Synergistic HNO3-H2SO4-NH3 upper tropospheric particle formation

Article

关键词: CHEMICAL-TRANSPORT MODEL;    SULFURIC-ACID;    ATMOSPHERIC AEROSOL;    ICE NUCLEATION;    MASS-SPECTROMETER;    HIGH-RESOLUTION;    DESERT DUST;    AMMONIA;    SIZE;    GROWTH;   

DOI  :  10.1038/s41586-022-04605-4

来源: SCIE

【 摘 要 】

New particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN)(1-4). However, the precursorvapoursthat drive the process are not well understood. With experiments performed under upper tropospheric conditions in the CERN CLOUD chamber, we showthat nitric acid, sulfuric acid and ammonia form particles synergistically, at ratesthat are orders of magnitude faster than those from any two ofthe three components. The importance ofthis 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 uppertroposphere overthe Asian monsoon region(5,6). 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 showthat 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 HNO3-H2SO4-NH3 nucleation in the uppertroposphere and producing ice nucleating particles that spread acrossthe mid-latitude Northern Hemisphere.

【 授权许可】

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