Anthropogenic emissions of nitrogen oxides (NOx) can change rapidly due to economic growth or control measures. Bottom‐up emissions estimated using source‐specific emission factors and activity statistics require years to compile and can become quickly outdated. We present a method to use satellite observations of tropospheric NO2 columns to estimate changes in NOx emissions. We use tropospheric NO2 columns retrieved from the SCIAMACHY satellite instrument for 2003–2009, the response of tropospheric NO2 columns to changes in NOx emissions determined from a global chemical transport model (GEOS‐Chem), and the bottom‐up anthropogenic NOx emissions for 2006 to hindcast and forecast the inventories. We evaluate our approach by comparing bottom‐up and hindcast emissions for 2003. The two inventories agree within 6.0% globally and within 8.9% at the regional scale with consistent trends in western Europe, North America, and East Asia. We go on to forecast emissions for 2009. During 2006–2009, anthropogenic NOx emissions over land increase by 9.2% globally and by 18.8% from East Asia. North American emissions decrease by 5.7%.
[1] Measurements of BrO suggest that inorganic bromine (Br y ) at and above the tropopause is 4 to 8 ppt greater than assumed in models used in past ozone trend assessment studies. This additional bromine is likely carried to the stratosphere by short-lived biogenic compounds and their decomposition products, including tropospheric BrO. Including this additional bromine in an ozone trend simulation increases the computed ozone depletion over the past $25 years, leading to better agreement between measured and modeled ozone trends. This additional Br y (assumed constant over time) causes more ozone depletion because associated BrO provides a reaction partner for ClO, which increases due to anthropogenic sources. Enhanced Br y causes photochemical loss of ozone below $14 km to change from being controlled by HO x catalytic cycles (primarily HO 2 +O 3 ) to a situation where loss by the BrO+HO 2 cycle is also important. Citation: Salawitch, R. J.,
Upper stratospheric enhancements in NOx (NO and NO2) were observed at high northern latitudes from March through at least July of 2004. Multi‐satellite data analysis is used to examine the temporal evolution of the enhancements, to place them in historical context, and to investigate their origin. The enhancements were a factor of 4 higher than nominal at some locations, and are unprecedented in the northern hemisphere since at least 1985. They were accompanied by reductions in O3 of more than 60% in some cases. The analysis suggests that energetic particle precipitation led to substantial NOx production in the upper atmosphere beginning with the remarkable solar storms in late October 2003 and possibly persisting through January. Downward transport of the excess NOx, facilitated by unique meteorological conditions in 2004 that led to an unusually strong upper stratospheric vortex from late January through March, caused the enhancements.
[1] Ozone profiles are derived from back scattered radiance spectra in the ultraviolet (289-339 nm) measured by the Global Ozone Monitoring Experiment (GOME) using the optimal estimation technique. Tropospheric Column Ozone (TCO) is directly derived using the known tropopause to divide the stratosphere and troposphere. To optimize the retrieval and improve the fitting precision needed for tropospheric ozone, we perform extensive wavelength and radiometric calibrations and improve forward model inputs. The a priori influence of retrieved TCO is $15% in the tropics and increases to $50% at high latitudes. The dominant error terms are the smoothing errors, instrumental randomnoise errors, and systematic temperature errors. We compare our GOME retrievals with Earth-Probe Total Ozone Mapping Spectrometer (TOMS) Total column Ozone (TO), Dobson/Brewer (DB) TO, and ozonesonde TCO at 33 World Ozone and Ultraviolet Radiation Data Centre (WOUDC) stations between 71°S and 75°N during 1996-1999. The mean biases with TOMS and DB TO are within 6 DU (2%, 1 DU = 2.69 Â 10 16 molecules cm À2) at most of the stations. The retrieved Tropospheric Column Ozone (TCO) captures most of the temporal variability in ozonesonde TCO; the mean biases are mostly within 3 DU (15%) and the standard deviations (1s) are within 3-8 DU (13-27%). We also compare our retrieved ozone profiles above $15 km against Stratospheric Aerosol and Gas Experiment II measurements from 1996 to 1999. The mean biases and standard deviations are usually within 15%.
[1] We retrieve tropospheric nitrogen dioxide (NO 2 ) columns for May 2004 to April 2005 from the SCIAMACHY satellite instrument to derive top-down emissions of nitrogen oxides (NO x = NO + NO 2 ) via inverse modeling with a global chemical transport model (GEOS-Chem). Simulated NO 2 vertical profiles used in the retrieval are evaluated with airborne measurements over and downwind of North America (ICARTT); a northern midlatitude lightning source of 1.6 Tg N yr À1 minimizes bias in the retrieval. Retrieved NO 2 columns are validated (r 2 = 0.60, slope = 0.82) with coincident airborne in situ measurements. The top-down emissions are combined with a priori information from a bottom-up emission inventory with error weighting to achieve an improved a posteriori estimate of the global distribution of surface NO x emissions. Our a posteriori NO x emission inventory for land surface NO x emissions (46.1 Tg N yr À1 ) is 22% larger than the GEIA-based a priori bottom-up inventory for 1998, a difference that reflects rising anthropogenic emissions, especially from East Asia. A posteriori NO x emissions for East Asia (9.8 Tg N yr À1 ) exceed those from other continents. The a posteriori inventory improves the GEOS-Chem simulation of NO x , peroxyacetylnitrate, and nitric acid with respect to airborne in situ measurements over and downwind of New York City. The a posteriori is 7% larger than the EDGAR 3.2FT2000 global inventory, 3% larger than the NEI99 inventory for the United States, and 68% larger than a regional inventory for 2000 for eastern Asia. SCIAMACHY NO 2 columns over the North Atlantic show a weak plume from lightning NO x .
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