Organic aerosol particles are known to often absorb/desorb water continuously with change in gas phase relative humidity (RH) without crystallization. Indeed, the prevalence of metastable ultraviscous liquid or amorphous phases in aerosol is well-established with solutes often far exceeding bulk phase solubility limits. Particles are expected to become increasingly viscous with drying, a consequence of the plasticizing effect of water. We report here measurements of the variation in aerosol particle viscosity with RH (equal to condensed phase water activity) for a range of organic solutes including alcohols (diols to hexols), saccharides (mono-, di-, and tri-), and carboxylic acids (di-, tri-, and mixtures). Particle viscosities are measured over a wide range (10 to 10 Pa s) using aerosol optical tweezers, inferring the viscosity from the time scale for a composite particle to relax to a perfect sphere following the coalescence of two particles. Aerosol measurements compare well with bulk phase studies (well-within an order of magnitude deviation at worst) over ranges of water activity accessible to both. Predictions of pure component viscosity from group contribution approaches combined with either nonideal or ideal mixing reproduce the RH-dependent trends particularly well for the alcohol, di-, and tricarboxylic acid systems extending up to viscosities of 10 Pa s. By contrast, predictions overestimate the viscosity by many orders of magnitude for the mono-, di-, and trisaccharide systems, components for which the pure component subcooled melt viscosities are ≫10 Pa s. When combined with a typical scheme for simulating the oxidation of α-pinene, a typical atmospheric pathway to secondary organic aerosol (SOA), these predictive tools suggest that the pure component viscosities are less than 10 Pa s for ∼97% of the 50,000 chemical products included in the scheme. These component viscosities are consistent with the conclusion that the viscosity of α-pinene SOA is most likely in the range 10 to 10 Pa s. Potential improvements to the group contribution predictive tools for pure component viscosities are considered.

The severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) pandemic has resulted in an unprecedented shutdown in social and economic activity, with the cultural sector particularly severely affected. Restrictions on musical performances have arisen from a perception that there is a significantly higher risk of aerosol production from singing than speaking, based upon high-profile A c c e p t e d M a n u s c r i p texamples of clusters of COVID-19 following choral rehearsals. However, comparing aerosol generation from different types of vocalization, including singing, across a range of volumes is a rapidly evolving area of research. Here, we measured aerosols from singing, speaking and breathing from a large cohort of 25 professional singers in a range of musical genres in a zero-background environment, allowing unequivocal attribution of aerosol production to specific vocalizations. We do not assess the relative volumes at which people speak and sing. However, both showed steep increases in mass concentration with increase in loudness (spanning a factor of 20-30 across the dynamic range measured, p<0.001). At the quietest volume (50 to 60 dBA), neither singing (p=0.19) nor speaking (p=0.20) were significantly different to breathing. At the loudest volume (90 to 100 dBA), a statistically significant difference (p<0.001) was observed between singing and speaking, but with singing only generating a factor of between 1.5 and 3.4 more aerosol mass. Guidelines for musical performances should be based on the loudness and duration of the vocalization, the number of participants and the environment in which the activity occurs, rather than the type of vocalization.Mitigations such as the use of amplification and increased attention to ventilation should be employed where practicable.

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We present an algorithm that can be used to simultaneously determine the radius and the refractive index (with dispersion) of a spherical, homogeneous particle. This is accomplished by fitting characteristic resonances calculated using Mie scattering coefficients to the measured whispering gallery mode resonances. The advantage of this algorithm over those that have been presented previously is that a large portion of the search can be reduced to two dimensions (a search that includes radius and refractive index with dispersion will always be at least three dimensions). Using this algorithm, we analyze two large sets of cavity-enhanced Raman spectra from optically trapped aerosol particles. The speed of the algorithm allows for best fits to be found in real time. Precision is found to be limited by the resolution of the spectrograph.