Comprehensive modelling study of ozonolysis of oleic acid aerosol based on real-time, online measurements of aerosol composition

The chemical composition of organic aerosols profoundly influences their atmospheric properties, but a detailed understanding of heterogeneous and in-particle reactivity is lacking. We present here a combined experimental and modeling study of the ozonolysis of oleic acid particles. An online mass spectrometry (MS) method, Extractive Electrospray Ionization (EESI), is used to follow the composition of the aerosol at a molecular level in real time; relative changes in the concentrations of both reactants and products are determined during aerosol aging. The results show evidence for multiple non-first-order reactions involving stabilized Criegee intermediates, including the formation of secondary ozonides and other oligomers. Offline liquid chromatography MS is used to confirm the online MS assignment of the monomeric and dimeric products. We explain the observed EESI-MS chemical composition changes, and chemical and physical data from previous studies, using a process-based aerosol chemistry simulation, the Pretty Good Aerosol Model (PG-AM). In particular, we extend previous studies of reactant loss by demonstrating success in reproducing the time dependence of product formation and the evolving particle size. This advance requires a comprehensive chemical scheme coupled to the partitioning of semivolatile products; relevant reaction and evaporation parameters have been refined using our new measurements in combination with PG-AM.This work was supported by the UK Natural Environment Research Council (NERC grant NE/I528277/1) and the European Research Council (ERC starting grant 279405 and the Atmospheric Chemistry Climate Interactions (ACCI) project, grant 267760). PTG thanks NCAS Climate for support

Assessing the Accuracy of Complex Refractive Index Retrievals from Single Aerosol Particle Cavity Ring-Down Spectroscopy

<p>Cavity ring-down spectroscopy (CRDS) of single, optically manipulated aerosol particles affords quantitative retrieval of refractive indices for particles of fixed or evolving composition with high precision. Here, we quantify the accuracy with which refractive index determinations can be made by CRDS for single particles confined within the core of a Bessel laser beam and how that accuracy is degraded as the particle size is progressively reduced from the coarse mode (>1 μm radius) to the accumulation mode (<500 nm radius) regime. We apply generalized Lorenz–Mie theory to the intra-cavity standing wave to explore the effect of particle absorption on the distribution of extinction cross section determinations resulting from stochastic particle motion in the Bessel beam trap. The analysis provides an assessment of the accuracy with which the real, <i>n</i>, and imaginary, κ, components of the refractive index can be determined for a single aerosol particle.</p> <p>Published with license by American Association for Aerosol Research</p> <p><a href="https://www.tandfonline.com/pb-assets/tandf/Migrated/UAST_VideoAbstract_Transcript.pdf" target="_blank">Read the transcript</a></p> <p><a href="https://vimeo.com/263371383" target="_blank">Watch the video on Vimeo</a></p

A purely kinetic description of the evaporation of water droplets

The process of water evaporation, although deeply studied, does not enjoy a kinetic description that captures known physics and can be integrated with other detailed processes such as drying of catalytic membranes embedded in vapor-fed devices and chemical reactions in aerosol whose volumes are changing dynamically. In this work, we present a simple, three-step kinetic model for water evaporation that is based on theory and validated by using well-established thermodynamic models of droplet size as a function of time, temperature, and relative humidity as well as data from time-resolved measurements of evaporating droplet size. The kinetic mechanism for evaporation is a combination of two limiting processes occurring in the highly dynamic liquid-vapor interfacial region: direct first order desorption of a single water molecule and desorption resulting from a local fluctuation, described using third order kinetics. The model reproduces data over a range of relative humidities and temperatures only if the interface that separates bulk water from gas phase water has a finite width, consistent with previous experimental and theoretical studies. The influence of droplet cooling during rapid evaporation on the kinetics is discussed; discrepancies between the various models point to the need for additional experimental data to identify their origin

Efficacy of face coverings in reducing transmission of COVID-19:Calculations based on models of droplet capture

In the COVID--19 pandemic, among the more controversial issues is the use of masks and face coverings. Much of the concern boils down to the question -- just how effective are face coverings? One means to address this question is to review our understanding of the physical mechanisms by which masks and coverings operate -- steric interception, inertial impaction, diffusion and electrostatic capture. We enquire as to what extent these can be used to predict the efficacy of coverings. We combine the predictions of the models of these mechanisms which exist in the filtration literature and compare the predictions with recent experiments and lattice Boltzmann simulations, and find reasonable agreement with the former and good agreement with the latter. Building on these results, we explore the parameter space for woven cotton fabrics to show that three-layered cloth masks can be constructed with comparable filtration performance to surgical masks under ideal conditions. Reusable cloth masks thus present an environmentally friendly alternative to surgical masks so long as the face seal is adequate enough to minimise leakage.Comment: 26 pages (13 + references, 10 pages supplementary), 10 figures (8 in main text, 2 in SI); accepted version, to appear in Physics of Fluids' special issue "Flow and the Virus

Probing the Evaporation Dynamics of Ethanol/Gasoline Biofuel Blends Using Single Droplet Manipulation Techniques

Peer reviewedPublisher PD

Optical extinction efficiency measurements on fine and accumulation mode aerosol using single particle cavity ring-down spectroscopy

We report a new single aerosol particle approach using cavity ringdown spectroscopy to accurately determine optical extinction cross sections at multiple wavelengths.</p