scholarly journals Atmospheric Chemistry Measurements at Whiteface Mountain, NY: Ozone and Reactive Trace Gases

2016 ◽  
Vol 16 (3) ◽  
pp. 873-884 ◽  
Author(s):  
Richard E. Brandt ◽  
James J. Schwab ◽  
Paul W. Casson ◽  
Utpal K. Roychowdhury ◽  
Douglas Wolfe ◽  
...  
2021 ◽  
Author(s):  
Mehliyar Sadiq ◽  
Paul I. Palmer ◽  
Mark F. Lunt ◽  
Liang Feng ◽  
Ingrid Super ◽  
...  

Abstract. We assess how nitrogen oxides (NOx = NO + NO2), carbon monoxide (CO) and formaldehyde (HCHO) can be used as proxies to determine the combustion contribution to atmospheric carbon dioxide (CO2) using satellite observations. We focus our analysis on 2018 when there is a full complement of column data from the TROPOspheric Monitoring Instrument (NO2, CO, and HCHO) and the Orbiting Carbon Observatory-2 (CO2). We use the nested GEOS-Chem atmospheric chemistry model to relate high-resolution emission inventories over Europe to these atmospheric data, taking into account scene-dependent averaging kernels. We find that that NO2 and CO are the better candidates to identify incomplete combustion and fingerprints of different combustion sectors, but both have their own challenges associated with properly describing their atmospheric chemistry. The secondary source of HCHO from oxidation of biogenic volatile organic compounds, particularly over southern European countries, compromises its use as a proxy for combustion emissions. We find a weak positive correlation between the CO : CO2 inventory ratio and observed column enhancements of ΔCO : ΔCO2 (R < 0.2), suggesting some consistency and linearity in CO chemistry and transport. However, we find a stronger negative correlation between the NOx : CO2 inventory ratio and observed column enhancements of ΔNO2 :ΔCO2 (R < 0.50), driven by non-linear photochemistry. Both of these observed ratios are described well by the GEOS-Chem atmospheric chemistry transport model, providing confidence of the quality of the emission inventory and that the model is a useful tool for interpreting these tracer-tracer ratios. Our results also provide some confidence in our ability to develop a robust method to infer combustion CO2 emission estimates using satellite observations of reactive trace gases that have up until now mostly been used to study surface air quality.


2019 ◽  
Vol 16 (9) ◽  
pp. 2003-2031 ◽  
Author(s):  
Philipp Porada ◽  
Alexandra Tamm ◽  
Jose Raggio ◽  
Yafang Cheng ◽  
Axel Kleidon ◽  
...  

Abstract. The reactive trace gases nitric oxide (NO) and nitrous acid (HONO) are crucial for chemical processes in the atmosphere, including the formation of ozone and OH radicals, oxidation of pollutants, and atmospheric self-cleaning. Recently, empirical studies have shown that biological soil crusts are able to emit large amounts of NO and HONO, and they may therefore play an important role in the global budget of these trace gases. However, the upscaling of local estimates to the global scale is subject to large uncertainties, due to unknown spatial distribution of crust types and their dynamic metabolic activity. Here, we perform an alternative estimate of global NO and HONO emissions by biological soil crusts, using a process-based modelling approach to these organisms, combined with global data sets of climate and land cover. We thereby consider that NO and HONO are emitted in strongly different proportions, depending on the type of crust and their dynamic activity, and we provide a first estimate of the global distribution of four different crust types. Based on this, we estimate global total values of 1.04 Tg yr−1 NO–N and 0.69 Tg yr−1 HONO–N released by biological soil crusts. This corresponds to around 20 % of global emissions of these trace gases from natural ecosystems. Due to the low number of observations on NO and HONO emissions suitable to validate the model, our estimates are still relatively uncertain. However, they are consistent with the amount estimated by the empirical approach, which confirms that biological soil crusts are likely to have a strong impact on global atmospheric chemistry via emissions of NO and HONO.


