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The availability of formaldehyde (HCHO) (a proxy for volatile organic compound reactivity) and nitrogen dioxide (NO 2) (a proxy for nitrogen oxides) tropospheric columns from ultraviolet–visible (UV–Vis) satellites has motivated many to use their ratios to gain some insights into the near-surface ozone sensitivity. Strong emphasis has been placed on the challenges that come with transforming what is being observed in the tropospheric column to what is actually in the planetary boundary layer (PBL) and near the surface; however, little attention has been paid to other sources of error such as chemistry, spatial representation, and retrieval uncertainties. Here we leverage a wide spectrum of tools and data to quantify those errors carefully. Concerning the chemistry error, a well-characterized box model constrained by more than 500 h of aircraft data from NASA's air quality campaigns is used to simulate the ratio of the chemical loss of HO 2 + RO 2 (LROx) to the chemical loss of NO x (LNOx). Subsequently, we challenge the predictive power of HCHO/NO2 ratios (FNRs), which are commonly applied in current research, in detecting the underlying ozone regimes by comparing them to LROx/LNOx. FNRs show a strongly linear (R2=0.94) relationship with LROx/LNOx , but only on the logarithmic scale. Following the baseline (i.e., ln(LROx/LNOx) = - 1.0 ± 0.2) with the model and mechanism (CB06, r2) used for segregating NOx -sensitive from VOC-sensitive regimes, we observe a broad range of FNR thresholds ranging from 1 to 4. The transitioning ratios strictly follow a Gaussian distribution with a mean and standard deviation of 1.8 and 0.4, respectively. This implies that the FNR has an inherent 20 % standard error (1σ) resulting from not accurately describing the ROx – HOx cycle. We calculate high ozone production rates (PO 3) dominated by large HCHO × NO 2 concentration levels, a new proxy for the abundance of ozone precursors. The relationship between PO 3 and HCHO × NO 2 becomes more pronounced when moving towards NOx -sensitive regions due to nonlinear chemistry; our results indicate that there is fruitful information in the HCHO × NO 2 metric that has not been utilized in ozone studies. The vast amount of vertical information on HCHO and NO 2 concentrations from the air quality campaigns enables us to parameterize the vertical shapes of FNRs using a second-order rational function permitting an analytical solution for an altitude adjustment factor to partition the tropospheric columns into the PBL region. We propose a mathematical solution to the spatial representation error based on modeling isotropic semivariograms. Based on summertime-averaged data, the Ozone Monitoring Instrument (OMI) loses 12 % of its spatial information at its native resolution with respect to a high-resolution sensor like the TROPOspheric Monitoring Instrument (TROPOMI) (> 5.5 × 3.5 km 2). A pixel with a grid size of 216 km 2 fails at capturing ∼ 65 % of the spatial information in FNRs at a 50 km length scale comparable to the size of a large urban center (e.g., Los Angeles). We ultimately leverage a large suite of in situ and ground-based remote sensing measurements to draw the error distributions of daily TROPOMI and OMI tropospheric NO 2 and HCHO columns. At a 68 % confidence interval (1σ), errors pertaining to daily TROPOMI observations, either HCHO or tropospheric NO 2 columns, should be above 1.2–1.5 × 10 16 molec. cm -2 to attain a 20 %–30 % standard error in the ratio. This level of error is almost non-achievable with the OMI given its large error in HCHO. The satellite column retrieval error is the largest contributor to the total error (40 %–90 %) in the FNRs. Due to a stronger signal in cities, the total relative error (< 50 %) tends to be mild, whereas areas with low vegetation and anthropogenic sources (e.g., the Rocky Mountains) are markedly uncertain (> 100 %). Our study suggests that continuing development in the retrieval algorithm and sensor design and calibration is essential to be able to advance the application of FNRs beyond a qualitative metric. [ABSTRACT FROM AUTHOR]

