periods. Besides eastern mainland China, temperate western Asia and tropical Asia also contributed significantly to global CFC-11 emissions during both periods and likely to the global CFC-11 emission increase. The atmospheric observations further provide strong constraints on CFC-11 emissions from North America and Europe, suggesting that each of them accounted for 10 %–15 % of global CFC-11 emissions during the HIPPO period and smaller fractions in the ATom period. For South America, Africa, and Australia, the derived regional emissions had larger dependence on the prior assumptions of emissions and emission changes due to a lower sensitivity of the observations considered here to emissions from these regions. However, significant increases in CFC-11 emissions from southern hemispheric lands were not likely due to the observed increase of north-to-south interhemispheric gradients in atmospheric CFC-11 mole fractions from 2012–2017. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
39. The potential role of organics in new particle formation and initial growth in the remote tropical upper troposphere
- Author
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Kupc, Agnieszka, Williamson, Christina J., Hodshire, Anna L., Kazil, Jan, Ray, Eric, Bui, T. Paul, Dollner, Maximilian, Froyd, Karl D., McKain, Kathryn, Rollins, Andrew, Schill, Gregory P., Thames, Alexander, Weinzierl, Bernadett B., Pierce, Jeffrey R., and Brock, Charles A.
- Subjects
Atmospheric Science ,13. Climate action ,14. Life underwater - Abstract
Global observations and model studies indicate that new particle formation (NPF) in the upper troposphere (UT) and subsequent particles supply 40–60 % of cloud condensation nuclei (CCN) in the lower troposphere, thus affecting the Earth's radiative budget. There are several plausible nucleation mechanisms and precursor species in this atmospheric region, which, in the absence of observational constraints, lead to uncertainties in modeled aerosols. In particular, the type of nucleation mechanism and concentrations of nucleation precursors, in part, determine the spatial distribution of new particles and resulting spatial distribution of CCN from this source. Although substantial advances in understanding NPF have been made in recent years, NPF processes in the UT in pristine marine regions are still poorly understood and are inadequately represented in global models. Here, we evaluate commonly used and state-of-the-art NPF schemes in a Lagrangian box model to assess which schemes and precursor concentrations best reproduce detailed in situ observations. Using measurements of aerosol size distributions (0.003
- Published
- 2020
40. The 2015–2016 Carbon Cycle As Seen from OCO-2 and the Global In Situ Network
- Author
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Crowell, Sean, Baker, David, Schuh, Andrew, Basu, Sourish, Jacobson, Andrew R., Chevallier, Frederic, Liu, Junjie, Deng, Feng, Feng, Liang, Chatterjee, Abhishek, Crisp, David, Eldering, Annmarie, Jones, Dylan B., Mckain, Kathryn, Miller, John, Nassar, Ray, Oda, Tomohiro, O'dell, Christopher, Palmer, Paul I., Schimel, David, Stephens, Britton, and Sweeney, Colm
- Abstract
The Orbiting Carbon Observatory-2 has been on orbit since 2014, and its global coverage holds the potential to reveal new information about the carbon cycle through the use of top-down atmospheric inversion methods combined with column average CO2 retrievals. We employ a large ensemble of atmospheric inversions utilizing different transport models, data assimilation techniques and prior flux distributions in order to quantify the satellite-informed fluxes from OCO-2 Version 7r land observations and their uncertainties at continental scales. Additionally, we use in situ measurements to provide a baseline against which to compare the satellite-constrained results. We find that within ensemble spread, in situ observations and satellite retrievals constrain a similar global total carbon sink of 3.7 ± 0.5 PgC, and 1.5 ± 0.6 PgC per year for global land, for the 2015–2016 annual mean. This agreement breaks down on smaller regions, and we discuss the differences between the experiments. Of particular interest is the difference between the different assimilation constraints in the tropics, with the largest differences occurring in tropical Africa, which could be an indication of the global perturbation from the 2015–2016 El Niño. Evaluation of posterior concentrations using TCCON and aircraft observations gives some limited insight into the quality of the different assimilation constraints, but the lack of such data in the tropics inhibits our ability to make strong conclusions there.
