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Maximum relative excitation of a specific vibrational mode via optimum laser pulse duration

For molecules and materials responding to femtosecond-scale optical laser pulses, we predict maximum relative excitation of a Raman-active vibrational mode with period T when the pulse has an FWHM duration of 0.42 T. This result follows from a general analytical model, and is precisely confirmed by detailed density-functional-based dynamical simulations for C60 and a carbon nanotube, which include anharmonicity, nonlinearity, no assumptions about the polarizability tensor, and no averaging over rapid oscillations within the pulse. The mode specificity is, of course, best at low temperature and for pulses that are electronically off-resonance, and the energy deposited in any mode is proportional to the fourth power of the electric field.