ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-11-4755-2011 Ternary homogeneous nucleation of H<sub>2</sub>SO<sub>4</sub>, NH<sub>3</sub>, and H<sub>2</sub>O under conditions relevant to the lower troposphere Benson D. R. 1 Yu J. H. 1 Markovich A. 1 Lee S.-H. 1 Kent State University, Department of Chemistry, Kent, Ohio 44240, USA 20 05 2011 11 10 4755 4766 This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. This article is available from http://www.atmos-chem-phys.net/11/4755/2011/acp-11-4755-2011.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/11/4755/2011/acp-11-4755-2011.pdf

Ternary homogeneous nucleation (THN) of H<sub>2</sub>SO<sub>4</sub>, NH<sub>3</sub> and H<sub>2</sub>O has been used to explain new particle formation in various atmospheric regions, yet laboratory measurements of THN have failed to reproduce atmospheric observations. Here, we report first laboratory observations of THN made under conditions relevant to the lower troposphere ([H<sub>2</sub>SO<sub>4</sub>] of 10<sup>6</sup>–10<sup>7</sup> cm<sup>−3</sup>, [NH<sub>3</sub>] of 0.08–20 ppbv, and a temperature of 288 K). Our observations show that NH<sub>3</sub> can enhance atmospheric H<sub>2</sub>SO<sub>4</sub> aerosol nucleation and the enhancement factor (EF) in nucleation rate (<i>J</i>) due to NH<sub>3</sub> (the ratio of <i>J</i> measured with vs. without NH<sub>3</sub>) increases linearly with increasing [NH<sub>3</sub>] and increases with decreasing [H<sub>2</sub>SO<sub>4</sub>] and RH. Two chemical ionization mass spectrometers (CIMS) are used to measure [H<sub>2</sub>SO<sub>4</sub>] and [NH<sub>3</sub>], as well as possible impurities of amines in the nucleation system. Aerosol number concentrations are measured with a water condensation counter (CPC, TSI 3786). The slopes of Log <i>J</i> vs. Log [H<sub>2</sub>SO<sub>4</sub>], Log <i>J</i> vs. Log RH, and Log <i>J</i> vs. Log [NH<sub>3</sub>] are 3–5, 1–4, and 1, respectively. These slopes and the threshold of [H<sub>2</sub>SO<sub>4</sub>] required for the unity nucleation vary only fractionally in the presence and absence of NH<sub>3</sub>. These observations can be used to improve aerosol nucleation models to assess how man-made SO<sub>2</sub> and NH<sub>3</sub> affect aerosol formation and CCN production at the global scale.

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