- Published
- 2019
- Full Text
- View/download PDF
41. Validation and error estimation of AIRS MUSES CO profiles with HIPPO, ATom, and NOAA GML aircraft observations.
- Author
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Hegarty, Jennifer D., Cady-Pereira, Karen E., Payne, Vivienne H., Kulawik, Susan S., Worden, John R., Kantchev, Valentin, Worden, Helen M., McKain, Kathryn, Pittman, Jasna V., Commane, Róisín, Daube Jr., Bruce C., and Kort, Eric A.
- Subjects
ATMOSPHERIC carbon monoxide ,ALTITUDE measurements ,STANDARD deviations ,ATOMS ,HIGH cycle fatigue - Abstract
Single-footprint retrievals of carbon monoxide from the Atmospheric Infrared Sounder (AIRS) are evaluated using aircraft in situ observations. The aircraft data are from the HIAPER Pole-to-Pole Observations (HIPPO, 2009–2011), the first three Atmospheric Tomography Mission (ATom, 2016–2017) campaigns, and the National Oceanic and Atmospheric Administration (NOAA) Global Monitoring Laboratory (GML) Global Greenhouse Gas Reference Network aircraft program in years 2006–2017. The retrievals are obtained using an optimal estimation approach within the MUlti-SpEctra, MUlti-SpEcies, MUlti-SEnsors (MUSES) algorithm. Retrieval biases and estimated errors are evaluated across a range of latitudes from the subpolar to tropical regions over both ocean and land points. AIRS MUSES CO profiles were compared with HIPPO, ATom, and NOAA GML aircraft observations with a coincidence of 9 h and 50 km to estimate retrieval biases and standard deviations. Comparisons were done for different pressure levels and column averages, latitudes, day, night, land, and ocean observations. We found mean biases of +6.6±4.6 %, +0.6±3.2 %, and -6.1±3.0 % for three representative pressure levels of 750, 510, and 287 hPa, as well as column average mean biases of 1.4±3.6 %. The mean standard deviations for the three representative pressure levels were 15 %, 11 %, and 12 %, and the column average standard deviation was 9 %. Observation errors (theoretical errors) from the retrievals were found to be broadly consistent in magnitude with those estimated empirically from ensembles of satellite aircraft comparisons, but the low values for these observation errors require further investigation. The GML aircraft program comparisons generally had higher standard deviations and biases than the HIPPO and ATom comparisons. Since the GML aircraft flights do not go as high as the HIPPO and ATom flights, results from these GML comparisons are more sensitive to the choice of method for extrapolation of the aircraft profile above the uppermost measurement altitude. The AIRS retrieval performance shows little sensitivity to surface type (land or ocean) or day or night but some sensitivity to latitude. Comparisons to the NOAA GML set spanning the years 2006–2017 show that the AIRS retrievals are able to capture the distinct seasonal cycles but show a high bias of ∼20% in the lower troposphere during the summer when observed CO mixing ratios are at annual minimum values. The retrieval bias drift was examined over the same years 2006–2017 and found to be small at <0.5%. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
