Reply on RC1

Abstract

Understanding the gas-particle partitioning of semivolatile organic compounds (SVOCs) is of crucial importance in the accurate representation of the global budget of atmospheric organic aerosols. In this study, we quantified the gas- vs. particle-phase fractions of a large number of SVOCs in real time in an urban area of East China with the use of a CHemical Analysis of aeRosols ONline (CHARON) inlet coupled to a high resolution Proton Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-ToF-MS). We demonstrated the use of the CHARON inlet for highly efficient collection of particulate SVOCs while maintaining the intact molecular structures of these compounds. The collected month-long dataset with hourly resolution allows us to examine the gas-particle partitioning behaviors of a variety of SVOCs under different ambient conditions. By comparing the measurements with model predictions using the instantaneous equilibrium partitioning theory, we found that the dissociation of large parent molecules during the PTR ionization process likely introduces large uncertainties to the measured gas- vs. particle-phase fractions of less oxidized SVOCs, and therefore, caution should be taken when linking the molecular composition to the particle volatility when interpreting the PTR-ToF-MS data. Our analysis suggests that understanding the fragmentation mechanism of oxidized SVOCs and accounting for the neutral losses of small moieties during the molecular feature extraction from the raw mass spectra could reduce, to a large extent, the uncertainties associated with the gas-particle partitioning measurement of SVOCs in the ambient atmosphere.