05 May 2022
05 May 2022

Constraining the particle-scale diversity of black carbon light absorption using a unified framework

Payton Beeler and Rajan Chakrabarty Payton Beeler and Rajan Chakrabarty
  • Center for Aerosol Science and Engineering, Department of Energy, Environmental and Chemical Engineering, Washington University in St. Louis, St. Louis, MO 63130

Abstract. Atmospheric black carbon (BC), the strongest absorber of visible solar radiation in the atmosphere, manifests across a wide spectrum of morphologies and compositional heterogeneity. Phenomenologically, the distribution of BC among diverse particles of varied composition gives rise to enhancement of its light absorption capabilities by over twofold in comparison to that of nascent or unmixed homogeneous BC. This situation has challenged the modeling community to consider the full complexity and diversity of BC on a per-particle basis for accurate estimation of its light absorption. The conventionally adopted core-shell approximation, although computationally inexpensive, is inadequate in not only estimating but also capturing absorption trends for ambient BC. Here we develop a unified framework that encompasses the complex diversity in BC morphology and composition using a single metric, the phase shift parameter (𝜌BC), which quantifies how much phase shift the incoming light waves encounter across a particle compared to that in its absence. We systematically investigate the variations in 𝜌BC across the multi-space distribution of BC morphology, mixing-state, mass, and composition as reported by field and laboratory observations. We find that 𝜌BC > 1 leads to decreased absorption enhancement by BC, which explains the weaker absorption enhancements observed in certain regional BC compared to laboratory results of similar mixing state. We formulate universal scaling laws centered on 𝜌BC and provide physics-based insights regarding core-shell approximation overestimating BC light absorption. We conclude by packaging our framework in an open-source Python application to facilitate community-level use in future BC-related research. The package has two main functionalities. The first functionality is for forward problems, where experimentally measured BC mixing state and assumed BC morphology are input, and the aerosol absorption properties are output. The second functionality is for inverse problems, where experimentally measured BC mixing state and absorption are input, and the morphology of BC is returned. Further, if absorption is measured at multiple wavelengths, the package facilitates the estimation of imaginary refractive index of coating materials by combining the forward and inverse procedures. Our framework thus provides a computationally inexpensive source for calculation of absorption by BC, and can be used to constrain light absorption throughout the atmospheric lifetime of BC.

Payton Beeler and Rajan Chakrabarty

Status: final response (author comments only)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on egusphere-2022-163', Anonymous Referee #1, 25 May 2022
    • AC1: 'Reply on RC1', Rajan Chakrabarty, 15 Sep 2022
  • CC1: 'Black-carbon phase shift parameter and soot restructuring', J. C. Corbin, 15 Jun 2022
  • RC2: 'Comment on egusphere-2022-163', Anonymous Referee #3, 05 Jul 2022

Payton Beeler and Rajan Chakrabarty

Payton Beeler and Rajan Chakrabarty


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Short summary
Understanding and parameterizing the influences of black carbon (BC) particle morphology and compositional heterogeneity on its light absorption is a fundamental problem. We develop scaling laws using a single unifying parameter that effectively encompasses the large-scale diversity observed in BC light absorption on a per particle basis. These laws help to reconcile the disparities between field observations and model predictions. Our framework is packaged in an open-source Python application.