NASA's Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ, conducted in 2011–2014) campaign in the United States and the joint NASA and National Institute of Environmental Research (NIER) Korea–United States Air Quality Study (KORUS-AQ, conducted in 2016) in South Korea were two field study programs that provided comprehensive, integrated datasets of airborne and surface observations of atmospheric constituents, including nitrogen dioxide (NO2), with the goal of improving the interpretation of spaceborne remote sensing data. Various types of NO2 measurements were made, including in situ concentrations and column amounts of NO2 using ground- and aircraft-based instruments, while NO2 column amounts were being derived from the Ozone Monitoring Instrument (OMI) on the Aura satellite. This study takes advantage of these unique datasets by first evaluating in situ data taken from two different instruments on the same aircraft platform, comparing coincidentally sampled profile-integrated columns from aircraft spirals with remotely sensed column observations from ground-based Pandora spectrometers, intercomparing column observations from the ground (Pandora), aircraft (in situ vertical spirals), and space (OMI), and evaluating NO2 simulations from coarse Global Modeling Initiative (GMI) and high-resolution regional models. We then use these data to interpret observed discrepancies due to differences in sampling and deficiencies in the data reduction process. Finally, we assess satellite retrieval sensitivity to observed and modeled a priori NO2 profiles. Contemporaneous measurements from two aircraft instruments that likely sample similar air masses generally agree very well but are also found to differ in integrated columns by up to 31.9 %. These show even larger differences with Pandora, reaching up to 53.9 %, potentially due to a combination of strong gradients in NO2 fields that could be missed by aircraft spirals and errors in the Pandora retrievals. OMI NO2 values are about a factor of 2 lower in these highly polluted environments due in part to inaccurate retrieval assumptions (e.g., a priori profiles) but mostly to OMI's large footprint (>312 km 2). [ABSTRACT FROM AUTHOR]

NASA's Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign in the United States and the joint NASA and National Institute of Environmental Research (NIER) Korea-United States Air Quality Study (KORUS-AQ) in South Korea were two field study programs that provided comprehensive, integrated datasets of airborne and surface observations of atmospheric constituents, including nitrogen dioxide (NO2), with a goal of improving the interpretation of spaceborne remote sensing data. Various types of NO2 measurements were made, including in situ concentrations and column amounts of NO2 using ground- and aircraft-based instruments, while NO2 column amounts were being derived from the Ozone Monitoring Instrument (OMI) on the Aura satellite. This study takes advantage of these unique data sets by first evaluating in situ data taken from two different instruments on the same aircraft platform, comparing coincidently sampled profile-integrated columns from aircraft spirals with remotely sensed column observations from ground-based Pandora spectrometers, intercomparing column observations from the ground (Pandora), aircraft (in situ vertical spirals), and space (OMI), and evaluating NO2 simulations from coarse Global Modeling Initiative (GMI) and high-resolution regional models. We then use these data to interpret observed discrepancies due to differences in sampling and deficiencies in the data reduction process. Finally, we assess satellite retrieval sensitivity to observed and modeled a-priori NO2 profiles. Contemporaneous measurements from two aircraft instruments that likely sample similar air masses generally agree very well but are also found to differ in integrated columns by up to 33.3%. These show even larger differences with Pandora, reaching up to 53.1%, potentially due to a combination of strong gradients in NO2 fields that could be missed by aircraft spirals and errors in the Pandora retrievals. OMI NO2 values are about a factor of two lower in these highly polluted environments, due in part to inaccurate retrieval assumptions (e.g., a priori profiles), but mostly to OMI's areal (> 312 km²) averaging. [ABSTRACT FROM AUTHOR]

The GEOstationary Coastal and Air Pollution Events (GEO-CAPE) Airborne Simulator (GCAS) was developed in support of NASA's decadal survey GEO-CAPE geostationary satellite mission. GCAS is an airborne push-broom remote-sensing instrument, consisting of two channels which make hyperspectral measurements in the ultraviolet/visible (optimized for air quality observations) and the visible–near infrared (optimized for ocean color observations). The GCAS instrument participated in its first intensive field campaign during the Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) campaign in Texas in September 2013. During this campaign, the instrument flew on a King Air B-200 aircraft during 21 flights on 11 days to make air quality observations over Houston, Texas. We present GCAS trace gas retrievals of nitrogen dioxide (NO2) and formaldehyde (CH2O), and compare these results with trace gas columns derived from coincident in situ profile measurements of NO2 and CH2O made by instruments on a P-3B aircraft, and with NO2 observations from ground-based Pandora spectrometers operating in direct-sun and scattered light modes. GCAS tropospheric column measurements correlate well spatially and temporally with columns estimated from the P-3B measurements for both NO2 (r2=0.89) and CH2O (r2=0.54) and with Pandora direct-sun (r2=0.85) and scattered light (r2=0.94) observed NO2 columns. Coincident GCAS columns agree in magnitude with NO2 and CH2O P-3B-observed columns to within 10 % but are larger than scattered light Pandora tropospheric NO2 columns by 33 % and direct-sun Pandora NO2 columns by 50 %. [ABSTRACT FROM AUTHOR]

