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

机译:成核率,存活率和凝结核形成之间的反馈分析

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摘要

Aerosol nucleation is an important source of particle number in theatmosphere. However, in order to become cloud condensation nuclei (CCN),freshly nucleated particles must undergo significant condensational growthwhile avoiding coagulational scavenging. In an effort to quantify thecontribution of nucleation to CCN, this work uses the GEOS-Chem-TOMAS globalaerosol model to calculate changes in CCN concentrations against a broadrange of nucleation rates and mechanisms. We then quantify the factors thatcontrol 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 growthof nucleated particles to CCN. Nucleation rate parameterizations tested inGEOS-Chem-TOMAS include ternary nucleation (with multiple tuning factors),activation nucleation (with two pre-factors), binary nucleation, andion-mediated nucleation. We find that nucleation makes a significantcontribution to boundary layer CCN(0.2%), but this contribution is onlymodestly 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 averagednucleation 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 anexponentially decreasing dependence on the square of the condensation sink.This functional form stems from a negative correlation between condensationsink and growth rate and a positive correlation between condensation sinkand coagulational scavenging. Conceptually, with a fixed condensable vaporbudget (sulfuric acid and organics), any increase in CCN concentrations dueto higher nucleation rates necessarily entails an increased aerosol surfacearea in the accumulation mode, resulting in a higher condensation sink, whichlowers vapor concentrations and growth rates. As a result, slowly growingnuclei are exposed to a higher frequency of coagulational scavenging for alonger period of time, thus reducing their survival probabilities andclosing a negative feedback loop that dampens the impact of nucleation onCCN. We confirm quantitatively that the decreases in survival probabilitypredicted by GEOS-Chem-TOMAS due to higher nucleation rates are inaccordance with this simple theory of survival probability.
机译:气溶胶成核是大气中颗粒数量的重要来源。然而,为了成为云凝结核(CCN),新核化的颗粒必须经历显着的凝结生长,同时避免凝结清除。为了量化成核对CCN的贡献,这项工作使用GEOS-Chem-TOMAS globalaerosol模型来计算各种成核速率和机制下CCN浓度的变化。然后,我们量化控制成核过程中CCN形成的因素,包括每日成核速率,生长速率,凝结汇,凝结汇,存活概率和CCN形成率,以便检查可能限制成核颗粒向CCN生长的反馈。在GEOS-Chem-TOMAS中测试的成核速率参数化包括三元成核(具有多个调节因子),活化成核(具有两个前置因子),二元成核和阴离子介导的成核。我们发现成核对边界层CCN的贡献很大(0.2%),但这种贡献仅对成核方案的选择适度敏感,与没有成核的对照模拟相比,浓度从49%增至78%。全球平均成核速率的数量级增加(通过调整因子的改变)导致全球CCN(0.2%)浓度的微小变化(小于10%)。为了解释这一点,我们提出了一个简单的理论,表明生存概率对冷凝槽的平方呈指数递减关系。这种功能形式源自冷凝槽与生长速率之间的负相关以及冷凝槽与凝结清除之间的正相关。从概念上讲,使用固定的可冷凝蒸气预算(硫酸和有机物),由于成核速率较高而导致的CCN浓度增加,必然会导致在累积模式下增加气溶胶表面积,从而导致更高的冷凝水槽,从而降低蒸气浓度和增长率。结果,缓慢生长的核在一段较长的时间内暴露于更高频率的凝结清除作用,从而降低了它们的生存概率,并关闭了负反馈回路,该回路抑制了成核作用对CCN的影响。我们定量地确认,GEOS-Chem-TOMAS由于较高的成核率而预测的生存概率降低与这种简单的生存概率理论不符。

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