42. The MOPITT Version 9 CO Product: Sampling Enhancements and Validation.
- Author
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Deeter, Merritt, Francis, Gene, Gille, John, Mao, Debbie, Martínez-Alonso, Sara, Worden, Helen, Ziskin, Dan, Drummond, James, Commane, Roísín, Diskin, Glenn, and McKain, Kathryn
- Subjects
CARBON monoxide ,POLLUTION measurement ,TROPOSPHERIC aerosols ,AEROSOLS ,TROPOSPHERE ,NEW product development - Abstract
Characteristics of the Version 9 (V9) MOPITT ("Measurements of Pollution in the Troposphere") satellite retrieval product for tropospheric carbon monoxide (CO) are described. The new V9 product includes many CO retrievals over land which, in previous MOPITT product versions, would have been discarded by the cloud detection algorithm. Globally, the number of daytime MOPITT retrievals over land has increased by 30-40 % relative to the Version 8 product, although the increase in retrieval coverage exhibits significant geographical variability. Areas benefiting from the improved cloud detection performance include (but are not limited to) source regions often characterized by high aerosol concentrations. The V9 MOPITT product also incorporates a modified calibration strategy for the MOPITT near-infrared (NIR) CO channels, resulting in greater temporal consistency for the NIR-only and thermal infrared-near infrared (TIR-NIR) retrieval variants. Validation results based on in-situ CO profiles acquired from aircraft in a variety of contexts indicate that retrieval biases for V9 are typically within the range of ±5 % and are generally comparable to results for the V8 product. [ABSTRACT FROM AUTHOR]
- Published
- 2021
- Full Text
- View/download PDF
43. Strong Southern Ocean carbon uptake evident in airborne observations.
- Author
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Long, Matthew C., Stephens, Britton B., McKain, Kathryn, Sweeney, Colm, Keeling, Ralph F., Kort, Eric A., Morgan, Eric J., Bent, Jonathan D., Chandra, Naveen, Chevallier, Frederic, Commane, Róisín, Daube, Bruce C., Krummel, Paul B., Loh, Zoë, Luijkx, Ingrid T., Munro, David, Patra, Prabir, Peters, Wouter, Ramonet, Michel, and Rödenbeck, Christian
- Published
- 2021
- Full Text
- View/download PDF
44. Methane Growth Rate Estimation and Its Causes in Western Canada Using Satellite Observations.
- Author
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Islam, S. M. Nazrul, Jackson, Peter L., Sweeney, Colm, McKain, Kathryn, Frankenberg, Christian, Aben, Ilse, Parker, Robert J., Boesch, Hartmut, and Wunch, Debra
- Subjects
ATMOSPHERIC methane ,ENERGY industries ,METHANE ,EMISSIONS (Air pollution) - Abstract
In this study, the GOSAT Proxy Retrieval (v9.0) data product of column‐averaged dry‐air mole fractions of atmospheric methane (XCH4) for the period 2009–2019 was analyzed to detect methane (CH4) trends in the three western Canadian provinces where oil and gas development activities have changed significantly over the last decade. Although we found statistically significant increasing XCH4 trends in all subdomains (northeast British Columbia‐NE, Alberta‐AB, southern Saskatchewan‐SK), XCH4 trends are not higher than the background trend (7.25 ± 0.30 ppb/yr) and enhancement trends (ΔXCH4, after removing the background quantity) are not detectable at any subdomain during 2009–2019. For further insight into trends in all subdomains, we divided the whole period (2009–2019) into two shorter periods (2009–2013 and 2014–2019) and estimated trends. We found XCH4 trends are higher than background trends particularly in the AB and SK subdomains during 2009–2013, and their ΔXCH4 trends are positive and also marginally statistically significant. However, we do not find any detectable ΔXCH4 trend if we consider either long‐term (2009–2019) or the second shorter period (2014–2019), suggesting local emission sources are dominating year to year fluctuation. From the source attribution analysis, we found both wetland and oil and gas sectors are controlling the CH4 growth rate in western Canada, but the oil and gas sector is the dominant driver in NE and SK subdomains. We also found the satellite‐based average ΔXCH4 trend (15.43 ± 8.19%/yr) between 2009 and 2013 likely reflects a trend in oil and gas CH4 emissions in AB and SK for the same period. Key Points: Methane growth rate in western Canada was positive during 2009–2013, fluctuated afterward, resulting in an undetectable trend after 2013Methane growth seemed to be related to emissions from oil and gas industriesAverage growth rate (15.43 ± 8.19%/yr) between 2009 and 2013 likely reflects a trend in oil and gas CH4 emissions in western Canada [ABSTRACT FROM AUTHOR]
