Understanding and predicting the temporal response of laser-induced incandescence from carbonaceous particles

This paper describes a model for analyzing and predicting the temporal behavior of laser-induced incandescence (LII) from combustion-generated soot, carbon black, and other carbonaceous particles on a nanosecond time scale. The model accounts for particle heating by absorption of light from a pulsed laser and cooling by sublimation, conduction, and radiation. The model also includes mechanisms for oxidation, melting, and annealing of the particles and nonthermal photodesorption of carbon clusters from the particle surface. At fluences above 0.1 J/cm2, particle temperatures during the laser pulse are determined by the balance between absorption and sublimation, whereas at lower fluences particle temperatures do not reach the sublimation temperature, and temperatures are predominantly controlled by absorption and conduction. After the laser pulse, temperatures are predominantly controlled by conductive cooling rates. Oxidative heating may compete with conductive cooling on these time scales. Annealing of the particles to a more ordered phase of carbon is predicted to occur at fluences as low as 0.02 J/cm2. Annealing may strongly influence sublimation rates, and changes in emissivity during annealing are predicted to increase signal decay rates. Supersonic expansion of the carbon clusters sublimed from the surface is calculated to occur at fluences above 0.12 J/cm2. When compared with LII measurements recorded in a flame at atmospheric pressure, the model reproduces the shapes and relative magnitudes of LII temporal profiles over a wide range of laser fluences. Comparisons between model predictions and experimental observations suggest that the particles do not melt at laser fluences that lead to melting of bulk graphite. These comparisons also indicate that the energy released during particle annealing is much smaller than that released during annealing of neutron- or electron-irradiated graphite. Despite good agreement between model and experimental results, large uncertainties exist for input parameters used to calculate annealing rates and rates of oxidation, conduction, absorption, emission, and photolytic desorption of carbon clusters for both the initial and annealed particles.