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Influences of specific sources of inorganic PM2.5 on peak and ambientaerosol concentrations in the US are evaluated using a combination of inversemodeling and sensitivity analysis. First, sulfate and nitrate aerosolmeasurements from the IMPROVE network are assimilated using thefour-dimensional variational (4D-Var) method into the GEOS-Chem chemicaltransport model in order to constrain emissions estimates in four separatemonth-long inversions (one per season). Of the precursor emissions, theseobservations primarily constrain ammonia (NH3). While the net result is adecrease in estimated US~NH3 emissions relative to the original inventory,there is considerable variability in adjustments made to NH3 emissions indifferent locations, seasons and source sectors, such as focused decreases inthe midwest during July, broad decreases throughout the US~in January,increases in eastern coastal areas in April, and an effective redistributionof emissions from natural to anthropogenic sources. Implementing theseconstrained emissions, the adjoint model is applied to quantify theinfluences of emissions on representative PM2.5 air quality metricswithin the US. The resulting sensitivity maps display a wide range ofspatial, sectoral and seasonal variability in the susceptibility of the airquality metrics to absolute emissions changes and the effectiveness ofincremental emissions controls of specific source sectors. NH3 emissionsnear sources of sulfur oxides (SOx) are estimated to most influencepeak inorganic PM2.5 levels in the East; thus, the most effectivecontrols of NH3 emissions are often disjoint from locations of peak NH3emissions. Controls of emissions from industrial sectors of SOx andNOx are estimated to be more effective than surface emissions, andchanges to NH3 emissions in regions dominated by natural sources aredisproportionately more effective than regions dominated by anthropogenicsources. NOx controls are most effective in northern states inOctober; in January, SOx controls may be counterproductive. Whenconsidering ambient inorganic PM2.5 concentrations, intercontinentalinfluences are small, though transboundary influences within North Americaare significant, with SOx emissions from surface sources in Mexicocontributing almost a fourth of the total influence from this sector

atmospheric chemistry and physics

Inverse modeling and mapping US air quality influences of inorganic PM&amp;lt;sub&amp;gt;2.5&amp;lt;/sub&amp;gt; precursor emissions using the adjoint of GEOS-Chem