Modelling black carbon absorption of solar radiation: Combining external and internal mixing assumptions

An accurate simulation of the absorption properties is key for assessing the radiative effects of aerosol on meteorology and climate. The representation of how chemical species are mixed inside the particles (the mixing state) is one of the major uncertainty factors in the assessment of these effects. Here we compare aerosol optical properties simulations over Europe and North America, coordinated in the framework of the third phase of the Air Quality Model Evaluation International Initiative (AQMEII), to 1 year of AERONET sunphotometer retrievals, in an attempt to identify a mixing state representation that better reproduces the observed single scattering albedo and its spectral variation. We use a single post-processing tool (FlexAOD) to derive aerosol optical properties from simulated aerosol speciation profiles, and focus on the absorption enhancement of black carbon when it is internally mixed with more scattering material, discarding from the analysis scenes dominated by dust.

We found that the single scattering albedo at 440&thinsp;nm (<span classCombining double low line"inline-formula">‰0,440)</span> is on average overestimated (underestimated) by 3-5&thinsp;% when external (core-shell internal) mixing of particles<span idCombining double low line"page182"/> is assumed, a bias comparable in magnitude with the typical variability of the quantity. The (unphysical) homogeneous internal mixing assumption underestimates <span classCombining double low line"inline-formula">‰0,440</span> by <span classCombining double low line"inline-formula">ĝ1/414</span>&thinsp;%. The combination of external and core-shell configurations (partial internal mixing), parameterized using a simplified function of air mass aging, reduces the <span classCombining double low line"inline-formula">‰0,440</span> bias to <span classCombining double low line"inline-formula"><math xmlnsCombining double low line"http://www.w3.org/1998/Math/MathML" idCombining double low line"M5" displayCombining double low line"inline" overflowCombining double low line"scroll" dspmathCombining double low line"mathml"><mrow><mo>-</mo><mn mathvariantCombining double low line"normal">1</mn><mo>/</mo><mo>-</mo><mn mathvariantCombining double low line"normal">3</mn></mrow></math><span><svg:svg xmlns:svgCombining double low line"http://www.w3.org/2000/svg" widthCombining double low line"39pt" heightCombining double low line"14pt" classCombining double low line"svg-formula" dspmathCombining double low line"mathimg" md5hashCombining double low line"ed67d70e5b0265304da1b69b819dd11d"><svg:image xmlns:xlinkCombining double low line"http://www.w3.org/1999/xlink" xlink:hrefCombining double low line"acp-19-181-2019-ie00001.svg" widthCombining double low line"39pt" heightCombining double low line"14pt" srcCombining double low line"acp-19-181-2019-ie00001.png"/></svg:svg></span></span>&thinsp;%. The black carbon absorption enhancement (<span classCombining double low line"inline-formula">Eabs)</span> in core-shell with respect to the externally mixed state is in the range 1.8-2.5, which is above the currently most accepted upper limit of <span classCombining double low line"inline-formula">ĝ1/41.5</span>. The partial internal mixing reduces <span classCombining double low line"inline-formula">Eabs</span> to values more consistent with this limit. However, the spectral dependence of the absorption is not well reproduced, and the absorption Ångström exponent AAE<span classCombining double low line"inline-formula"><math xmlnsCombining double low line"http://www.w3.org/1998/Math/MathML" idCombining double low line"M9" displayCombining double low line"inline" overflowCombining double low line"scroll" dspmathCombining double low line"mathml"><mrow><msubsup><mi/><mn mathvariantCombining double low line"normal">675</mn><mn mathvariantCombining double low line"normal">440</mn></msubsup></mrow></math><span><svg:svg xmlns:svgCombining double low line"http://www.w3.org/2000/svg" widthCombining double low line"16pt" heightCombining double low line"17pt" classCombining double low line"svg-formula" dspmathCombining double low line"mathimg" md5hashCombining double low line"f40632cc1b94d2fa6ba42353b246d109"><svg:image xmlns:xlinkCombining double low line"http://www.w3.org/1999/xlink" xlink:hrefCombining double low line"acp-19-181-2019-ie00002.svg" widthCombining double low line"16pt" heightCombining double low line"17pt" srcCombining double low line"acp-19-181-2019-ie00002.png"/></svg:svg></span></span> is overestimated by 70-120&thinsp;%. Further testing against more comprehensive campaign data, including a full characterization of the aerosol profile in terms of chemical speciation, mixing state, and related optical properties, would help in putting a better constraint on these calculations.