- Published
- 2021
- Full Text
- View/download PDF
45. Continental-scale contributions to the global CFC-11 emission increase between 2012 and 2017.
- Author
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Lei Hu, Montzka, Stephen A., Moore, Fred, Hintsa, Eric, Dutton, Geoff, Siso, M. Carolina, Thoning, Kirk, Portmann, Robert W., McKain, Kathryn, Sweeney, Colm, Vimont, Isaac, Nance, David, Hall, Bradley, and Wofsy, Steven
- Abstract
The early detection of a global emission increase of CFC-11 after 2012 (Montzka et al., 2018) alerted society to a possible violation of the Montreal Protocol on Substances that Deplete the Ozone Layer (MP). This early alert resulted in parties participating in the MP taking urgent actions (United Nations Environment Programme (UNEP), 2019). As a result, atmospheric measurements made in 2019 suggest a sharp decline in global CFC-11 emissions (Montzka et al., 2021). Despite the success in the early detection and mitigation of some of this problem, regions fully responsible for the recent global emission changes of CFC-11 have not yet been identified. Roughly two thirds (60 ± 40 %) of the emission increase between 2008 - 2012 and 2014 - 2017 and two thirds (60 ± 30 %) of emission decline between 2014 - 2017 and 2019 was explained by regional emission changes in eastern mainland China (Park et al., 2021; Rigby et al., 2019). Here, we used atmospheric CFC-11 measurements made from two global aircraft surveys, the HIAPER Pole-to-Pole Observations (HIPPO) in November 2009 - September 2011 and the Atmospheric Tomography Mission (ATom) in August 2016 - May 2018, in combination with the global CFC- 11 measurements made by the U.S. National Oceanic and Atmospheric Administration during these two periods, to derive global and regional emission changes of CFC-11. Our results suggest Asia accounted for the largest fractions of global CFC-11 emissions in both periods, 43 (37 - 52) % during November 2009 - September 2011 and 57 (49 - 62) % during August 2016 - May 2018. Asia was also primarily responsible for the emission increase between these two periods, accounting for 86 (59 - 115) % of the global CFC-11 emission rise between the two periods. Besides eastern mainland China, we find that temperate western Asia and tropical Asia also contributed significantly to global CFC-11 emissions during both periods and likely to the global CFC-11 emission increase between these periods. Besides Asia, the atmospheric observations also provide strong constraints on CFC-11 emissions from North America and Europe, suggesting that each of them accounted for 10 - 15 % of global CFC-11 emissions during the HIPPO period and smaller fractions in the ATom period. For South America, Africa, and Australia, the derived regional emissions had larger dependence on the prior assumptions of emissions and emission changes, due to a lower sensitivity of the observations considered here to emissions from these regions. However, significant increases in CFC-11 emissions from the southern hemispheric lands were not likely due to the observed increase of north-to-south interhemispheric gradients in atmospheric CFC-11 mole fractions from 2012 to 2017. [ABSTRACT FROM AUTHOR]
- Published
- 2021
- Full Text
- View/download PDF
46. Evaluating consistency between total column CO2 retrievals from OCO-2 and the in situ network over North America: implications for carbon flux estimation.
- Author
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Rastogi, Bharat, Miller, John B., Trudeau, Micheal, Andrews, Arlyn E., Hu, Lei, Mountain, Marikate, Nehrkorn, Thomas, Baier, Bianca, McKain, Kathryn, Mund, John, Guan, Kaiyu, and Alden, Caroline B.
