Climatologies of NOxx and NOy: A comparison of data and models

Emmons, L. K.; Carroll, Mary Anne; Hauglustaine, Didier; Brasseur, Guy; Atherton, C. S.; Penner, Joyce E.; Sillman, Sanford; Levy, H.; Rohrer, Franz; Wauben, W. M. F.; Velthoven, P. F. J. van; Wang, Y.; Jacob, Daniel J.; Bakwin, Peter S.; Dickerson, Russell R.; Doddridge, Bruce G.; Gerbig, Christoph; Honrath, R. E.; Hübler, G.; Jaffe, Daniel A.; Kondo, Yutaka; Munger, J. William; Torres, A. L.; Volz‐Thomas, A.

doi:10.1016/s1352-2310(96)00334-2

Cited by 119 publications

(73 citation statements)

References 144 publications

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“…The literature however provides support that TM3 produces realistic NO x distributions. For instance, we note that various studies (Emmonds et al, 1997;Wauben et al, 1997;Meijer et al, 2000) have indicated that TM3 is capable of reproducing aircraft-and surface-observed NO x concentrations for a range of different meteorological and chemical situations. Also, recent studies by Brunner et al (2003Brunner et al ( , 2005 showed that TM3 is well capable of reproducing observed NO x and NO x -related species.…”

Section: Tm3 Errorsmentioning

confidence: 96%

Estimates of lightning NO<sub>x</sub> production from GOME satellite observations

et al. 2005

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Abstract. Tropospheric NO 2 column retrievals from the Global Ozone Monitoring Experiment (GOME) satellite spectrometer are used to quantify the source strength and 3-D distribution of lightning produced nitrogen oxides (NO x =NO+NO 2 ). A sharp increase of NO 2 is observed at convective cloud tops with increasing cloud top height, consistent with a power-law behaviour with power 5±2. Convective production of clouds with the same cloud height are found to produce NO 2 with a ratio 1.6/1 for continents compared to oceans. This relation between cloud properties and NO 2 is used to construct a 10:30 local time global lightning NO 2 production map for 1997. An extensive statistical comparison is conducted to investigate the capability of the TM3 chemistry transport model to reproduce observed patterns of lightning NO 2 in time and space. This comparison uses the averaging kernel to relate modelled profiles of NO 2 to observed NO 2 columns. It exploits a masking scheme to minimise the interference of other NO x sources on the observed total columns. Simulations are performed with two lightning parameterizations, one relating convective preciptation (CP scheme) to lightning flash distributions, and the other relating the fifth power of the cloud top height (H5 scheme) to lightning distributions. The satellite-retrieved NO 2 fields show significant correlations with the simulated lightning contribution to the NO 2 concentrations for both parameterizations. Over tropical continents modelled lightning NO 2 shows remarkable quantitative agreement with observations. Over the oceans however, the two model lightning parameterizations overestimate the retrieved NO 2 attributed to lightning. Possible explanations for these overestimations are discussed. The ratio between satellite-retrieved NO 2 and modelled lightning NO 2 is used to rescale the original modelled lightning NO x production. Eight estimates of the lightning NO x production in 1997 are obtained from spatial and temporal correCorrespondence to: K. F. Boersma (boersma@knmi.nl) lation methods, from cloud-free and cloud-covered observations, and from two different lightning parameterizations. Accounting for a wide variety of random and possible systematic errors, we estimate the global NO x production from lightning to be in the range 1.1-6.4 Tg N in 1997.

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Section: Tm3 Errorsmentioning

confidence: 96%

Estimates of lightning NO<sub>x</sub> production from GOME satellite observations

et al. 2005

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“…Background levels for NO y and NMOC and their relevance to O 3 production have not been addressed extensively in the literature. NO y background derives from sources such as soil respiration and lightning, as well as an intra-and intercontinental residual (e.g., Guenther et al, 2000;Emmons et al, 1997;Bradshaw et al, 2000). For the marine background, NO x levels are at the 10-100 pptv level.…”

