Effects of Mixing State on Black Carbon Measurements by Laser-Induced Incandescence

Abstract

Laboratory experiments and theoretical calculations were made to characterize the performance of a Single Particle Soot Photometer (SP2) manufactured by Droplet Measurement Technologies (DMT), which was designed to measure the mass and the mixing state of individual black carbon (BC) or elemental carbon (EC) particles, based on the laser-induced incandescence (LII) technique. In this study, graphite was used as a surrogate of EC. Graphite particles with mass equivalent diameters of 110–200 nm were layered with organic liquids (glycerol and oleic acid) to produce coated graphite with diameters up to 650–800 nm. These were sampled by the SP2 to measure the waveforms (i.e., time development) of the LII and scattering signals. The peak temperature and the peak LII signal of graphite particles were independent of the coating thickness or the coating material to within experimental errors. These results indicate that the mass of EC can be measured by using peak LII signal without interference by the coating conditions. It was also shown that the difference between the times of the scattering and LII peaks can be used as an indicator of coating on EC with thicknesses larger than about 100–200 nm. LII and scattering waveforms were calculated using a newly developed theoretical model that takes into account the physical processes controlling the temperature and evaporation rate of the coated graphite particle in the laser beam. The calculations reproduced the general features of observed waveforms of LII and scattering signals, providing a firm theoretical basis for the interpretation of the SP2 data.

Acknowledgments

This work was supported by the Ministry of Education, Culture, Sports, Science, and Technology (MEXT), the Japanese Science and Technology Agency (JST), and the global environment research fund of the Japanese Ministry of the Environment (C-051). We are indebted to S. Nakamura for taking TEM images of colloidal graphite particles. We thank Y. Komazaki, N. Takegawa, Y.Miyazaki, M. Koike, and M. Watanabe for assistance in the experiments and giving us useful comments. We also thank D.W. Fahey, J. P. Schwarz, R. S. Gao, J. R. Spackman, G. L. Kok, and D. G. Baumgardner for very stimulating discussions and sharing their works prior to publication.