Scaling Laws for Light Absorption Enhancement Due to Nonrefractory Coating of Atmospheric Black Carbon Aerosol.

Black carbon (BC) aerosol, the strongest absorber of visible solar radiation in the atmosphere, contributes to a large uncertainty in direct radiative forcing estimates. A primary reason for this uncertainty is inaccurate parametrizations of the BC mass absorption cross section (MAC_{BC}) and its enhancement factor (E_{MAC_{BC}})-resulting from internal mixing with nonrefractory and nonlight absorbing materials-in climate models. Here, applying scaling theory to numerically exact electromagnetic calculations of simulated BC particles and observational data on BC light absorption, we show that MAC_{BC} and E_{MAC_{BC}} evolve with increasing internal mixing ratios in simple power-law exponents of 1/3. Remarkably, MAC_{BC} remains inversely proportional to the wavelength of light at any mixing ratio. When mixing states are represented using mass-equivalent core-shell spheres, as is done in current climate models, it results in significant underprediction of MAC_{BC}. We elucidate the responsible mechanism based on shielding of photons by a sphere's skin depth and establish a correction factor that scales with a ¾ power-law exponent.

[1]  T. Cheng,et al.  Fractal Dimensions and Mixing Structures of Soot Particles during Atmospheric Processing , 2017 .

[2]  G. Mcfiggans,et al.  Black-carbon absorption enhancement in the atmosphere determined by particle mixing state , 2017 .

[3]  Rajan K. Chakrabarty,et al.  Fractal scaling of coated soot aggregates , 2017 .

[4]  A. Laskin,et al.  Morphology and mixing of black carbon particles collected in central California during the CARES field study , 2016 .

[5]  A. Robinson,et al.  Optical properties of black carbon in cookstove emissions coated with secondary organic aerosols: Measurements and modeling , 2016 .

[6]  O. Boucher,et al.  Jury is still out on the radiative forcing by black carbon , 2016, Proceedings of the National Academy of Sciences.

[7]  Y. Kim,et al.  Sensitivity and Contribution of Organic Aerosols to Aerosol Optical Properties Based on Their Refractive Index and Hygroscopicity , 2016 .

[8]  V. Ramanathan,et al.  Convergence on climate warming by black carbon aerosols , 2016, Proceedings of the National Academy of Sciences.

[9]  Y. Wang,et al.  Markedly enhanced absorption and direct radiative forcing of black carbon under polluted urban environments , 2016, Proceedings of the National Academy of Sciences.

[10]  R. Chakrabarty,et al.  Fractal morphology of black carbon aerosol enhances absorption in the thermal infrared wavelengths. , 2016, Optics letters.

[11]  C. Sorensen,et al.  A new parameter to describe light scattering by an arbitrary sphere , 2015 .

[12]  Edward Charles Fortner,et al.  Enhanced light absorption by mixed source black and brown carbon particles in UK winter , 2015, Nature Communications.

[13]  A. Stohl,et al.  Light‐absorbing properties of ambient black carbon and brown carbon from fossil fuel and biomass burning sources , 2015 .

[14]  C. Sorensen,et al.  Effect of the imaginary part of the refractive index on light scattering by spheres. , 2015, Journal of the Optical Society of America. A, Optics, image science, and vision.

[15]  Y. Rudich,et al.  Optical properties of secondary organic aerosols and their changes by chemical processes. , 2015, Chemical reviews.

[16]  Qiaoqiao Wang,et al.  Global budget and radiative forcing of black carbon aerosol: Constraints from pole‐to‐pole (HIPPO) observations across the Pacific , 2014 .

[17]  M. Dubey,et al.  Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles , 2013, Nature Communications.

[18]  J. Seinfeld,et al.  The 2010 California Research at the Nexus of Air Quality and Climate Change (CalNex) field study , 2013 .

[19]  B. DeAngelo,et al.  Bounding the role of black carbon in the climate system: A scientific assessment , 2013 .

[20]  Qi Zhang,et al.  Evolution of Multispectral Aerosol Absorption Properties in a Biogenically-Influenced Urban Environment during the CARES Campaign , 2017 .

[21]  J. Seinfeld,et al.  Secondary Organic Aerosol Coating Formation and Evaporation: Chamber Studies Using Black Carbon Seed Aerosol and the Single-Particle Soot Photometer , 2013 .

[22]  杨鉴初 “Bulletin of the American Meteorological Society”杂志第32卷中文摘 , 2013 .

[23]  T. Petäjä,et al.  Radiative Absorption Enhancements Due to the Mixing State of Atmospheric Black Carbon , 2012, Science.

[24]  A. Middlebrook,et al.  Brown carbon and internal mixing in biomass burning particles , 2012, Proceedings of the National Academy of Sciences.

[25]  C. Sorensen,et al.  A three parameter description of the structure of diffusion limited cluster fractal aggregates. , 2012, Journal of colloid and interface science.

[26]  Alfons G. Hoekstra,et al.  The discrete-dipole-approximation code ADDA: Capabilities and known limitations , 2011 .

[27]  Hajime Okamoto,et al.  Validity criteria of the discrete dipole approximation. , 2010, Applied optics.

[28]  Y. Kondo,et al.  Amplification of Light Absorption of Black Carbon by Organic Coating , 2010 .

[29]  John H. Seinfeld,et al.  The formation, properties and impact of secondary organic aerosol: current and emerging issues , 2009 .

[30]  G. Evans,et al.  Mass Absorption Cross-Section of Ambient Black Carbon Aerosol in Relation to Chemical Age , 2009 .

[31]  V. Ramanathan,et al.  Global and regional climate changes due to black carbon , 2008 .

[32]  T. Henning,et al.  Effective medium theories for irregular fluffy structures: aggregation of small particles. , 2007, Applied optics.

[33]  A. Weinheimer,et al.  Fast airborne aerosol size and chemistry measurements with the high resolution aerosol mass spectrometer during the MILAGRO Campaign , 2007 .

[34]  Philip J. Rasch,et al.  Present-day climate forcing and response from black carbon in snow , 2006 .

[35]  T. Bond,et al.  Light Absorption by Carbonaceous Particles: An Investigative Review , 2006 .

[36]  John H. Seinfeld,et al.  Climate response of direct radiative forcing of anthropogenic black carbon , 2005 .

[37]  C. Sorensen,et al.  Cluster shape anisotropy in irreversibly aggregating particulate systems. , 2004, Langmuir : the ACS journal of surfaces and colloids.

[38]  M. Jacobson,et al.  Strong radiative heating due to the mixing state of black carbon in atmospheric aerosols , 2022 .

[39]  Barbara J. Turpin,et al.  Species Contributions to PM2.5 Mass Concentrations: Revisiting Common Assumptions for Estimating Organic Mass , 2001 .

[40]  C. Sorensen Light Scattering by Fractal Aggregates: A Review , 2001 .

[41]  P. Koepke,et al.  Optical Properties of Aerosols and Clouds: The Software Package OPAC , 1998 .

[42]  J. Herskowitz,et al.  Proceedings of the National Academy of Sciences, USA , 1996, Current Biology.

[43]  H. Horvath Atmospheric light absorption : a review , 1993 .

[44]  P. Meakin Computer simulation of cluster-cluster aggregation using linear trajectories: Results from three-dimensional simulations and a comparison with aggregates formed using brownian trajectories , 1984 .

[45]  H. V. Hulst Light Scattering by Small Particles , 1957 .