- Subjects
CARBON dioxide ,CARBON cycle ,ATMOSPHERIC transport ,MOLE fraction ,CLIMATE feedbacks ,CARBON - Abstract
Feedbacks between the climate system and the carbon cycle represent a key source of uncertainty in model projections of Earth's climate, in part due to our inability to directly measure large-scale biosphere–atmosphere carbon fluxes. In situ measurements of the CO2 mole fraction from surface flasks, towers, and aircraft are used in inverse models to infer fluxes, but measurement networks remain sparse, with limited or no coverage over large parts of the planet. Satellite retrievals of total column CO2 (XCO2), such as those from NASA's Orbiting Carbon Observatory-2 (OCO-2), can potentially provide unprecedented global information about CO2 spatiotemporal variability. However, for use in inverse modeling, data need to be extremely stable, highly precise, and unbiased to distinguish abundance changes emanating from surface fluxes from those associated with variability in weather. Systematic errors in XCO2 have been identified and, while bias correction algorithms are applied globally, inconsistencies persist at regional and smaller scales that may complicate or confound flux estimation. To evaluate XCO2 retrievals and assess potential biases, we compare OCO-2 v10 retrievals with in situ data-constrained XCO2 simulations over North America estimated using surface fluxes and boundary conditions optimized with observations that are rigorously calibrated relative to the World Meteorological Organization X2007 CO2 scale. Systematic errors in simulated atmospheric transport are independently evaluated using unassimilated aircraft and AirCore profiles. We find that the global OCO-2 v10 bias correction shifts the distribution of retrievals closer to the simulated XCO2 , as intended. Comparisons between bias-corrected and simulated XCO2 reveal differences that vary seasonally. Importantly, the difference between simulations and retrievals is of the same magnitude as the imprint of recent surface flux in the total column. This work demonstrates that systematic errors in OCO-2 v10 retrievals of XCO2 over land can be large enough to confound reliable surface flux estimation and that further improvements in retrieval and bias correction techniques are essential. Finally, we show that independent observations, especially vertical profile data, such as those from the National Oceanic and Atmospheric Administration aircraft and AirCore programs are critical for evaluating errors in both satellite retrievals and carbon cycle models. [ABSTRACT FROM AUTHOR]
- Published
- 2021
- Full Text
- View/download PDF
47. Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements.
- Author
-
Guo, Hao, Flynn, Clare M., Prather, Michael J., Strode, Sarah A., Steenrod, Stephen D., Emmons, Louisa, Lacey, Forrest, Lamarque, Jean-Francois, Fiore, Arlene M., Correa, Gus, Murray, Lee T., Wolfe, Glenn M., St. Clair, Jason M., Kim, Michelle, Crounse, John, Diskin, Glenn, DiGangi, Joshua, Daube, Bruce C., Commane, Roisin, and McKain, Kathryn
- Subjects
CHEMICAL models ,TROPOSPHERIC chemistry ,TROPOSPHERE ,PEROXYACETYL nitrate ,CHEMICAL species ,HETEROGENEITY - 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 O 3 and CH 4 (O 3 , CH 4 , CO, H 2 O, HCHO, H 2 O 2 , CH 3 OOH, C 2 H 6 , higher alkanes, alkenes, aromatics, NO x , HNO 3 , HNO 4 , peroxyacetyl nitrate, other organic nitrates), consisting of 146 494 distinct air parcels from ATom deployments 1 through 4. Six models calculated the O 3 and CH 4 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. In other words, accurate simulation of the least reactive 50 % of the troposphere is unimportant for global budgets. Surprisingly, the probability densities of species and reactivities averaged on a model scale (100 km) differ only slightly from the 2 km ATom 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 excellent agreement with the loss of O 3 and CH 4 but sharp disagreement with production of O 3. The models sharply underestimate O 3 production below 4 km in both Pacific and Atlantic basins, and this can be traced to lower NO x 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. [ABSTRACT FROM AUTHOR]
- Published
- 2021
- Full Text
- View/download PDF
48. COS-derived GPP relationships with temperature and light help explain high-latitude atmospheric CO2 seasonal cycle amplification.