2018 ◽  
Author(s):  
Philipp Porada ◽  
Alexandra Tamm ◽  
Axel Kleidon ◽  
Ulrich Pöschl ◽  
Bettina Weber

Abstract. The reactive trace gases nitric oxide (NO) and nitrous acid (HONO) are crucial for chemical processes in the atmosphere, including the formation of ozone and OH radicals, oxidation of pollutants and atmospheric self-cleaning. Recently, empirical studies showed that biological soil crusts are able to emit large amounts of NO and HONO and they may therefore play an important role in the global budget of these trace gases. However, the upscaling of local estimates to the global scale is subject to large uncertainties, due to unknown spatial distribution of crust types and their dynamic metabolic activity. Here, we perform an alternative estimate of global NO and HONO emissions by biological soil crusts, using a process-based modelling approach to these organisms, combined with global datasets of climate and land cover. We thereby consider that NO and HONO are emitted in strongly different proportions, depending on the type of crust and their dynamic activity, and we provide a first estimate of the global distribution of four different crust types. Based on this, we estimate global total values of 1.04 Tg yr−1 NO-N and 0.69 Tg yr−1 HONO-N released by biological soil crusts. This is consistent with the amount estimated by the empirical approach and confirms that biological soil crusts are likely to have a strong impact on global atmospheric chemistry via emissions of NO and HONO.


2014 ◽  
Vol 14 (10) ◽  
pp. 15645-15682 ◽  
Author(s):  
M. J. Tang ◽  
R. A. Cox ◽  
M. Kalberer

Abstract. Diffusion of gas molecules to the surface is the first step for all gas-surface reactions. Gas phase diffusion can influence and sometimes even limit the overall rates of these reactions; however, there is no database of the gas phase diffusion coefficients of atmospheric reactive trace gases. Here we compile and evaluate, for the first time, the diffusivities (pressure-independent diffusion coefficients) of atmospheric inorganic reactive trace gases reported in the literature. The measured diffusivities are then compared with estimated values using a semi-empirical method developed by Fuller et al. (1966). The diffusivities estimated using Fuller's method are typically found to be in good agreement with the measured values within ±30%, and therefore Fuller's method can be used to estimate the diffusivities of trace gases for which experimental data are not available. The two experimental methods used in the atmospheric chemistry community to measure the gas phase diffusion coefficients are also discussed.


2014 ◽  
Vol 14 (17) ◽  
pp. 9233-9247 ◽  
Author(s):  
M. J. Tang ◽  
R. A. Cox ◽  
M. Kalberer

Abstract. Diffusion of gas molecules to the surface is the first step for all gas–surface reactions. Gas phase diffusion can influence and sometimes even limit the overall rates of these reactions; however, there is no database of the gas phase diffusion coefficients of atmospheric reactive trace gases. Here we compile and evaluate, for the first time, the diffusivities (pressure-independent diffusion coefficients) of atmospheric inorganic reactive trace gases reported in the literature. The measured diffusivities are then compared with estimated values using a semi-empirical method developed by Fuller et al. (1966). The diffusivities estimated using Fuller's method are typically found to be in good agreement with the measured values within ±30%, and therefore Fuller's method can be used to estimate the diffusivities of trace gases for which experimental data are not available. The two experimental methods used in the atmospheric chemistry community to measure the gas phase diffusion coefficients are also discussed. A different version of this compilation/evaluation, which will be updated when new data become available, is uploaded online (https://sites.google.com/site/mingjintang/home/diffusion).


2017 ◽  
Vol 71 (11) ◽  
pp. 778-778
Author(s):  
Céline Pascale ◽  
Daiana Leuenberger ◽  
Myriam Guillevic ◽  
Andreas Ackermann ◽  
Bernhard Niederhauser

2021 ◽  
Author(s):  
Roland Potthast ◽  
Wolfgang Müller ◽  
Barbara Früh ◽  
Peter Korn ◽  
Susanne Brienen ◽  
...  

