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Light scattering and extinction measurements combined with laser-induced incandescence for the real-time determination of soot mass absorption cross-section.
  • Jonathan Thompson
Jonathan Thompson
Texas Tech University

Corresponding Author:[email protected]

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Abstract

An aerosol albedometer was combined with laser-induced incandescence (LII) to achieve simultaneous measurements of aerosol scattering, extinction coefficient, and soot mass concentration. Frequency doubling of a Nd:YAG laser line resulted in a colinear beam of both λ = 532 and 1064 nm. The green beam was used to perform cavity ring-down spectroscopy (CRDS), with simultaneous measurements of scattering coefficient made through use of a reciprocal sphere nephelometer. The 1064 nm beam was selected and directed into a second integrating sphere and used for LII of light-absorbing kerosene lamp soot. Thermal denuder experiments showed the LII signals were not affected by the particle mixing state when laser peak power was 1.5–2.5 MW. The combined measurements of optical properties and soot mass concentration allowed determination of mass absorption cross section (M.A.C., m2/g) with 1 min time resolution when soot concentrations were in the low microgram per cubic meter range. Fresh kerosene nanosphere soot (ns-soot) exhibited a mean M.A.C and standard deviation of 9.3 ± 2.7 m2/g while limited measurements on dry ambient aerosol yielded an average of 8.2 ± 5.9 m2/g when soot was >0.25 μg/m3. The method also detected increases in M.A.C. values associated with enhanced light absorption when polydisperse, laboratory-generated ns-soot particles were embedded within or coated with ammonium nitrate, ammonium sulfate, and glycerol. Glycerol coatings produced the largest fractional increase in M.A.C. (1.41-fold increase), while solid coatings of ammonium sulfate and ammonium nitrate produced increases of 1.10 and 1.06, respectively. Fresh, ns-soot did not exhibit increased M.A.C. at high relative humidity (RH); however, lab-generated soot coated with ammonium nitrate and held at 85% RH exhibited M.A.C. values nearly double the low-humidity case. The hybrid instrument for simultaneously tracking soot mass concentration and aerosol optical properties in real time is a valuable tool for probing enhanced absorption by soot at atmospherically relevant concentrations.