Abstract

Abstract. Particle morphology is an important parameter affecting aerosol optical properties that are relevant to climate and air quality, yet it is poorly constrained due to sparse in situ measurements. Biomass burning is a large source of aerosol that generates particles with different morphologies. Quantifying the optical contributions of non-spherical aerosol populations is critical for accurate radiative transfer models, and for correctly interpreting remote sensing data. We deployed a laser imaging nephelometer at the Missoula Fire Sciences Laboratory to sample biomass burning aerosol from controlled fires during the FIREX intensive laboratory study. The laser imaging nephelometer measures the unpolarized scattering phase function of an aerosol ensemble using diode lasers at 375 and 405 nm. Scattered light from the bulk aerosol in the instrument is imaged onto a charge-coupled device (CCD) using a wide-angle field-of-view lens, which allows for measurements at 4–175∘ scattering angle with ∼ 0.5∘ angular resolution. Along with a suite of other instruments, the laser imaging nephelometer sampled fresh smoke emissions both directly and after removal of volatile components with a thermodenuder at 250 ∘C. The total integrated aerosol scattering signal agreed with both a cavity ring-down photoacoustic spectrometer system and a traditional integrating nephelometer within instrumental uncertainties. We compare the measured scattering phase functions at 405 nm to theoretical models for spherical (Mie) and fractal (Rayleigh–Debye–Gans) particle morphologies based on the size distribution reported by an optical particle counter. Results from representative fires demonstrate that particle morphology can vary dramatically for different fuel types. In some cases, the measured phase function cannot be described using Mie theory. This study demonstrates the capabilities of the laser imaging nephelometer instrument to provide realtime, in situ information about dominant particle morphology, which is vital for understanding remote sensing data and accurately describing the aerosol population in radiative transfer calculations.

Highlights

  • Atmospheric aerosol particles absorb and scatter light, strongly influencing Earth’s climate (Davidson et al, 2005; Stocker et al, 2013)

  • Aerosol morphology is important in implementing global radiative transfer calculations, since the directionality of scattered light from aerosol relative to the solar zenith angle will vary with particle shape (Kahnert and Devasthale, 2011)

  • While the phase functions modeled using RDG are sensitive to these values, as well as the monomer diameter, a comprehensive analysis of the full range of possible RDG parameterization is beyond the scope of this paper; rather, here we present an initial “best guess” of the RDG parameterization based on the limited literature on biomass burning-produced soot and scanning electron microscope (SEM) micrographs

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Summary

Introduction

Atmospheric aerosol particles absorb and scatter light, strongly influencing Earth’s climate (Davidson et al, 2005; Stocker et al, 2013). The first polarized imaging nephelometer used for field measurements employed a wide-angle lens and charge-coupled device (CCD) to record the scattering phase function under two orthogonal linear polarization conditions at three wavelengths (473, 532, and 671 nm) and derive both the phase function and degree of linear polarization across the visible spectral region (Dolgos and Martins, 2014; Espinosa et al, 2017) This instrument was deployed on the NASA DC8 aircraft for the Deep Convective Clouds and Chemistry (DC3) campaign in 2012 (Barth et al, 2015) and the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) mission in 2014 (Toon et al, 2016). We compare the retrieved phase functions to models of spherical and fractal particles to provide direct verification that the predominant morphology of the freshly emitted particles varied by fuel type, and demonstrate the ability to assign particle morphology from the phase function

Description of the laser imaging nephelometer
Image processing for the laser imaging nephelometer
Aerosol sampling at the Fire Sciences Laboratory
Parameterizations of phase functions from particle morphology
Precision and accuracy of the scattering phase function
Comparison of integrated scattering
Summary and conclusions
Full Text
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