Section: Significance Of Backgroundmentioning

confidence: 99%

Precursor reductions and ground-level ozone in the Continental United States

Hidy¹,

Blanchard²

2015

Journal of the Air & Waste Management Association

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Numerous papers analyze ground-level ozone (O 3 ) trends since the 1980s, but few have linked O 3 trends with observed changes in nitrogen oxide (NO x ) and volatile organic compound (VOC) emissions and ambient concentrations. This analysis of emissions and ambient measurements examines this linkage across the United States on multiple spatial scales from continental to urban. O 3 concentrations follow the general decreases in both NO x and VOC emissions and ambient concentrations of precursors (nitrogen dioxide, NO 2 ; nonmethane organic compounds, NMOCs). Annual fourth-highest daily peak 8-hr average ozone and annual average or 98th percentile daily maximum hourly NO 2 concentrations show a statistically significant (p < 0.05) linear fit whose slope is less than 1:1 and intercept is in the 30 to >50 ppbv range. This empirical relationship is consistent with current understanding of O 3 photochemistry. The linear O 3 -NO 2 relationships found from our multispatial scale analysis can be used to extrapolate the rate of change of O 3 with projected NO x emission reductions, which suggests that future declines in annual fourth-highest daily average 8-hr maximum O 3 concentrations are unlikely to reach 65 ppbv or lower everywhere in the next decade. Measurements do not indicate increased annual reduction rates in (high) O 3 concentrations beyond the multidecadal precursor proportionality, since aggressive measures for NO x and VOC reduction are in place and have not produced an accelerated O 3 reduction rate beyond that prior to the mid-2000s. Empirically estimated changes in O 3 with emissions suggest that O 3 is less sensitive to precursor reductions than is found by the CAMx (v. 6.1) photochemical model. Options for increasing the rate of O 3 change are limited by photochemical factors, including the increase in NO x sensitivity with time (NMOC/NO x ratio increase), increase in O 3 production efficiency at lower NO x concentrations (higher O 3 /NO y ratio), and the presence of natural NO x and NMOC precursors and background O 3 .Implications: This analysis demonstrates empirical relations between O 3 and precursors based on long term trends in U.S. locations. The results indicate that ground-level O 3 concentrations have responded predictably to reductions in VOC and NO x since the 1980s. The analysis reveals linear relations between the highest O 3 and NO 2 concentrations. Extrapolation of the historic trends to the future with expected continued precursor reductions suggest that achieving the 2014 proposed reduction in the U.S. National Ambient Air Quality Standard to a level between 65 and 70 ppbv is unlikely within the next decade. Comparison of measurements with national results from a regulatory photochemical model, CAMx, v. 6.1, suggests that model predictions are more sensitive to emissions changes than the observations would support.

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“…PAN also has an effect on the oxidising power of the atmosphere through its reaction with the hydroxyl radical, OH (Talukdar et al, 1995). In the atmosphere, PAN has only been measured by in situ studies such as those made by Gas Chromatography Electron Capture Detection (GC-ECD) techniques (Tanimoto et al, 1999) during aircraft campaigns such as those detailed by Emmons et al, (1997). The typically low concentrations of PAN (<100 pptv) make it difficult to detect by these methods and errors remain high (typically 30%), with a limit of detection of around 50 pptv.…”

Section: Introductionmentioning

confidence: 99%

Improved mid-infrared cross-sections for peroxyacetyl nitrate (PAN) vapour

et al. 2005

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Abstract. Absorption spectra of peroxyacetyl nitrate (PAN, CH 3 C(O)OONO 2 ) vapour at room temperature (295K) have been measured in the mid-infrared range, 550-2200 cm −1 (18.2-4.55 µm), using a Fourier Transform infrared spectrometer at instrument resolutions of 0.25 and 0.03 cm −1 (unapodised). Between five and eight measurements were obtained for each spectral band of PAN in the pressure range 0.24-2.20 mb showing good agreement with Beer's law. Both cross-section data and integrated absorption intensities for the five principal bands in the PAN spectra in this spectral range have been derived with peak cross-sections of the 794, 1163, 1302, 1741 and 1842 cm −1 bands measured to be 0.95(±0.02), 1.21(±0.03), 0.92(±0.02), 2.39(±0.06) and 0.74(±0.03) (×10 −18 cm 2 molecule −1 ) respectively. Band intensities and band centre absorptivities are also reported for four weaker PAN absorption bands in the mid infrared for the first time. These observations are the highest spectral resolution measurements of PAN bands reported in the infrared to date. For three of the five strongest bands, the absolute integrated absorption intensities are in excellent agreement with previous studies. A 4.8% lower integrated intensity was found for the 1741 cm −1 ν as (NO 2 ) PAN absorption band, possibly as a result of the removal in this work of spectra affected by acetone contamination, while a 10.6% higher intensity was determined for the 1163 cm −1 ν(C-O) absorption band. No resolution of fine structure in the PAN absorption bands was observed at the resolutions studied. The confirmation of absorption cross-sections and estimated errors in this work will allow more accurate investigations of PAN using infrared spectroscopy, particularly for remote sensing of PAN in the atmosphere.

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Climatologies of NOxx and NOy: A comparison of data and models

Cited by 119 publications

References 144 publications

Estimates of lightning NO<sub>x</sub> production from GOME satellite observations

Estimates of lightning NO<sub>x</sub> production from GOME satellite observations

Precursor reductions and ground-level ozone in the Continental United States

Improved mid-infrared cross-sections for peroxyacetyl nitrate (PAN) vapour

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Climatologies of NOxx and NOy: A comparison of data and models

Cited by 119 publications

References 144 publications

Estimates of lightning NO&lt;sub&gt;x&lt;/sub&gt; production from GOME satellite observations

Estimates of lightning NO&lt;sub&gt;x&lt;/sub&gt; production from GOME satellite observations

Precursor reductions and ground-level ozone in the Continental United States

Improved mid-infrared cross-sections for peroxyacetyl nitrate (PAN) vapour

Contact Info

Product

Resources

About

Estimates of lightning NO<sub>x</sub> production from GOME satellite observations

Estimates of lightning NO<sub>x</sub> production from GOME satellite observations