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Analysis of feedbacks between nucleation rate, survival probability and cloud condensation nuclei formation

机译:成核率,存活概率和云凝结核形成的反馈分析

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Aerosol nucleation is an important source of particle number in the atmosphere. However, in order to become cloud condensation nuclei (CCN), freshly nucleated particles must undergo significant condensational growth while avoiding coagulational scavenging. In an effort to quantify the contribution of nucleation to CCN, this work uses the GEOS-Chem-TOMAS global aerosol model to calculate changes in CCN concentrations against a broad range of nucleation rates and mechanisms. We then quantify the factors that control CCN formation from nucleation, including daily nucleation rates, growth rates, coagulation sinks, condensation sinks, survival probabilities, and CCN formation rates, in order to examine feedbacks that may limit growth of nucleated particles to CCN. Nucleation rate parameterizations tested in GEOS-Chem-TOMAS include ternary nucleation (with multiple tuning factors), activation nucleation (with two pre-factors), binary nucleation, and ion-mediated nucleation. We find that nucleation makes a significant contribution to boundary layer CCN(0.2%), but this contribution is only modestly sensitive to the choice of nucleation scheme, ranging from 49 to 78% increase in concentrations over a control simulation with no nucleation. Moreover, a two order-of-magnitude increase in the globally averaged nucleation rate (via changes to tuning factors) results in small changes (less than 10%) to global CCN(0.2%) concentrations. To explain this, we present a simple theory showing that survival probability has an exponentially decreasing dependence on the square of the condensation sink. This functional form stems from a negative correlation between condensation sink and growth rate and a positive correlation between condensation sink and coagulational scavenging. Conceptually, with a fixed condensable vapor budget (sulfuric acid and organics), any increase in CCN concentrations due to higher nucleation rates necessarily entails an increased aerosol surface area in the accumulation mode, resulting in a higher condensation sink, which lowers vapor concentrations and growth rates. As a result, slowly growing nuclei are exposed to a higher frequency of coagulational scavenging for a longer period of time, thus reducing their survival probabilities and closing a negative feedback loop that dampens the impact of nucleation on CCN. We confirm quantitatively that the decreases in survival probability predicted by GEOS-Chem-TOMAS due to higher nucleation rates are in accordance with this simple theory of survival probability.
机译:气溶胶成核的粒子数在大气中的重要来源。然而,为了成为云凝结核(CCN),新鲜核粒子必须同时避免coagulational扫气经历显著凝结增长。在努力量化核到CCN的贡献,这项工作采用GEOS-CHEM-TOMAS全球气溶胶模式对CCN浓度变化计算针对广泛的成核速率和机制。然后,我们量化的因素,从成核控制CCN形成,包括日常核率,增长率,凝汇,凝结水槽,生存概率和CCN形成速率,以检查反馈,这可能限制核粒子的增长CCN。在GEOS-CHEM-TOMAS测试核率参数化包括三元成核(具有多个调谐因子),活化成核(有两个预因素),二进制成核,和离子介导的成核。我们发现,核使边界层CCN(0.2%)一个显著的贡献,但这种贡献是只选择核计划,范围从49到78的浓度%,增幅比控制仿真没有核适度敏感。此外,二阶的数量级增加的全球平均成核速率(通过改变调谐因子)导致的小变化(小于10%),以全球CCN(0.2%)的浓度。为了解释这一点,我们提出显示出生存概率的简单理论对冷凝水槽的平方的指数下降的依赖。此功能形式从冷凝水槽和生长速率和缩合水槽和coagulational扫气之间的正相关之间的负相关茎。从概念上讲,具有固定冷凝的蒸汽预算(硫酸和有机物),由于较高的成核速率的任何增加在CCN浓度必然需要在累积模式的增加的气雾剂的表面积,从而导致更高的缩合水槽,从而降低蒸汽浓度和增长率。其结果是,缓慢生长的核暴露于coagulational扫气的的时间较长时间的较高的频率,从而降低了它们的生存概率和闭合负反馈回路,其衰减成核上CCN的影响。我们量化了由GEOS-CHEM-TOMAS预测生存概率降低证实是由于较高的成核速率是按照生存概率的这个简单的理论。

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