Qian Xiao

This study characterizes the spatial and vertical nature of aerosol hygroscopicity in Southeast Asia and relates it to aerosol composition and sources. Aerosol hygroscopicity via the light scattering hygroscopic growth factor, f(RH), is calculated from the amplification of PM₅ (particulate matter with a particle diameter, D_p, 2Ex) between August and October 2019 over the northwest tropical Pacific. Median f(RH) is low (1.26 with lower to upper quartiles of 1.05 to 1.43) like polluted environments, due to the dominance of the mixture of organic carbon and elemental carbon. The f(RH) is lowest due to smoke from the Maritime Continent (MC) during its peak biomass burning season, coincident with high carbon monoxide concentrations (>0.25 ppm) and pronounced levels of accumulation-mode particles and organic mass fractions. The highest f(RH) values are linked to coarser particles from the West Pacific and aged biomass burning particles in the region farthest away from the MC, where f(RH) values are lower than typical polluted marine environments. Convective transport and associated cloud processing in these regions decrease and increase hygroscopicity aloft in cases with transported air masses exhibiting increased organic and sulfate mass fractions, respectively. An evaluation of the Community Atmosphere Model with Chemistry (CAM-chem) for cases of vertical transport showed the underrepresentation of organics, resulting in overestimated modeled aerosol hygroscopicity. These findings on aerosol hygroscopicity can help to improve aerosol representation in models and the understanding of cloud formation.

This study characterizes the spatial and vertical nature of aerosol hygroscopicity in Southeast Asia and relates it to aerosol composition and sources. Aerosol hygroscopicity via the light scattering hygroscopic growth factor, f(RH), is calculated from the amplification of PM₅ aerosol (D_p < 5 μm) scattering measurements from < 40 % to 82 % relative humidity during the Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP²Ex) between August to October 2019 over the northwest tropical Pacific. Median f(RH) is relatively low (1.26 with lower to upper quartiles of 1.05 to 1.43) like polluted environments, due to the dominance of the mixture of organic carbon and elemental carbon. The f(RH) is lowest due to smoke from the Maritime Continent (MC) during its peak biomass burning season, coincident with high carbon monoxide concentrations (> 0.25 ppm) and pronounced levels of accumulation mode particles and organic mass fractions. The highest f(RH) values are linked to coarser particles from the West Pacific and aged biomass burning particles in the region farthest away from the MC, where f(RH) values are lower than typical polluted marine environments. Convective transport and associated cloud processing in these regions decrease and increase hygroscopicity aloft in cases with transported air masses exhibiting increased organic and sulfate mass fractions, respectively. An evaluation of a global chemical transport model (CAM-chem) for cases of vertical transport showed the underrepresentation of organics resulting in overestimated modeled aerosol hygroscopicity. These findings on aerosol hygroscopicity can help to improve aerosol representation in models and the understanding of cloud formation.

Improving parameterizations of convective microphysics in Earth system models (ESMs) requires well-constrained cases suitable for scaling between cloud-resolving models and ESMs. We propose a benchmark large eddy simulation (LES) cumulus congestus case study from the NASA Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP²Ex) and demonstrate its observational constraints using novel polarimetric retrievals and in situ cloud microphysics measurements. Simulations using bulk and bin microphysics with observed aerosol input are compared to cloud-top retrievals of cloud droplet effective radius (R_eff) and number concentration (N_d) from the airborne Research Scanning Polarimeter (RSP). The bulk scheme reasonably reproduces characteristic profiles of cloud-top N_d that decrease with altitude, while the bin simulation realizes greater discrepancies due to weaker precipitation formation. The N_d profile is strongly sensitive to the collision-coalescence process and the vertically resolved aerosol distribution, but appears well-constrained, whereas a persistent low-bias in R_eff is evident in both schemes. Comparison of simulated and in situ droplet size distributions (DSDs) show that low-biased R_eff originates from a cloud droplet mode that is too narrow relative to observations. Finally, a thermal-tracking framework demonstrates that the dilution of N_d throughout a thermal's lifetime is heavily determined by collision-coalescence and the height-varying aerosol distribution, and that in the absence of these, the impact of entrainment on diluting N_d is largely offset by continuous aerosol activation. Implications for developing warm-phase convective microphysics schemes for ESMs, evaluation of cumulus congestus using single column model versions of ESMs, and translating results to global, space-based polarimetry platforms are discussed.

Nucleation in the free troposphere (FT) and subsequent growth of new particles represent a globally important source of cloud condensation nuclei (CCN). Whereas new particle formation (NPF) has been shown to occur frequently in the upper troposphere over tropical oceans, there have been few studies of NPF at lower altitudes. In addition, the impact of urban emissions and biomass burning on the NPF in tropical marine FT remains poorly understood. In this study, we examine NPF in the lower and mid-troposphere (3–8.5 km) over the tropical ocean and coastal region using airborne measurements during the recent Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex). NPF was mostly observed above 5.5 km and coincided with elevated relative humidity (RH) and reduced condensation sink (CS), suggesting that NPF occurs in convective cloud outflow. The frequency of NPF increases with altitude, reaching ∼ 50 % above 8 km. An abrupt decrease in NPF frequency coincides with early monsoon transition and is attributed to increased CS resulting from reduced convective activity and more frequent transport of aged urban plumes. Surprisingly, a large fraction of NPF events in background air were observed in the early morning, and the NPF is likely made possible by very low CS despite low actinic flux. Convectively detrained biomass-burning plumes and fresh urban emissions enhance NPF as a result of elevated precursor concentrations and scavenging of pre-existing particles. In contrast, NPF is suppressed in aged urban plumes where the reactive precursors are mostly consumed, while CS remains relatively high. This study shows a strong impact of urban and biomass-burning emissions on the NPF in tropical marine FT. The results also illustrate the competing influences of different variables and interactions among anthropogenic emissions, convective clouds, and meteorology, which lead to NPF under a variety of conditions in tropical marine environments.