Airborne observations during KORUS-AQ show that aerosol optical depths are more spatially self-consistent than aerosol intensive properties

Abstract

Aerosol particles can be emitted, transported, removed, or transformed, leading to aerosol variability at scales impacting the climate (days to years and over hundreds of kilometers) or the air quality (hours to days and from meters to hundreds of kilometers). We present the temporal and spatial scales of changes in AOD (aerosol optical depth) and aerosol size (using Ångström exponent – AE; fine-mode fraction – FMF) over Korea during the 2016 KORUS-AQ (KORea–US Air Quality) atmospheric experiment. We use measurements and retrievals of aerosol optical properties from airborne instruments for remote sensing (4STAR; Spectrometers for Sky-Scanning Sun-Tracking Atmospheric Research) and in situ (LARGE; NASA Langley Aerosol Research Group Experiment) on board the NASA DC-8 and geostationary satellites (GOCI; Geostationary Ocean Color Imager; Yonsei aerosol retrieval – YAER, version 2) as well as from reanalysis (MERRA-2; Modern-Era Retrospective Analysis for Research and Applications, version 2). Measurements from 4STAR when flying below 1000 m show an average AOD at 501 nm of 0.36 and an average AE of 1.11 with large standard deviation (0.12 and 0.15 for AOD and AE, respectively), likely due to mixing of different aerosol types (fine and coarse mode). The majority of AOD due to fine-mode aerosol is observed at altitudes lower than 2 km. Even though there are large variations, for 18 out of the 20 flight days, the column AOD measurements by 4STAR along the NASA DC-8 flight trajectories match the South Korean regional average derived from GOCI. GOCI-derived FMF, which was found to be slightly low compared to AErosol RObotic NETwork (AERONET) sites (Choi et al., 2018), is lower than 4STAR's observations during KORUS-AQ. Understanding the variability of aerosols helps reduce uncertainties in the aerosol direct radiative effect by quantifying the errors due to interpolating between sparse aerosol observation sites or modeled pixels, potentially reducing uncertainties in the upcoming observational capabilities. We observed that, contrary to the prevalent understanding, AE and FMF are more spatially variable than AOD during KORUS-AQ, even when accounting for potential sampling biases by using Monte Carlo resampling. Averaging between measurements and models for the entire KORUS-AQ period, the reduction in correlation by 15 % is 65.0 km for AOD and shorter at 22.7 km for AE. While there are observational and model differences, the predominant factor influencing spatial–temporal homogeneity is the meteorological period. High spatiotemporal variability occurs during the dynamic period (25–31 May), and low spatiotemporal variability occurs during the blocking pattern (1–7 June). While AOD and FMF / AE are interrelated, the spatial variability and relative variability of these parameters in this study indicate that microphysical processes vary at scales shorter than aerosol concentration processes at which microphysical processes such as aerosol particle formation, growth, and coagulation mostly impact the dominant aerosol size (characterized by, e.g., FMF / AE) and to some degree AOD. In addition to impacting aerosol size, aerosol concentration processes such as aerosol emission, transport, and removal mostly impact the AOD.