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      A statistical proxy for sulphuric acid concentration

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          Abstract

          <p><strong>Abstract.</strong> Gaseous sulphuric acid is a key precursor for new particle formation in the atmosphere. Previous experimental studies have confirmed a strong correlation between the number concentrations of freshly formed particles and the ambient concentrations of sulphuric acid. This study evaluates a body of experimental gas phase sulphuric acid concentrations, as measured by Chemical Ionization Mass Spectrometry (CIMS) during six intensive measurement campaigns and one long-term observational period. The campaign datasets were measured in Hyytiälä, Finland, in 2003 and 2007, in San Pietro Capofiume, Italy, in 2009, in Melpitz, Germany, in 2008, in Atlanta, Georgia, USA, in 2002, and in Niwot Ridge, Colorado, USA, in 2007. The long term data were obtained in Hohenpeissenberg, Germany, during 1998 to 2000. The measured time series were used to construct proximity measures ("proxies") for sulphuric acid concentration by using statistical analysis methods. The objective of this study is to find a proxy for sulfuric acid that is valid in as many different atmospheric environments as possible. Our most accurate and universal formulation of the sulphuric acid concentration proxy uses global solar radiation, SO<sub>2</sub> concentration, condensation sink and relative humidity as predictor variables, yielding a correlation measure (<i>R</i>) of 0.87 between observed concentration and the proxy predictions. Interestingly, the role of the condensation sink in the proxy was only minor, since similarly accurate proxies could be constructed with global solar radiation and SO<sub>2</sub> concentration alone. This could be attributed to SO<sub>2</sub> being an indicator for anthropogenic pollution, including particulate and gaseous emissions which represent sinks for the OH radical that, in turn, is needed for the formation of sulphuric acid.</p>

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          Most cited references44

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          Nonlinear Regression Analysis and Its Applications

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            The Role of Sulfuric Acid in Atmospheric Nucleation

            Nucleation is a fundamental step in atmospheric new-particle formation. However, laboratory experiments on nucleation have systematically failed to demonstrate sulfuric acid particle formation rates as high as those necessary to account for ambient atmospheric concentrations, and the role of sulfuric acid in atmospheric nucleation has remained a mystery. Here, we report measurements of new particles (with diameters of approximately 1.5 nanometers) observed immediately after their formation at atmospherically relevant sulfuric acid concentrations. Furthermore, we show that correlations between measured nucleation rates and sulfuric acid concentrations suggest that freshly formed particles contain one to two sulfuric acid molecules, a number consistent with assumptions that are based on atmospheric observations. Incorporation of these findings into global models should improve the understanding of the impact of secondary particle formation on climate.
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              Measurements of new particle formation and ultrafine particle growth rates at a clean continental site

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                Author and article information

                Journal
                Atmospheric Chemistry and Physics
                Atmos. Chem. Phys.
                Copernicus GmbH
                1680-7324
                2011
                November 14 2011
                : 11
                : 21
                : 11319-11334
                Article
                10.5194/acp-11-11319-2011
                4ed86da7-554c-4e5c-ab38-803a4485948b
                © 2011

                https://creativecommons.org/licenses/by/3.0/

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