Reactive nitrogen in the global upper troposphere from NASA DC8 and MOZAIC aircraft campaigns

Author(s):  
Nana wei ◽  
eloise a. marais ◽  
paul o. wennberg ◽  
hannah m. allen ◽  
john d. crounse ◽  
...  

<p>Reactive nitrogen in the upper troposphere (~8-12 km) impacts global climate, air quality and the oxidizing capacity of the whole troposphere. Here we use aircraft observations from instruments onboard the NASA DC8 aircraft for campaigns from 1997 (SONEX) to the recent ATom campaign (2016-2018) and the MOZAIC commercial aircraft campaign (2003-2005) to address uncertainties in the dynamics of reactive nitrogen (NO<sub>y</sub> = NO<sub>x</sub> + NO<sub>x</sub> reservoir compounds) in the global upper troposphere (UT). Our initial analysis of the DC8 aircraft observations is consistent with previous work in that PAN is the dominant NO<sub>y</sub> component (average: 43%; range: 40-60%), followed by NO<sub>x </sub>(on average, 21%), with smaller contributions (on average, 3.5-12.5%) from pernitric acid (HNO<sub>4</sub>), organonitrate (RONO<sub>2</sub>) and nitric acid (HNO<sub>3</sub>). We go on to compare multiyear mean NO<sub>y</sub> from MOZAIC to the combination of all NASA DC8 campaigns to determine whether we can build a near-global climatology of NO<sub>y</sub> and its components to compare to GEOS-Chem to assess our understanding of these very important atmospheric components.</p>

2020 ◽  
Author(s):  
Eloise Marais ◽  
Joanna Joiner ◽  
Sungyeon Choi

<p>Nitrogen oxides (NO<sub> x</sub> = NO + NO<sub>2</sub>) in the upper troposphere (~10-12 km) are effective at producing ozone in the upper troposphere where ozone is a potent greenhouse gas. Observations of NO<sub>x</sub> in the upper troposphere are limited in time to a few intensive research aircraft campaigns and in space to commercial aircraft campaigns. There are satellite-derived observations of NO<sub>2</sub> in the upper troposphere from the Ozone Monitoring Instrument (OMI), but these are at very coarse resolutions (seasonal, > 2,000 km). The high-resolution Sentinel-5P/TROPOMI instrument offers higher spatial resolution and better cloud-resolving capability than OMI. Here we use synthetic columns of NO<sub>2</sub> from the GEOS-Chem chemical transport model to assess feasibility of deriving NO<sub>2</sub> in the upper troposphere using partial columns of NO<sub>2</sub> above cloudy scenes (the so-called cloud-slicing technique). The model is also used to quantify errors induced by uncertainties in cloud-top height and to determine whether NO<sub>2</sub> over cloudy scenes is representative of all-sky conditions (the "truth"). We find that the cloud-slicing approach is spatially consistent (R =0.5) with the "truth", but with a small (10 pptv) bias in background NO<sub>2</sub>. Cloud-slicing is then applied to TROPOMI total columns of NO<sub>2</sub> to derive near-global observations of NO<sub>2</sub> in the upper troposphere and assessed against the existing OMI products and aircraft observations from NASA DC8 aircraft campaigns.</p>


2019 ◽  
Author(s):  
Matthieu Riva ◽  
Yuzhi Chen ◽  
Zhang, Yue ◽  
Ziying Lei ◽  
Nicole Olson ◽  
...  

<div>Acid-driven multiphase chemistry of isoprene epoxydiols (IEPOX), a key isoprene oxidation product, with inorganic sulfate aerosol yields substantial amounts of secondary organic aerosol (SOA) through the formation of organosulfur. The extent and implications of inorganic-to-organic sulfate conversion, however, are unknown. Herein, we reveal that extensive consumption of inorganic sulfate occurs, which increases with the IEPOX-to-inorganic sulfate ratio (IEPOX:Sulf<sub>inorg</sub>), as determined by laboratory and field measurements. We further demonstrate that organosulfur greatly modifies critical aerosol properties, such as acidity, morphology, viscosity, and phase state. These new mechanistic insights reveal that changes in SO<sub>2</sub> emissions, especially in isoprene-dominated environments, will significantly alter biogenic SOA physicochemical properties. Consequently, IEPOX:Sulf<sub>inorg</sub> will play a central role in understanding historical climate and determining future impacts of biogenic SOA on global climate and air quality.</div>


