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Nonlinear Optics

Molecular photon echoes as a signature of vibrational cat states

Holger Friedrich Hofmann, Takao Fuji, Atsushi Sugita, Takayoshi Kobayashi

Published Jan 1, 2000• 0 citations
Publisher

Abstract

Quantum interference between two distinct vibrational trajectories induced by two pulse femtosecond excitation in molecules is shown to result in a photon echo, providing direct evidence of the cat state superposition of Gaussian vibrational wavepackets.
DOI
10.1364/nlo.2000.wb24

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A pair of coherent femtosecond pulse excitations applied to a molecule with strong electron-phonon coupling creates a coherent superposition of a low momentum and a high momentum wavepacket in the vibrational states of both the excited state and the ground state of the coherent transition. As the excited state is accelerated further, interference between the high momentum ground state contribution and the low momentum excited state contribution causes a photon echo. This photon echo is a direct consequence of quantum interference between separate vibrational trajectories and can therefore provide experimental evidence of the non-classical properties of molecular vibrations.