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We present the systematic analysis of individual black carbon (BC) mixing state and its impact on radiative forcing from an urban Indian city, Kanpur, located in Indo-Gangetic Plain (IGP). Simultaneous measurements using Single Particle Soot Photometer (SP2), Photo-Acoustic Soot Spectrometer (PASS-3) and High-Resolution Time-of-Flight Aerosol Mass Spectrometer (AMS) were conducted from 8 January 2015 to 28 February 2015 at Kanpur. BC mass and number concentrations varied between 0.7 and 17 mu g/m(3) and 277-5866 #/cm(3) with a mean of 4.06 mu g/m3 and 1314 #/cm3, respectively. The diurnal variation of BC mass concentration showed a traffic hour peak during both the morning and late night. The mean fraction of thickly coated BC particles (fTC(Bc)) was found to be 61.6%, indicating that a large fraction of BC particles was internally mixed. The fTCBc increased after sunrise with a peak at about noontime, indicating that the formation of secondary organic aerosol under active photochemistry can enhance organic coating on a core of black carbon. High-resolution positive matrix factorization (HR-PMF) factors showed distinct characteristics with fTCBc. While primary organic aerosols like cooking organic aerosols (COA) and biomass burning organic aerosols (BBOA) were negatively correlated with fTCBc = -0.78 and -0.51, respectively), aged low volatile oxygenated organic aerosol (LVOOA) was forming a coating over BC (r = 0.6). Similar positive correlation of fTCBc with inorganic species like ammonium (r = 0.58) and nitrate (r = 0.47) further suggested that BC appears to be largely coated with LVOOA, ammonium, and nitrate. A positive correlation between the fTCBc and the mass absorption cross- at 781 nm (MAC(781)) was also observed (r = 0.58). Our results suggest that the observed fTCBc could amplify the MAC781 approximately by a factor of 1.8, which may catalyze the positive radiative forcing in the IGP.

期刊论文 2017-11-15 DOI: 10.1016/j.atmosres.2017.07.007 ISSN: 0169-8095

Stratospheric aerosols cool the Earth by scattering sunlight. Although sulfuric acid dominates the stratospheric aerosol, this study finds that organic material in the lowermost stratosphere contributes 30-40% of the nonvolcanic stratospheric aerosol optical depth (sAOD). Simulations indicate that nonvolcanic sAOD has increased 77% since 1850. Stratospheric aerosol accounts for 21% of the total direct aerosol radiative forcing (which is negative) and 12% of the total aerosol optical depth (AOD) increase from organics and sulfate. There is a larger stratospheric influence on radiative forcing (i.e., 21%) relative to AOD (i.e., 12%) because an increase of tropospheric black carbon warms the planet while stratospheric aerosols (including black carbon) cool the planet. Radiative forcing from nonvolcanic stratospheric aerosol mass of anthropogenic origin, including organics, has not been widely considered as a significant influence on the climate system.

期刊论文 2016-09-01 DOI: 10.1002/2016GL070153 ISSN: 0094-8276
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