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<p><strong>Abstract.</strong> Organic aerosol formation and transformation occurs within aqueous aerosol and cloud droplets, yet little is known about the composition of high molecular weight organic compounds in cloud water. Cloud water samples collected at Whiteface Mountain, New York during August–September 2014 were analyzed by ultrahigh-resolution mass spectrometry to investigate the molecular composition of dissolved organic carbon, with focus on sulfur- and nitrogen-containing compounds. Organic molecular composition was evaluated in the context of cloud water inorganic ion concentrations, pH, and total organic carbon concentrations to gain insights into the sources and aqueous phase processes of the observed high molecular weight organic compounds. The molecular composition of the cloud water depended on the influencing sources (biogenic, urban, wildfire) and showed evidence of aqueous-phase processes. Cloud water acidity was correlated with the average oxygen:carbon ratio of the organic constituents, suggesting the influence of aqueous acid-catalyzed oxidation processes. Organosulfate compounds, with both biogenic and anthropogenic volatile organic compound precursors, were detected for cloud water samples influenced by air masses that had traveled over forested and populated areas. Oxidation products of long-chain (C<sub>10-12</sub>) alkane precursors were detected during urban influence. Influence of Canadian wildfires resulted in increased numbers of identified sulfur-containing compounds and oligomeric species, including those formed through aqueous-phase reactions involving methylglyoxal. Light absorbing aqueous-phase products of syringol and guaiacol oxidation were observed in the wildfire-influenced samples, and dinitroaromatic compounds were observed in all cloud water samples (wildfire, biogenic/urban, and urban-influenced).</p>

Long-term records of condensed-phase chemical data are presented from the Adirondack Mountain region of northern New York, USA. These data records are particularly valuable due to the combinations of aerosol, cloud, and precipitation measurements. Objectives of the research and this overview paper include the evaluation of emission reductions of regulated air pollutants and the observed effects on measured deposition, as well as the implications of changing pollutant concentration levels on human health and climate. Summer season cloud chemistry and year-round wet deposition and particulate matter data from two stations on Whiteface Mountain are presented to highlight some of the research and monitoring activities at this mountain location. Clear decreases in the anion concentrations and increases in pH over the past two decades have been observed in cloud and precipitation results. Large decreases in aerosol sulfate (> 80%) and aerosol optical black carbon (> 60%) have been observed for these species over the nearly 40 year summit observatory data record for these measurements, and decreases in PM 2.5 mass, sulfate, nitrate, and ammonium have also been recorded over the shorter 15 year period of measurement at the Marble Mountain Lodge level. The studies cited here highlight some of the past successes of air pollution regulation under the Clean Air Act and Amendments and pave the way for future progress in reducing air pollution.

Increasing pH and decreasing Al in surface waters recovering from acidification have been accompanied by increasing concentrations of dissolved organic carbon (DOC) and associated organic acids that partially offset pH increases and complicate assessments of recovery from acidification. To better understand the processes of recovery, monthly chemistry from 42 lakes in the Adirondack region, NY, collected from 1994 to 2011, were used to (1) evaluate long-term changes in DOC and associated strongly acidic organic acids and (2) use the base-cation surplus (BCS) as a chemical index to assess the effects of increasing DOC concentrations on the Al chemistry of these lakes. Over the study period, the BCS increased (p < 0.01) and concentrations of toxic inorganic monomeric Al (IMAl) decreased (p < 0.01). The decreases in IMAl were greater than expected from the increases in the BCS. Higher DOC concentrations that increased organic complexation of Al resulted in a decrease in the IMAl fraction of total monomeric Al from 57% in 1994 to 23% in 2011. Increasing DOC concentrations have accelerated recovery in terms of decreasing toxic Al beyond that directly accomplished by reducing atmospheric deposition of strong mineral acids.