An instrumented NASA P-3B aircraft was used for airborne sampling of trace gases in a plume that had emanated from a small forest understory fire in Georgia, USA. The plume was sampled at its origin to derive emission factors and followed ~13.6 km downwind to observe chemical changes during the first hour of atmospheric aging. The P-3B payload included a proton-transfer-reaction timeof- flight mass spectrometer (PTR-ToF-MS), which measured non-methane organic gases (NMOGs) at unprecedented spatiotemporal resolution (10m spatial / 0.1 s temporal). Quantitative emission data are reported for CO2, CO, NO, NO2, HONO, NH3, and 16NMOGs (formaldehyde, methanol, acetonitrile, propene, acetaldehyde, formic acid, acetone plus its isomer propanal, acetic acid plus its isomer glycolaldehyde, furan, isoprene plus isomeric pentadienes and cyclopentene, methyl vinyl ketone plus its isomers crotonaldehyde and methacrolein, methylglyoxal, hydroxy acetone plus its isomers methyl acetate and propionic acid, benzene, 2,3-butanedione, and 2-furfural) with molar emission ratios relative to CO larger than 1 ppbV ppmV-1. Formaldehyde, acetaldehyde, 2-furfural, and methanol dominated NMOG emissions. No NMOGs with more than 10 carbon atoms were observed at mixing ratios larger than 50 pptV ppmV-1 CO. Downwind plume chemistry was investigated using the observations and a 0-D photochemical box model simulation. The model was run on a nearly explicit chemical mechanism (MCM v3.3) and initialized with measured emission data. Ozone formation during the first hour of atmospheric aging was well captured by the model, with carbonyls (formaldehyde, acetaldehyde, 2,3-butanedione, methylglyoxal, 2-furfural) in addition to CO and CH4 being the main drivers of peroxy radical chemistry. The model also accurately reproduced the sequestration of NOx into peroxyacetyl nitrate (PAN) and the OH-initiated degradation of furan and 2-furfural at an average OH concentration of 7.45±1.07 106 cm-3 in the plume. Formaldehyde, acetone/propanal, acetic acid/glycolaldehyde, and maleic acid/maleic anhydride (tentatively identified) were found to be the main NMOGs to increase during 1 h of atmospheric plume processing, with the model being unable to capture the observed increase. A mass balance analysis suggests that about 50% of the aerosol mass formed in the downwind plume is organic in nature. [ABSTRACT FROM AUTHOR]

This study quantifies the immediate influences of aerosols from urban anthropogenic and shipping emission sources on carbon and water fluxes in East Asia on a cloudy day in spring 2016 when strong regional pollution transport occurred and intensive field campaign measurements are available. Within National Aeronautics and Space Administration (NASA)'s Land Information System (LIS), a long‐term offline Noah‐multiparameterization (MP) simulation with dynamic vegetation is performed. Modeled soil moisture and leaf area index are evaluated with satellite observations to ensure that land surface conditions are moderately well reproduced. The LIS output is then used to initialize several coupled NASA‐Unified Weather Research and Forecasting model simulations with online chemistry in which urban anthropogenic and shipping emissions are (1) largely based on the Hemispheric Transport of Air Pollution Phase 2 inventory for 2010, (2) reduced by 20% and 50% for all chemical species, and (3) adjusted only for nitrogen oxides (NOx) using satellite observations. Overall, modeled gross primary productivity and evapotranspiration almost linearly increase with the all‐species emission reductions, but their responses to emission‐induced aerosol optical depth (AOD) changes show strong spatial variability resulting from combined radiation and temperature impacts. Using satellite‐observation‐constrained NOx emissions, modeled nitrogen species and AOD better match various measurements at some locations/times. All‐species and NOx‐only emission adjustments lead to different gross primary productivity and evapotranspiration changes with AOD, especially over South Korea. This study demonstrates the importance of accurately quantifying emission impacts on atmosphere‐biosphere interactions. Improving more species' emission inputs for Earth system models, including applying effective chemical data assimilation methods, is strongly encouraged. Key Points: Carbon and water fluxes are calculated by Noah‐MP (with dynamic vegetation) coupled with atmospheric weather and chemistryOverall, GPP and ET almost linearly increase with the all‐species urban/shipping emission reductions on a cloudy day in East AsiaGPP and ET responses to emission‐induced AOD changes differ by region and for all‐species and NOx‐only emission adjustments [ABSTRACT FROM AUTHOR]