- Author
-
Lei Hu, Montzka, Stephen A., Kaushik, Aleya, Andrews, Arlyn E., Sweeney, Colm, Miller, John, Baker, Ian T., Denning, Scott, Campbell, Elliott, Shiga, Yoichi P., Tans, Pieter, Siso, M. Carolina, Crotwell, Molly, McKain, Kathryn, Thoning, Kirk, Hall, Bradley, Vimont, Isaac, Elkins, James W., Whelan, Mary E., and Suntharalingam, Parvadha
- Subjects
SEASONS ,SOIL temperature ,CHLOROPHYLL spectra ,CARBON emissions ,TEMPERATURE - Abstract
In the Arctic and Boreal region (ABR) where warming is especially pronounced, the increase of gross primary production (GPP) has been suggested as an important driver for the increase of the atmospheric CO
2 seasonal cycle amplitude (SCA). However, the role of GPP relative to changes in ecosystem respiration (ER) remains unclear, largely due to our inability to quantify these gross fluxes on regional scales. Here, we use atmospheric carbonyl sulfide (COS) measurements to provide observation-based estimates of GPP over the North American ABR. Our annual GPP estimate is 3.6 (2.4 to 5.5) PgC ⋅ y-1 between 2009 and 2013, the uncertainty of which is smaller than the range of GPP estimated from terrestrial ecosystem models (1.5 to 9.8 PgC ⋅ y-1 ). Our COS-derived monthly GPP shows significant correlations in space and time with satellite-based GPP proxies, solar-induced chlorophyll fluorescence, and near-infrared reflectance of vegetation. Furthermore, the derived monthly GPP displays two different linear relationships with soil temperature in spring versus autumn, whereas the relationship between monthly ER and soil temperature is best described by a single quadratic relationship throughout the year. In spring to midsummer, when GPP is most strongly correlated with soil temperature, our results suggest the warming-induced increases of GPP likely exceeded the increases of ER over the past four decades. In autumn, however, increases of ER were likely greater than GPP due to light limitations on GPP, thereby enhancing autumn net carbon emissions. Both effects have likely contributed to the atmospheric CO2 SCA amplification observed in the ABR. [ABSTRACT FROM AUTHOR]- Published
- 2021
- Full Text
- View/download PDF
49. Validation and Error Estimation of AIRS MUSES CO Profiles with HIPPO, ATom and NOAA GML Aircraft Observations.
- Author
-
Hegarty, Jennifer D., Cady-Pereira, Karen E., Payne, Vivienne H., Kulawik, Susan S., Worden, John R., Kantchev, Valentin, Worden, Helen M., McKain, Kathryn, Pittman, Jasna V., Commane, Róisín, Bruce C. Daube Jr., and Kort, Eric A.
- Subjects
ATMOSPHERIC carbon monoxide ,STANDARD deviations ,ALGORITHMS ,ATOMS ,ALTITUDE measurements ,HIGH cycle fatigue - Abstract
Single footprint retrievals of carbon monoxide from the Atmospheric Infrared Sounder (AIRS) are evaluated using aircraft in situ observations. The aircraft data are from the HIAPER Pole-to-Pole (HIPPO, 2009–2011), the first three Atmospheric Tomography Mission (ATom, 2016–2017) campaigns and the National Oceanic and Atmospheric Administration (NOAA) Global Monitoring Laboratory (GML) Global Greenhouse Gas Reference Network Aircraft Program between 2006 - 2017. The retrievals are obtained using an optimal estimation approach within the MUlti-SpEctra, MUlti-SpEcies, MUlti-Sensors (MUSES) algorithm. Retrieval biases and estimated errors are evaluated across a range of latitudes from the sub-polar to tropical regions over both ocean and land points. AIRS MUSES CO profiles were compared with HIPPO, ATom, and NOAA GML aircraft observations with a coincidence of 9 hours and 50 km to estimate retrieval biases and standard deviations. Comparisons were done for different pressure levels and column averages, latitudes, day, night, land, and ocean observations. We find mean biases of + 6.6% +/- 4.6%, +0.6% +/- 3.2%, -6.1% +/- 3.0%, and 1.4% +/- 3.6%, for 750 hPa, 510 hPa, 287 hPa, and the column averages, respectively. The mean standard deviation is 15%, 11%, 12%, and 9% at these same pressure levels, respectively. Observation errors (theoretical errors) from the retrievals were found to be broadly consistent