&lt;p&gt;ICON-seamless entwickelt ein neues Erdsystemmodell, als Grundlage f&amp;#252;r Wettervorhersage, saisonale und dekadische Klimavorhersagen, bis hin zu Klimaprojektionen. Dabei nutzen wir die Expertise, die ICON-NWV als zuverl&amp;#228;ssiges Modell f&amp;#252;r numerische Wettervorhersage (NWV) betreibt und pflegt sowie die Erfahrungen mit der ersten ICON-Erdsystemversion basierend auf der Physik der MPI-Atmosph&amp;#228;re ECHAM. Das Ziel ist, gemeinsame Komponenten f&amp;#252;r alle meteorologischen Zeitskalen nutzen zu k&amp;#246;nnen. Der erste Schritt entwickelt ein Modell f&amp;#252;r saisonale und dekadische Zeitskalen.&lt;/p&gt; &lt;p&gt;ICON-seamless baut auf der Kopplung der Komponenten ICON-NWV (Atmosph&amp;#228;re) und ICON-O (Ozean) auf. Mit Hilfe des speziell entwickelten Kopplungs-Tools YAC k&amp;#246;nnen beide Komponenten Variablen austauschen, die f&amp;#252;r die Wechselwirkung zwischen Atmosph&amp;#228;re und Ozean wichtig sind. Auch die Parametrisierung von Meereis stellt einen wichtigen Baustein dar. Zur Wiedergabe eines geschlossenen hydrologischen Kreislaufs und um den Kohlenstoffkreislauf sauber darzustellen, wird ferner ein geeignetes Bodenmodell, ICON-L, an die Atmosph&amp;#228;renphysik von ICON-NWV gekoppelt. Zudem werden transiente Aerosolfelder, Treibhausgase, und Strahlungsantriebe neu in ICON-NWV eingelesen, um historische Zeitr&amp;#228;ume nachzuvollziehen. Parallel hierzu werden die ART Module (Aerosol and Reactive Trace gases), die eine dynamische Behandlung von Gasen und Aerosolen gestatten, an die modifizierte Modellphysik angepasst. Eine intensive Modelldiagnostik unterst&amp;#252;tzt das Tuning. F&amp;#252;r die zuk&amp;#252;nftige Verwendung im Bereich der (Wetter- und) Klimavorhersagen wird parallel die gekoppelte Datenassimilation entwickelt.&lt;/p&gt; &lt;p&gt;Wir geben einen &amp;#220;berblick &amp;#252;ber den aktuellen Stand der Entwicklung, der Experimente und potentieller Anwendungsbereiche.&lt;/p&gt;


2017 ◽  
Vol 17 (18) ◽  
pp. 11521-11539 ◽  
Author(s):  
Stefan Lossow ◽  
Hella Garny ◽  
Patrick Jöckel

Abstract. The amplitude of the annual variation in water vapour exhibits a distinct isolated maximum in the middle and upper stratosphere in the southern tropics and subtropics, peaking typically around 15° S in latitude and close to 3 hPa (∼  40.5 km) in altitude. This enhanced annual variation is primarily related to the Brewer–Dobson circulation and hence also visible in other trace gases. So far this feature has not gained much attention in the literature and the present work aims to add more prominence. Using Envisat/MIPAS (Environmental Satellite/Michelson Interferometer for Passive Atmospheric Sounding) observations and ECHAM/MESSy (European Centre for Medium-Range Weather Forecasts Hamburg/Modular Earth Submodel System) Atmospheric Chemistry (EMAC) simulations we provide a dedicated illustration and a full account of the reasons for this enhanced annual variation.


2020 ◽  
Vol 101 (10) ◽  
pp. E1820-E1841
Author(s):  
Sara Lance ◽  
Jie Zhang ◽  
James J. Schwab ◽  
Paul Casson ◽  
Richard E. Brandt ◽  
...  

AbstractAqueous chemical processing within cloud and fog water is thought to be a key process in the production and transformation of secondary organic aerosol mass, found abundantly and ubiquitously throughout the troposphere. Yet, significant uncertainty remains regarding the organic chemical reactions taking place within clouds and the conditions under which those reactions occur, owing to the wide variety of organic compounds and their evolution under highly variable conditions when cycled through clouds. Continuous observations from a fixed remote site like Whiteface Mountain (WFM) in New York State and other mountaintop sites have been used to unravel complex multiphase interactions in the past, particularly the conversion of gas-phase emissions of SO2 to sulfuric acid within cloud droplets in the presence of sunlight. These scientific insights led to successful control strategies that reduced aerosol sulfate and cloud water acidity substantially over the following decades. This paper provides an overview of observations obtained during a pilot study that took place at WFM in August 2017 aimed at obtaining a better understanding of Chemical Processing of Organic Compounds within Clouds (CPOC). During the CPOC pilot study, aerosol cloud activation efficiency, particle size distribution, and chemical composition measurements were obtained below-cloud for comparison to routine observations at WFM, including cloud water composition and reactive trace gases. Additional instruments deployed for the CPOC pilot study included a Doppler lidar, sun photometer, and radiosondes to assist in evaluating the meteorological context for the below-cloud and summit observations.


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