Measuring the Chemical Evolution of Levitated Particles: A Study on the Evaporation of Multicomponent Organic Aerosol.

Single-particle levitation methods provide an effective platform for probing the physical properties of atmospheric aerosol via micrometer-sized particles. Until recently, chemical composition measurements on levitated particles were limited to spectroscopy, yielding only basic chemical information. Here, we describe, benchmark, and discuss the applications of an approach for probing the physical properties and chemical composition of single levitated particles using high-resolution mass spectrometry (MS). Using a linear quadrupole electrodynamic balance (LQ-EDB) coupled to paper spray mass spectrometry, we report accurate measurements of the evolving size within 5 nm (using broadband light scattering) and relative composition (using MS) of evaporating multicomponent levitated particles in real time. Measurements of the evaporation dynamics of semivolatile organic particles containing a range of n-ethylene glycols (n = 3, 4, and 6) in various binary and ternary mixtures were made under dry conditions and compared with predictions from a gas-phase diffusion evaporation model. Under assumptions of ideal mixing, excellent agreement for both size and composition evolution between measurements and models were obtained for these mixtures. At increased relative humidity, the presence of water in particles causes the assumption of ideality to break down, and the evaporative mass flux becomes a function of the mole fraction and activity coefficient. Through compositionally resolved evaporation measurements and thermodynamic models, we characterize the activity of organic components in multicomponent particles. Our results demonstrate that the LQ-EDB-MS platform can identify time-dependent size and compositional changes with high precision and reproducibility, yielding an effective methodology for future studies on chemical aging and gas-particle partitioning in suspended particles.