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The picosecond thermal response of a normal octadecanethiol self-assembledmonolayer on a gold surface was studied using pump-probe, broadband-infrared,background-suppressed and vibrational sum frequency generation spectroscopy.The orientation fluctuations in response to flash heating were characterizedfrom the intensity kinetics of the terminal methyl C-H stretching vibrations.An intensity decrease (5.7 +/- 1.3 ps) in the asymmetric modes indicated thatstochastic processes of molecular conformations developed during multiplelight-matter interactions. Including torsional diffusion into the rotation termof second order electrosusceptibility explained the experimental surfacetemperature increment two order-of-magnitudes smaller than the activationenergy of the dihedral angles (~15 K).

Molecular stochastic process on gold surface observed in  broadband-infrared, background-suppressed, sum frequency generation  spectroscopy: picosecond heat transfer to self-assembled monolayers