Atmospheric aerosols are key contributors to cloud condensation nuclei (CCN) and ice nucleating particle (INP) formation, which can offset positive radiative forcing. Aerosol particles can undergo many cycles of droplet activation and subsequent drying before their removal from the atmosphere through dry or wet deposition. Cloud-aerosol-precipitation interactions are affected by cloud droplet or ice crystal formation, which is related to the physicochemical properties of aerosol particles. Isoprene-derived secondary organic aerosol (iSOA) is an abundant component aerosol and has been previously found in INPs and cloud water residues, and it includes both soluble and insoluble residues in its particle matrix. Currently, most of our understanding of iSOA is derived from studying the soluble residues, but there has been a measurement gap for characterizing the insoluble residues. These measurements are needed as previous research has suggested that insoluble components could be important with respect to CCN and INP formation. Herein, a unique approach is utilized to collect the insoluble residues of SOA in ~3 μm droplets collected from a Spot Sampler from Aerosol Devices, Inc. iSOA is generated by reactive uptake of IEPOX onto acidic seed particles (ammonium sulfate + sulfuric acid) in a humidified atmospheric chamber under dark conditions. Droplets are impacted directly on a substrate or in a liquid medium to study the roles of insoluble residues from both single-particle and bulk perspectives. A suite of microspectroscopy techniques, including Raman and optical photothermal infrared (O-PTIR) spectroscopy, are used to probe the chemical composition of the residues. Atomic force microscopy – photothermal infrared (AFM-PTIR) spectroscopy and Nanoparticle Tracking Analysis (NTA) are used to measure the size distributions of the residues. These insights may help understand the properties of residues from cloud droplet evaporation and subsequent cloud-aerosol-precipitation interactions in the atmosphere.
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Synergistic HNO3–H2SO4–NH3 upper tropospheric particle formation
Abstract New particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN) 1–4 . 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 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 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 3 –H 2 SO 4 –NH 3 nucleation in the upper troposphere and producing ice nucleating particles that spread across the mid-latitude Northern Hemisphere.
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- NSF-PAR ID:
- 10326856
- Author(s) / Creator(s):
- ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; more »
- Date Published:
- Journal Name:
- Nature
- Volume:
- 605
- Issue:
- 7910
- ISSN:
- 0028-0836
- Page Range / eLocation ID:
- 483 to 489
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1038/s41586-022-04605-4
