Dynamic viscosity mapping of the oxidation of squalene aerosol particles.
File(s)PCCPsqualene_supplementary_revision0510_final.pdf (1.51 MB) Manuscript_revision.pdf (988.44 KB)
Supporting information
Accepted version
Author(s)
Type
Journal Article
Abstract
Organic aerosols (OAs) play important roles in multiple atmospheric processes, including climate change, and can impact human health. The physico-chemical properties of OAs are important for all these processes and can evolve through reactions with various atmospheric components, including oxidants. The dynamic nature of these reactions makes it challenging to obtain a true representation of their composition and surface chemistry. Here we investigate the microscopic viscosity of the model OA composed of squalene, undergoing chemical aging. We employ Fluorescent Lifetime Imaging Microscopy (FLIM) in conjunction with viscosity sensitive probes termed molecular rotors, in order to image the changes in microviscosity in real time during oxidation with ozone and hydroxyl radicals, which are two key oxidising species in the troposphere. We also recorded the Raman spectra of the levitated particles to follow the reactivity during particle ozonolysis. The levitation of droplets was achieved via optical trapping that enabled simultaneous levitation and measurement via FLIM or Raman spectroscopy and allowed the true aerosol phase to be probed. Our data revealed a very significant increase in viscosity of the levitated squalene droplets upon ozonolysis, following their transformation from the liquid to solid phase that was not observable when the oxidation was carried out on coverslip mounted droplets. FLIM imaging with sub-micron spatial resolution also revealed spatial heterogeneity in the viscosity distribution of oxidised droplets. Overall, a combination of molecular rotors, FLIM and optical trapping is able to provide powerful insights into OA chemistry and the microscopic structure that enables the dynamic monitoring of microscopic viscosity in aerosol particles in their true phase.
Date Issued
2016-10-12
Date Acceptance
2016-10-12
Citation
Physical Chemistry Chemical Physics, 2016, 18 (44), pp.30385-30393
ISSN
1463-9084
Publisher
Royal Society of Chemistry
Start Page
30385
End Page
30393
Journal / Book Title
Physical Chemistry Chemical Physics
Volume
18
Issue
44
Copyright Statement
© 2016 The Owner Societies
Sponsor
Engineering & Physical Science Research Council (EPSRC)
Engineering & Physical Science Research Council (EPSRC)
Engineering & Physical Science Research Council (EPSRC)
Identifier
http://www.ncbi.nlm.nih.gov/pubmed/27781216
Grant Number
EP/I003983/1
EP/K503381/1
EP/K030760/1
Subjects
Chemical Physics
02 Physical Sciences
03 Chemical Sciences
Publication Status
Published
Coverage Spatial
England