Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA, USA.
Department of Chemistry, Carnegie Mellon University, Pittsburgh, PA, USA.
Nature. 2022 May;605(7910):483-489. doi: 10.1038/s41586-022-04605-4. Epub 2022 May 18.
New particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN). However, the precursor vapours that drive the process are not well understood. With experiments performed under upper tropospheric conditions in the CERN CLOUD chamber, we show that nitric acid, sulfuric acid and ammonia form particles synergistically, at rates that are orders of magnitude faster than those from any two of the three components. The importance of this mechanism depends on the availability of ammonia, which was previously thought to be efficiently scavenged by cloud droplets during convection. However, surprisingly high concentrations of ammonia and ammonium nitrate have recently been observed in the upper troposphere over the Asian monsoon region. Once particles have formed, co-condensation of ammonia and abundant nitric acid alone is sufficient to drive rapid growth to CCN sizes with only trace sulfate. Moreover, our measurements show that these CCN are also highly efficient ice nucleating particles-comparable to desert dust. Our model simulations confirm that ammonia is efficiently convected aloft during the Asian monsoon, driving rapid, multi-acid HNO-HSO-NH nucleation in the upper troposphere and producing ice nucleating particles that spread across the mid-latitude Northern Hemisphere.
在上层自由大气层中新颗粒的形成是云凝结核(CCN)的主要全球来源。然而,驱动这一过程的前体蒸气还没有得到很好的理解。在 CERN CLOUD 室的上层大气条件下进行的实验表明,硝酸、硫酸和氨协同形成颗粒,其速率比三种成分中的任何两种都快几个数量级。这种机制的重要性取决于氨的可用性,氨以前被认为在对流过程中会被云滴有效地清除。然而,令人惊讶的是,在亚洲季风区的上层大气中,最近观测到了高浓度的氨和硝酸铵。一旦颗粒形成,仅氨和大量硝酸的共同冷凝就足以驱动快速生长到 CCN 大小,而只有痕量的硫酸盐。此外,我们的测量表明,这些 CCN 也是高效的冰成核粒子——与沙漠尘埃相当。我们的模型模拟证实,在亚洲季风期间,氨在上空被有效地输送,在上层大气中驱动快速的多酸 HNO-HSO-NH 成核,并产生冰成核粒子,这些粒子在中纬度北半球扩散。