Laboratory of Atmospheric Chemistry, Paul Scherrer Institut, CH-5232 Villigen PSI, Switzerland.
Proc Natl Acad Sci U S A. 2010 Apr 13;107(15):6646-51. doi: 10.1073/pnas.0911330107. Epub 2010 Jan 19.
New particle formation in the atmosphere is an important parameter in governing the radiative forcing of atmospheric aerosols. However, detailed nucleation mechanisms remain ambiguous, as laboratory data have so far not been successful in explaining atmospheric nucleation. We investigated the formation of new particles in a smog chamber simulating the photochemical formation of H(2)SO(4) and organic condensable species. Nucleation occurs at H(2)SO(4) concentrations similar to those found in the ambient atmosphere during nucleation events. The measured particle formation rates are proportional to the product of the concentrations of H(2)SO(4) and an organic molecule. This suggests that only one H(2)SO(4) molecule and one organic molecule are involved in the rate-limiting step of the observed nucleation process. Parameterizing this process in a global aerosol model results in substantially better agreement with ambient observations compared to control runs.
大气中新粒子的形成是控制大气气溶胶辐射强迫的一个重要参数。然而,详细的成核机制仍不清楚,因为迄今为止,实验室数据还未能成功解释大气成核。我们在一个烟雾箱中研究了新粒子的形成,该烟雾箱模拟了 H(2)SO(4)和有机可凝结物种的光化学形成。成核发生在 H(2)SO(4)浓度类似于在成核事件期间在环境大气中发现的浓度。测量的粒子形成速率与 H(2)SO(4)浓度和有机分子的浓度的乘积成正比。这表明在观察到的成核过程的限速步骤中,只涉及一个 H(2)SO(4)分子和一个有机分子。在全球气溶胶模型中对这个过程进行参数化,与对照运行相比,结果与环境观测的吻合度大大提高。