Accurate particle sizing through time-resolved laser-induced incandescence (TR-LII) requires knowledge of the thermal accommodation coefficient, but the underlying physics of this parameter is poorly understood. If the particle size is known a priori, however, TR-LII data can instead be used to infer the thermal accommodation coefficient. Thermal accommodation coefficients measured between soot and different monatomic and polyatomic gases show that the accommodation coefficient increases with molecular mass for monatomic gases and is lower for polyatomic gases. This latter result indicates that surface energy is accommodated preferentially into translational modes over internal modes for these gases.