...
首页> 外文期刊>Atmospheric Chemistry and Physics Discussions >Boundary layer nucleation as a source of new CCN in savannah environment
【24h】

Boundary layer nucleation as a source of new CCN in savannah environment

机译:边界层成核作为大草原环境中的新CCN的来源

获取原文
           

摘要

The South African savannah region is a complex environment of air pollution and natural emissions influenced by a strong seasonal cycle in biomass burning and strong precipitation. However, the scarcity of long-term observations means that the knowledge of controlling aerosol processes in this environment is limited. Here we use a recent dataset of 18 months of aerosol size distribution observations trying to understand the annual cycle of cloud condensation nuclei (CCN). Our observations show that the concentration of CCN-sized particles remains, in line with previous studies, high throughout the year with the highest concentrations during the dry winter and the lowest during the wet summer. During the wet season with reduced anthropogenic and biomass burning primary emissions, this pool of CCN is partly filled by boundary layer nucleation with subsequent growth. The enhanced importance of formation and growth during the wet season is addressed to increased biogenic activity together with enhanced free tropospheric removal decreasing the concentration of pre-existing CCN. During the dry season, while frequent new particle formation takes place, particle growth is reduced due to reduced condensing vapour concentrations. Thus in the dry season particles are not able to grow to sizes where they may act as CCN nearly as efficiently as during the wet season. The observations are compared to simulations by a global aerosol model GLOMAP. To our surprise, the global aerosol model utilized to explain the observations was not capable of re-producing the characteristics of particle formation and the annual CCN cycle, despite earlier good performance in predicting the particle concentrations in a number of diverse environments, including the South African savannah region. While the average yearly CCN concentrations of modelled CCN is close to observed concentrations, the characteristics of nucleation bursts and subsequent growth are not captured satisfactory by the model. Our sensitivity tests using different nucleation parameterizations and condensing organic vapour production rates show that neither of these is likely to explain the differences between observed and modelled nucleation and growth rates. A sensitivity study varying 28 modelling parameters indicates that the main uncertainties in the result are due to uncertainties in biomass burning emissions during the dry season, and anthropogenic sulphur emissions during the wet season, both in terms or emitted mass and particle sizes. The uncertainties appear to be mostly related to uncertainties in primary particle emissions, including the emissions variability not captured by monthly emission inventories. The results of this paper also highlights the fact that deficiencies in emissions estimates may result in deficiencies in particle production fluxes, while the end product such as modelled CCN concentration may be in line with observations.
机译:南非大草原地区是一种复杂的空气污染环境,受到生物量燃烧和强烈降水的强烈季节性循环的自然排放。然而,长期观测的稀缺意味着在这种环境中控制气溶胶过程的知识是有限的。在这里,我们使用最近的18个月的雾化尺寸分布观测观察,试图了解云凝结核(CCN)的年度周期。我们的观察结果表明,CCN大小颗粒的浓度依次与先前的研究一致,全年高,干燥冬季期间最高的浓度,潮湿夏季最低。在潮湿的季节减少的人为和生物质燃烧初级排放时,这种CCN池由边界层成核部分填充,随后的生长。在湿季期间的形成和生长增强了重要性,以增加生物活性,增强自由的对流层去除降低预先存在的CCN的浓度。在干燥的季节期间,在发生频繁的新颗粒形成时,由于降低的蒸气浓度,颗粒生长减少。因此,在干燥的季节中,颗粒不能生长到尺寸,其中它们可以像湿季节一样充当CCN。通过全球气溶胶模型Glomap进行比较观察。令我们奇迹,利用用于解释观察的全球气溶胶模型不能再产生粒子形成和年度CCN循环的特征,尽管在包括南方包括南部的多种不同环境中的颗粒浓度方面非洲大草原地区。虽然建模的CCN的平均CCN浓度接近观察到的浓度,但是模型的成核突发的特征和随后的生长并未达到令人满意。我们使用不同成核参数化和凝结有机蒸汽生产率的灵敏度试验表明,这些可能解释了观察和模拟的成核和生长速率之间的差异。敏感性研究改变28型建模参数表明结果的主要不确定性是由于生物量在干燥季节燃烧排放的不确定性,湿季期间的人为硫排放,都在术语或发出的质量和颗粒尺寸。不确定性似乎主要与原发性粒子排放中的不确定性相关,包括月度排放库存未被捕获的排放变异性。本文的结果还强调了排放估计中的缺陷可能导致颗粒生产通量的缺陷,而诸如建模的CCN浓度的最终产品可能与观察结果一致。

著录项

获取原文

客服邮箱:kefu@zhangqiaokeyan.com

京公网安备:11010802029741号 ICP备案号:京ICP备15016152号-6 六维联合信息科技 (北京) 有限公司©版权所有
  • 客服微信

  • 服务号