in magnitude with those estimated empirically from ensembles of satellite aircraft comparisons. The GML Aircraft Program comparisons generally had higher standard deviations and biases than the HIPPO and ATom comparisons. Since the GML aircraft flights do not go as high as the HIPPO and ATom flights, results from these GML comparisons are more sensitive to the choice of method for extrapolation of the aircraft profile above the uppermost measurement altitude. The AIRS retrieval performance shows little sensitivity to surface type (land or ocean) or day or night but some sensitivity to latitude. Comparisons to the NOAA GML set spanning the years 2006-2017 show that the AIRS retrievals are able to capture the distinct seasonal cycles but show a high bias of ~ 20% in the lower troposphere during the summer when observed CO mixing ratios are at annual minimum values. The retrieval bias drift was examined over the same period and found to be small at < 0.5% over the 2006-2017 time period. [ABSTRACT FROM AUTHOR]
- Published
- 2021
- Full Text
- View/download PDF
50. Calibration and field testing of cavity ring-down laser spectrometers measuring CH4, CO2, and δ13CH4 deployed on towers in the Marcellus Shale region
- Author
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Miles, Natasha L., Martins, Douglas K., Richardson, Scott J., Rella, Christopher W., Arata, Caleb, Lauvaux, Thomas, Davis, Kenneth J., Barkley, Zachary R., McKain, Kathryn, and Sweeney, Colm
- Abstract
Four in situ cavity ring-down spectrometers (G2132-i, Picarro, Inc.) measuring methane dry mole fraction (CH4), carbon dioxide dry mole fraction (CO2), and the isotopic ratio of methane (δ13CH4) were deployed at four towers in the Marcellus Shale natural gas extraction region of Pennsylvania. In this paper, we describe laboratory and field calibration of the analyzers for tower-based applications and characterize their performance in the field for the period January–December 2016. Prior to deployment, each analyzer was tested using bottles with various isotopic ratios, from biogenic to thermogenic source values, which were diluted to varying degrees in zero air, and an initial calibration was performed. Furthermore, at each tower location, three field tanks were employed, from ambient to high mole fractions, with various isotopic ratios. Two of these tanks were used to adjust the calibration of the analyzers on a daily basis. We also corrected for the cross-interference from ethane on the isotopic ratio of methane. Using an independent field tank for evaluation, the standard deviation of 4 h means of the isotopic ratio of methane difference from the known value was found to be 0.26 ‰ δ13CH4. Following improvements in the field tank testing scheme, the standard deviation of 4 h means was 0.11 ‰, well within the target compatibility of 0.2 ‰. Round-robin style testing using tanks with near-ambient isotopic ratios indicated mean errors of −0.14 to 0.03 ‰ for each of the analyzers. Flask to in situ comparisons showed mean differences over the year of 0.02 and 0.08 ‰, for the east and south towers, respectively. Regional sources in this region were difficult to differentiate from strong perturbations in the background. During the afternoon hours, the median differences of the isotopic ratio measured at three of the towers, compared to the background tower, were &minus0.15 to 0.12 ‰ with standard deviations of the 10 min isotopic ratio differences of 0.8 ‰. In terms of source attribution, analyzer compatibility of 0.2 ‰ δ13CH4 affords the ability to distinguish a 50 ppb CH4 peak from a biogenic source (at −60 ‰, for example) from one originating from a thermogenic source (−35 ‰), with the exact value dependent upon the source isotopic ratios. Using a Keeling plot approach for the non-afternoon data at a tower in the center of the study region, we determined the source isotopic signature to be −31.2 ± 1.9 ‰, within the wide range of values consistent with a deep-layer Marcellus natural gas source.
- Published
- 2018
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