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1. Development of a single-particle technique to study insoluble residues from isoprene-derived secondary organic aerosol in droplets

   Parham, Rebecca; Fankhauser, Alison; Shi, Jia; Cooke, Madeline; YAN, JIN; Waters, Cara; Xiao, Yao; Kolozsvari, Katherine; Armstrong, N Cazimir; Zhang, Zhenfa; et al (March 2023, 2023 Spring ACS Meet ing)

   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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2. Insoluble Residues from Isoprene-Derived Secondary Organic Aerosol Determined by Nanoparticle Tracking Analysis and Microspectroscopy Techniques

   PARHAM, REBECCA; Fankhauser, Alison; Shi, Jia; Cooke, Madeline; Yan, Jin; Waters, Cara; Xiao, Yao; Kolozsvari, Katherine; Armstrong, N. Cazimir; Zhang, Zhenfa; et al (October 2022, AAAR 40th Annual Conference)

   Atmospheric aerosols significantly offset positive radiative forcing due to their contributions as cloud condensation nuclei (CCN) and ice nucleating particles (INPs). The cloud-aerosol-precipitation interactions in the atmosphere are determined by physical and chemical properties of aerosol particles, which can undergo many cycles of droplet activation and subsequent drying before dry or wet deposition from the atmosphere. Secondary organic aerosol (SOA) is an abundant class of aerosol and has been previously shown to contribute to aerosol formed from cloud processing. Isoprene-derived secondary organic aerosol SOA (iSOA) is a particularly important class of aerosol involved in cloud processing. iSOA has both soluble and insoluble components, but there has been a measurement gap in characterizing the insoluble components, as most analyses have focused on soluble components. These measurements are needed as previous research has suggested that insoluble components could be important with respect to CCN and INP formation. Herein, we analyze the insoluble components of SOA generated from the reactive uptake of IEPOX onto acidic seed particles (ammonium sulfate + sulfuric acid at different ratios for different pH conditions) in an atmospheric chamber. We characterize the size distributions and chemical composition, using NanoParticle Tracking Analysis (NTA), Raman microspectroscopy and atomic force microscopy infrared (AFM-IR) spectroscopy as a function of sulfate aerosol seed pH. These insights may help understand aerosol properties after cloud cycling in the atmosphere. 

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3. Decrease in Nucleated Particles and Cloud Condensation Nuclei Observed across a Range of Environments

   https://doi.org/10.1021/acs.est.5c18035  

   Park, Do-Hyeon; Laj, Paolo; Andrews, Elisabeth; Rose, Clémence; Benedetti, Angela; Kulmala, Markku; Zabala, Inés; Ahlberg, Erik; Alastuey, Andrés; Asmi, Eija; et al (May 2026, Environmental Science & Technology)

   Understanding new particle formation (NPF) and the fate of nanoparticles is crucial because of their close links to air quality, cloud formation, and climate. These effects vary spatially and temporally owing to diverse aerosol sources and their relatively short atmospheric lifetime. Here, we present a comprehensive analysis of long-term trends in NPF-associated nucleation-mode particles and cloud condensation nuclei (CCN) concentrations across diverse observation environments using quality-controlled particle number size distribution (PNSD) and CCN data from 37 sites, primarily from Global Atmosphere Watch (GAW) stations. We identify declining decadal trends in both NPF occurrences and nucleated particle concentrations across most site types, with the strongest declines in urban areas. We observe simultaneous reductions in both CCN concentrations and nucleation-mode particles, suggesting that newly formed particles are a potential source of CCN. This, in turn, suggests that cloud microphysical properties and radiative effects can be indirectly influenced through aerosol−cloud interactions that modify cloud droplet formation. These findings indicate that decreasing anthropogenic emissions could influence the climate forcing potential of aerosol−cloud interactions, with important implications for future climate projections. 

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4. Ion-induced cloud modulation through new particle formation and runaway cloud condensation nuclei production

   https://doi.org/10.1093/oxfclm/kgae018  

   Chandrakar, Kamal Kant; Cantrell, Will; Shaw, Raymond A (September 2024, Oxford Open Climate Change)

   Abstract Cloud formation in the Pi Convection–Cloud Chamber is achieved via ionization in humid conditions, without the injection of aerosol particles to serve as cloud condensation nuclei (CCN). Abundant ions, turbulence, and supersaturated water vapor combine to produce new particles, which grow to become CCN sized and eventually are activated to form clouds. Coupling between the new particle formation and cloud droplets causes predator-prey type oscillations in aerosol and droplet concentrations under turbulent conditions. Leading terms are identified in the budgets for Aitken and accumulation mode aerosols and for cloud droplets. The cloud coupling is proposed to be a result of cloud-induced runaway CCN production through aerosol scavenging. The experiments suggest potential applications to marine cloud brightening, in which ions rather than sea-salt aerosols are generated. 

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5. Aerosol interactions with deep convective clouds

   https://doi.org/10.1016/B978-0-12-819766-0.00001-8  

   Fan, Jiwen; Li, Zhanqing (January 2022, Elsevier)

   Deep convective clouds (DCCs) are associated with the vertical ascent of air from the lower to the upper atmosphere. They appear in various forms such as thunderstorms, supercells, and squall lines. These convective systems play important roles in the hydrological cycle, Earth’s radiative budget, and the general circulation of the atmosphere. Changes in aerosol (both cloud condensation nuclei and ice-nucleating particles) affect cloud microphysics and dynamics, and thereby influence convective intensity, precipitation, and the radiative effects of deep clouds and their cirrus anvils. However, the very complex dynamics and cloud microphysics of DCCs means that many of these processes are not yet accurately quantified in observations and models. This chapter outlines the main ways in which changes in aerosol affect the microphysical, dynamical, and radiative properties of DCCs. Aerosol interactions with DCCs depend on aerosol properties, storm dynamics, and meteorological conditions. When aerosol particles are light-absorbing, such as soot from industry or biomass burning, the aerosol radiative effects can alter the meteorological conditions under which DCCs form. These radiative effects modify temperature profiles and planetary boundary layer heights, thus changing atmospheric stability and circulation, and affecting the onset and development of DCCs. These large-scale effects, such as the effect of anthropogenic aerosol on the East and South Asian monsoons, can be simulated in coarse-resolution models. These processes are described in Chapter 13. This chapter is concerned with aerosol interactions with DCC systems ranging from individual clouds to mesoscale convective systems. Increases in cloud condensation nuclei (CCN) can enhance cloud droplet number concentrations and decrease droplet sizes, thereby narrowing the droplet size spectrum. For DCCs, a narrowed droplet size spectrum suppresses warm rain formation (rain derived from non-ice-phase processes), allowing the transport of more, smaller droplets to altitudes below 0°C. This may result in (i) freezing of more supercooled water, thereby enhancing latent heating from icerelated microphysical processes and invigorating storms (ice-phase invigoration); (ii) modification of ice-related microphysical processes, which changes cold pools, precipitation rates, and hailstone frequency and size; (iii) expansion of the mixed-phase zone and decreases in the cloud glaciation temperature; and (iv) slowing down of cloud dissipation, resulting in larger cloud cover and cloud depth in the stratiform and anvil regions due to numerous smaller ice particles. The increased cloud cover and cloud depth constitute an influence of aerosol on the cloud radiative effect. Reduced diurnal temperature variation has been observed and simulated as a result of enhanced daytime cooling and nighttime warming by expanded anvil cloud area in polluted environments. However, the global radiative effect of aerosol interactions with DCCs remains to be quantified. 

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