Impulsive Excitation of Phonon-Pair Combination States by Second-Order Raman Scattering

The excitation of (100)-oriented ${\mathrm{KTaO}}_3$ with 25-fs laser pulses impulsively drives phonon-pair combination states via second-order Raman scattering. Oscillations in the phonon-amplitude covariance at the sum and difference frequency of the two involved phonons are observed in a spectrally and temporally resolved pump-probe experiment. Transmission changes of the sample are dominated by contributions of wave vector conserving phonon-pair combinations from the entire Brillouin zone that have maxima in their combined density of states. For low temperatures the temperature dependence of the covariance oscillations of different phonon combinations is reproduced by a quantum-mechanical model.