Cloud response to co-condensation of water and organic vapors over the boreal forest
Authors: Heikkinen Liine , Partridge Daniel G. , Huang Wei , Blichner Sara , Ranjan Rahul , Tovazzi Emanuele , Petäjä Tuukka , Mohr Claudia , Riipinen Ilona 
Published: February 2023

Abstract. Accounting for the condensation of organic vapors along with water vapor (co-condensation) has been shown in adiabatic cloud parcel model (CPM) simulations to enhance the number of aerosol particles that activate to form cloud droplets. The boreal forest is an important source of biogenic organic vapors, but the role of these vapors in co-condensation has not been systematically investigated. In this work, the environmental conditions under which strong co-condensation -driven cloud droplet number enhancements would be expected over the boreal biome are identified. Recent measurement technology, specifically the Filter Inlet for Gases and AEROsols (FIGAERO) coupled to an iodide-adduct Chemical Ionization Mass Spectrometer (I-CIMS), is utilized to construct a volatility distribution of the boreal atmospheric organics. Then, a suite of CPM simulations initialized with a comprehensive set of concurrent aerosol observations collected in the boreal forest of Finland during Spring 2014 is performed. The degree to which co-condensation impacts droplet formation in the model is shown to be dependent on the initialization of the updraft velocity, aerosol size distribution, organic vapor concentration and the volatility distribution. The predicted median enhancement in cloud droplet number concentration (CDNC) due to accounting for the co-condensation of water and organics is 20 % (interquartile range 29–14 %). This corresponds to activating particles 12–16 nm smaller in dry diameter, that would otherwise remain as interstitial aerosol. The highest CDNC enhancements (ΔCDNC) are predicted in the presence of a nascent ultrafine aerosol mode with a geometric mean diameter of ~40 nm and no clear Hoppel minimum, indicative of pristine environments with a source of ultrafine particles (e.g., via new particle formation processes). Such aerosol size distributions are observed 30–40 % of the time in the studied boreal forest environment in spring and fall when new particle formation frequency is the highest (six years of statistics). Five years of UK Earth System Model (UKESM1) simulations are further used to evaluate the frequencies to which such distributions are experienced by an Earth System Model over the whole boreal biome. The frequencies are substantially lower than those observed at the boreal forest measurement site (< 6 % of the time) and the positive values, peaking in spring, are modeled only over Fennoscandia and western parts of Siberia. For the aerosol size distribution regime simulated by UKESM1, offline simulations with the adiabatic parcel model reveal the ΔCDNC to be sensitive to the concentrations of semi-volatile and some intermediate-volatility organic compounds (SVOCs and IVOCs). The magnitudes of ΔCDNC remain less affected by the more volatile vapors such as formic acid and extremely low and low volatility organic compounds (ELVOCs and LVOCs) in the CPM simulations. The reasons for this are that most volatile organic vapors condense inefficiently due to their high volatility below cloud base and the concentrations of LVOCs and ELVOCs are too low to gain significant concentrations of soluble mass to reduce critical supersaturations needed for droplet activation. Suppression of the critical supersaturation caused by organic condensation is the main driver of the modeled ΔCDNC. The results highlight the potential significance of co-condensation in pristine boreal environments close to sources of fresh ultrafine particles. For accurate predictions of co-condensation effects on CDNC, the representation of the aerosol size distribution is of essence. Further studies targeted at finding observational evidence and constraints for co-condensation in the field are encouraged.