2014 ◽  
Vol 53 (6) ◽  
pp. 1416-1432 ◽  
Author(s):  
R. D. Sharman ◽  
L. B. Cornman ◽  
G. Meymaris ◽  
J. Pearson ◽  
T. Farrar

AbstractThe statistical properties of turbulence at upper levels in the atmosphere [upper troposphere and lower stratosphere (UTLS)] are still not well known, partly because of the lack of adequate routine observations. This is despite the obvious benefit that such observations would have for alerting aircraft of potentially hazardous conditions, either in real time or for route planning. To address this deficiency, a research project sponsored by the Federal Aviation Administration has developed a software package that automatically estimates and reports atmospheric turbulence intensity levels (as EDR ≡ ε1/3, where ε is the energy or eddy dissipation rate). The package has been tested and evaluated on commercial aircraft. The amount of turbulence data gathered from these in situ reports is unprecedented. As of January 2014, there are ~200 aircraft outfitted with this system, contributing to over 137 million archived records of EDR values through 2013, most of which were taken at cruise levels of commercial aircraft, that is, in the UTLS. In this paper, techniques used for estimating EDR are outlined and comparisons with pilot reports from the same or nearby aircraft are presented. These reports allow calibration of EDR in terms of traditionally reported intensity categories (“light,” “moderate,” or “severe”). The results of some statistical analyses of EDR values are also presented. These analyses are restricted to the United States for now, but, as this program is expanded to international carriers, such data will begin to become available over other areas of the globe.


2021 ◽  
Author(s):  
Andreas Petzold ◽  
Valerie Thouret ◽  
Christoph Gerbig ◽  
Andreas Zahn ◽  
Martin Gallagher ◽  
...  

&lt;p&gt;IAGOS (www.iagos.org) is a European Research Infrastructure using commercial aircraft (Airbus A340, A330, and soon A350) for automatic and routine measurements of atmospheric composition including reactive gases (ozone, carbon monoxide, nitrogen oxides, volatile organic compounds), greenhouse gases (water vapour, carbon dioxide, methane), aerosols and cloud particles along with essential thermodynamic parameters. The main objective of IAGOS is to provide the most complete set of high-quality essential climate variables (ECV) covering several decades for the long-term monitoring of climate and air quality. The observations are stored in the IAGOS data centre along with added-value products to facilitate the scientific interpretation of the data. IAGOS began as two European projects, MOZAIC and CARIBIC, in the early 1990s. These projects demonstrated that commercial aircraft are ideal platforms for routine atmospheric measurements. IAGOS then evolved as a European Research Infrastructure offering a mature and sustainable organization for the benefits of the scientific community and for the operational services in charge of air quality and climate change issues such as the Copernicus Atmosphere Monitoring Services (CAMS) and the Copernicus Climate Change Service (C3S). IAGOS is also a contributing network of the World Meteorological Organization (WMO).&lt;/p&gt; &lt;p&gt;IAGOS provides measurements of numerous chemical compounds which are recorded simultaneously in the critical region of the upper troposphere &amp;#8211; lower stratosphere (UTLS) and geographical regions such as Africa and the mid-Pacific which are poorly sampled by other means. The data are used by hundreds of groups worldwide performing data analysis for climatology and trend studies, model evaluation, satellite validation and the study of detailed chemical and physical processes around the tropopause. IAGOS data also play an important role in the re-assessment of the climate impact of aviation.&lt;/p&gt; &lt;p&gt;Most important in the context of weather-related research, IAGOS and its predecessor programmes provide long-term observations of water vapour and relative humidity with respect to ice in the UTLS as well as throughout the tropospheric column during climb-out and descending phases around airports, now for more than 25 years. The high quality and very good resolution of IAGOS observations of relative humidity over ice are used to better understand the role of water vapour and of ice-supersaturated air masses in the tropopause region and to improve their representation in numerical weather and climate forecasting models. Furthermore, CAMS is using the water vapour vertical profiles in near real time for the continuous validation of the CAMS atmospheric models. &lt;/p&gt;