We quantify both the spatial and temporal variability of column integrated O 3 , NO 2 , CO, SO 2 , and HCHO over the Baltimore/Washington, DC area using output from the Weather Research and Forecasting model with on-line chemistry (WRF/Chem) for the entire month of July 2011, coinciding with the first deployment of the NASA Earth Venture program mission Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ). Using structure function analyses, we find that the model reproduces the spatial variability observed during the campaign reasonably well, especially for O 3 . The Tropospheric Emissions: Monitoring of Pollution (TEMPO) instrument will be the first NASA mission to make atmospheric composition observations from geostationary orbit and partially fulfills the goals of the Geostationary Coastal and Air Pollution Events (GEO-CAPE) mission. We relate the simulated variability to the precision requirements defined by the science traceability matrices of these space-borne missions. Results for O 3 from 0 to 2 km altitude indicate that the TEMPO instrument would be able to observe O 3 air quality events over the Mid-Atlantic area, even on days when the violations of the air quality standard are not widespread. The results further indicated that horizontal gradients in CO from 0 to 2 km would be observable over moderate distances (≥20 km). The spatial and temporal results for tropospheric column NO 2 indicate that TEMPO would be able to observe not only the large urban plumes at times of peak production, but also the weaker gradients between rush hours. This suggests that the proposed spatial and temporal resolutions for these satellites as well as their prospective precision requirements are sufficient to answer the science questions they are tasked to address. [ABSTRACT FROM AUTHOR]

In this study, we contrasted major secondary inorganic species and processes responsible for submicron particle formation (SPF) events in the boundary layer (BL) and free troposphere (FT) over the Korean Peninsula during Korea-United States Air Quality (KORUS-AQ) campaign (May–June 2016) using aircraft observations. The number concentration of ultrafine particles with diameters between 3 nm and 10 nm (N CN3 – 10) during the entire KORUS-AQ period reached a peak (7606 ± 12,003 cm−3) at below 1 km altitude, implying that the particle formation around the Korean Peninsula primarily occurred in the daytime BL. During the BL SPF case (7 May 2016), the SPF over Seoul metropolitan area was more attributable to oxidation of NO 2 rather than SO 2 -to-sulfate conversion. From the analysis of the relationship between nitrogen oxidation ratio (NOR) and temperature or relative humidity (RH), NOR showed a positive correlation only with temperature. This suggests that homogeneous gas-phase reactions of NO 2 with OH or O 3 contributed to nitrate formation. From the relationship between N CN3 – 10 (> 10,000 cm−3) and the NOR (or sulfur oxidation ratio) at Olympic Park in Seoul during the entire KORUS-AQ period, it was regarded that the relative importance of nitrogen oxidation was grown as the N CN3 – 10 increased. During the FT SPF case (31 May 2016) over the yellow sea, the SO 2 -to-sulfate conversion seemed to influence SPF highly. The sulfate/CO ratio had a positive correlation with both the temperature and RH, suggesting that aqueous-phase pathways as well as gas-phase reactions might be attributable to sulfate formation in the FT. In particular, FT SPF event on 31 May was possibly caused by the direct transport of SO 2 precursors from the continent above the shallow marine boundary layer under favorable conditions for FT SPF events, such as decreased aerosol surface area and increased solar radiation. [Display omitted] • Submicron particle formation (SPF) events around the Korean Peninsula primarily occurred in the boundary layer (BL). • BL SPF case (7 May 2016) was primarily attributable to gas-phase oxidation of NO 2. • As the number of nucleation-mode particles increased, the relative importance of nitrogen oxidation was enhanced. • The SO 2 -to-sulfate conversion seemed to highly influence SPF in free troposphere (FT; 31 May 2016). • FT SPF event was possibly caused by the direct transport of SO 2 precursors. [ABSTRACT FROM AUTHOR]