A portable, four-wavelength, single-cell photoacoustic spectrometer for ambient aerosol absorption

ABSTRACT

Aerosols directly affect Earth's climate by scattering and absorbing solar radiation. Although they are ubiquitous in Earth's atmosphere, direct, in situ, wavelength-resolved measurements of aerosol optical properties remain challenging. As a result, the so-called aerosol direct effects are one of the largest uncertainties in predictions of Earth's future climate, and new instrumentation is needed to provide measurements of the absorption of sunlight by atmospheric particles. We have developed a portable, four-wavelength, single-cell photoacoustic spectrometer for simultaneous measurement of aerosol absorption at 406, 532, 662, and 785 nm, with an additional extinction measurement at 662 nm via a built-in cavity ringdown spectrometer. The instrument, dubbed MultiPAS-IV, is compact, robust, has low power requirements, and utilizes a multipass optical arrangement to achieve typical detection limits of 0.6–0.7 Mm⁻¹ for absorption (2σ, 2-min average). Tests with nigrosin aerosols show agreement with Mie theory calculations to within 2%, and comparison with a 7-wavelength aethalometer shows good correlation for ambient (Athens, GA, USA) aerosols. We demonstrate the utility of the broad spectral coverage and sensitivity of the MultiPAS-IV for calculating the absorption Ångström exponent of black carbon (AAE_BC, median value of 0.70) in ambient aerosols and use this value to derive the brown carbon contributions to absorption at 406 nm (43%) and 532 nm (13%) and its wavelength dependence (AAE_BrC = 6.3).

Copyright © 2018 American Association for Aerosol Research

EDITOR:

• Pramod Kulkarni

Acknowledgments

The authors wish to thank Prof. Rawad Saleh (School of Engineering, University of Georgia) for loan of the aethalometer, atomizer, and a diffusion drier used in this study and the UGA Instrument Shop for construction of the PAS and CRD cells.

Funding

The authors gratefully acknowledge support for this work by the National Science Foundation, Division of Atmospheric and Geospace Sciences (AGS-1241621 and AGS-1638307).