Refractive Index and Absorption Attribution of Highly Absorbing Brown Carbon Aerosols from an Urban Indian City-Kanpur.

Atmospheric aerosols influence Earth's radiative balance, having both warming and cooling effects. Though many aerosols reflect radiation, carbonaceous aerosols such as black carbon and certain organic carbon species known as brown carbon have the potential to warm the atmosphere by absorbing light. Black carbon absorbs light over the entire solar spectrum whereas brown carbon absorbs near-UV wavelengths and, to a lesser extent, visible light. In developing countries, such as India, where combustion sources are prolific, the influence of brown carbon on absorption may be significant. In order to better characterize brown carbon, we present experimental and modeled absorption properties of submicron aerosols measured in an urban Indian city (Kanpur). Brown carbon here is found to be fivefold more absorbing at 365 nm wavelength compared to previous studies. Results suggest ~30% of total absorption in Kanpur is attributed to brown carbon, with primary organic aerosols contributing more than secondary organics. We report the spectral brown carbon refractive indices along with an experimentally constrained estimate of the influence of aerosol mixing state on absorption. We conclude that brown carbon in Kanpur is highly absorbing in nature and that the mixing state plays an important role in light absorption from volatile species.

Contribution of Brown Carbon to Direct Radiative Forcing over the Indo-Gangetic Plain.

The Indo-Gangetic Plain is a region of known high aerosol loading with substantial amounts of carbonaceous aerosols from a variety of sources, often dominated by biomass burning. Although black carbon has been shown to play an important role in the absorption of solar energy and hence direct radiative forcing (DRF), little is known regarding the influence of light absorbing brown carbon (BrC) on the radiative balance in the region. With this in mind, a study was conducted for a one month period during the winter-spring season of 2013 in Kanpur, India that measured aerosol chemical and physical properties that were used to estimate the sources of carbonaceous aerosols, as well as parameters necessary to estimate direct forcing by aerosols and the contribution of BrC absorption to the atmospheric energy balance. Positive matrix factorization analyses, based on aerosol mass spectrometer measurements, resolved organic carbon into four factors including low-volatile oxygenated organic aerosols, semivolatile oxygenated organic aerosols, biomass burning, and hydrocarbon like organic aerosols. Three-wavelength absorption and scattering coefficient measurements from a Photo Acoustic Soot Spectrometer were used to estimate aerosol optical properties and estimate the relative contribution of BrC to atmospheric absorption. Mean ± standard deviation values of short-wave cloud free clear sky DRF exerted by total aerosols at the top of atmosphere, surface and within the atmospheric column are -6.1 ± 3.2, -31.6 ± 11, and 25.5 ± 10.2 W/m(2), respectively. During days dominated by biomass burning the absorption of solar energy by aerosols within the atmosphere increased by ∼35%, accompanied by a 25% increase in negative surface DRF. DRF at the top of atmosphere during biomass burning days decreased in negative magnitude by several W/m(2) due to enhanced atmospheric absorption by biomass aerosols, including BrC. The contribution of BrC to atmospheric absorption is estimated to range from on average 2.6 W/m(2) for typical ambient conditions to 3.6 W/m(2) during biomass burning days. This suggests that BrC accounts for 10-15% of the total aerosol absorption in the atmosphere, indicating that BrC likely plays an important role in surface and boundary temperature as well as climate.

Comparison of experimental and modeled absorption enhancement by black carbon (BC) cored polydisperse aerosols under hygroscopic conditions.

The quantification of the radiative impacts of light absorbing ambient black carbon (BC) particles strongly depends on accurate measurements of BC mass concentration and absorption coefficient (ß(abs)). In this study, an experiment has been conducted to quantify the influence of hygroscopic growth of ambient particles on light absorption. Using the hygroscopic growth factor (i.e., Zdanovskii-Stokes-Robinson (ZSR) approach), a model has been developed to predict the chemical composition of particles based on measurements, and the absorption and scattering coefficients are derived using a core-shell assumption with light extinction estimates based on Mie theory. The estimated optical properties agree within 7% for absorption coefficient and 30% for scattering coefficient with that of measured values. The enhancement of absorption is found to vary according to the thickness of the shell and BC mass, with a maximum of 2.3 for a shell thickness of 18 nm for the particles. The findings of this study underline the importance of considering aerosol-mixing states while calculating their radiative forcing.