2011 ◽  
Vol 11 (1) ◽  
pp. 2183-2231 ◽  
Author(s):  
Y. F. Lam ◽  
J. S. Fu ◽  
S. Wu ◽  
L. J. Mickley

Abstract. Simulations of present and future average regional ozone and PM2.5 concentrations over the United States were performed to investigate the potential impacts of global climate change and emissions on regional air quality using CMAQ. Various emissions and climate conditions with different biogenic emissions and domain resolutions were implemented to study the sensitivity of future air quality trends from the impacts of changing biogenic emissions. A comparison of GEOS-Chem and CMAQ was performed to investigate the effect of downscaling on the prediction of future air quality trends. For ozone, the impacts of global climate change are relatively smaller when compared to the impacts of anticipated future emissions reduction, except for the Northeast area, where increasing biogenic emissions due to climate change have stronger positive effects (increases) to the regional ozone air quality. The combination effect from both climate change and emission reductions leads to approximately a 10% or 5 ppbv decrease of the maximum daily average eight-hour ozone (MDA8) over the Eastern United States. For PM2.5, the impacts of global climate change have shown insignificant effect, where as the impacts of anticipated future emissions reduction account for the majority of overall PM2.5 reductions. The annual average 24-h PM2.5 of the future-year condition was found to be about 40% lower than the one from the present-year condition, of which 60% of its overall reductions are contributed to by the decrease of SO4 and NO3 particulate matters. Changing the biogenic emissions model increases the MDA8 ozone by about 5–10% or 3–5 ppbv in the Northeast area. Conversely, it reduces the annual average PM2.5 by 5% or 1.0 μg/m3 in the Southeast region.


2012 ◽  
Vol 117 (D11) ◽  
pp. n/a-n/a ◽  
Author(s):  
Annica M. L. Ekman ◽  
Markus Hermann ◽  
Peter Groß ◽  
Jost Heintzenberg ◽  
Dongchul Kim ◽  
...  

2013 ◽  
Vol 6 (5) ◽  
pp. 1429-1445 ◽  
Author(s):  
M. Trail ◽  
A. P. Tsimpidi ◽  
P. Liu ◽  
K. Tsigaridis ◽  
Y. Hu ◽  
...  

Abstract. Climate change can exacerbate future regional air pollution events by making conditions more favorable to form high levels of ozone. In this study, we use spectral nudging with the Weather Research and Forecasting (WRF) model to downscale NASA earth system GISS modelE2 results during the years 2006 to 2010 and 2048 to 2052 over the contiguous United States in order to compare the resulting meteorological fields from the air quality perspective during the four seasons of five-year historic and future climatological periods. GISS results are used as initial and boundary conditions by the WRF regional climate model (RCM) to produce hourly meteorological fields. The downscaling technique and choice of physics parameterizations used are evaluated by comparing them with in situ observations. This study investigates changes of similar regional climate conditions down to a 12 km by 12 km resolution, as well as the effect of evolving climate conditions on the air quality at major US cities. The high-resolution simulations produce somewhat different results than the coarse-resolution simulations in some regions. Also, through the analysis of the meteorological variables that most strongly influence air quality, we find consistent changes in regional climate that would enhance ozone levels in four regions of the US during fall (western US, Texas, northeastern, and southeastern US), one region during summer (Texas), and one region where changes potentially would lead to better air quality during spring (Northeast). Changes in regional climate that would enhance ozone levels are increased temperatures and stagnation along with decreased precipitation and ventilation. We also find that daily peak temperatures tend to increase in most major cities in the US, which would increase the risk of health problems associated with heat stress. Future work will address a more comprehensive assessment of emissions and chemistry involved in the formation and removal of air pollutants.


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