Soot particles are a major absorber of shortwave radiation in the atmosphere. They exert a rather uncertain direct and semi-direct radiative effect, which causes a heating or in some cases a cooling of the atmosphere. The mass absorption coefficient is an essential quantity to describe this light absorption process. This work presents new experimental data on the mass absorption coefficient of soot particles in the troposphere over Central Europe. Mass absorption coefficients were derived as the ratio between the light absorption coefficient determined by multi angle absorption photometry (MAAP), and the soot mass concentration determined by Raman spectroscopy. The Raman method is sensitive to graphitic structures present in the particle samples, and was calibrated in the laboratory using Printex90 model particles. The mass absorption coefficients were determined for a number of seven observation sites, ranging between 3.9 and 7.4 m²/g depending on measurement site and observational period.
The highest values were found in an continentally aged air mass in winter, where we presumed soot particles to be present mainly in internal mixture.
The regional model WRF-Chem was used in conjunction with a high resolution soot emission inventory to simulate soot mass concentrations and absorption coefficients for the Central European Troposphere. The model was validated using soot mass concentrations from Raman measurements and absorption coefficients. Simulated soot mass concentrations were found to be too low by around 50 %, which could be improved by scaling the emissions by a factor of two. In contrast, the absorption coefficient was positively biased by around 20%. Adjusting the modeled mass absorption coefficient to measurements, the simulation of soot light absorption was improved.
Finally, the positive direct radiative forcing at top of the atmosphere was found to be lowered by up to 70% for the model run with adjusted soot absorption behaviour, , indicating a decreased heating effect on the atmosphere.
| Identifer | oai:union.ndltd.org:DRESDEN/oai:qucosa.de:bsz:15-qucosa-109901 |
| Date | 09 April 2013 |
| Creators | Nordmann, Stephan |
| Contributors | Universität Leipzig,, Prof. Dr. Alfred Wiedensohler, Prof. Dr. Gregory Carmichael |
| Publisher | Universitätsbibliothek Leipzig |
| Source Sets | Hochschulschriftenserver (HSSS) der SLUB Dresden |
| Language | English |
| Detected Language | English |
| Type | doc-type:doctoralThesis |
| Format | application/pdf |
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