Initial pH Governs Secondary Organic Aerosol Phase State and Morphology after Uptake of Isoprene Epoxydiols (IEPDX)

Aerosol acidity increases secondary organic aerosol (SOA) formed from the reactive uptake of isoprene-derived epoxydiols (IEPDX) by enhancing condensed-phase reactions within sulfate-containing submicron particles, leading to low-volatility organic products. However, the link between the initial aerosol acidity and the resulting physicochemical properties of IEPDX-derived SOA remains uncertain. Herein, we show distinct differences in the morphology, phase state, and chemical composition of individual organic-inorganic mixed particles after IEPDX uptake to ammonium sulfate particles with different initial atmospherically relevant acidities (pH = 1, 3, and 5). Physicochemical properties were characterized via atomic force microscopy coupled with photothermal infrared spectroscopy (AFM-PTIR) and Raman microspectroscopy. Compared to less acidic particles (pH 3 and 5), reactive uptake of IEPDX to the most acidic particles (pH 1) resulted in 50% more organosulfate formation, clearer phase separation (core-shell), and more irregularly shaped morphologies, suggesting that the organic phase transitioned to semisolid or solid. This study highlights that initial aerosol acidity may govern the subsequent aerosol physicochemical properties, such as viscosity and morphology, following the multiphase chemical reactions of IEPDX. These results can be used in future studies to improve model parameterizations of SOA formation from IEPDX and its properties, toward the goal of bridging predictions and atmospheric observations.