Vibrational Two-Photon Emission from Coherently Excited Solid Parahydrogen

We report the observation of two-photon emission from a coherently excited vibrational state of solid parahydrogen, which is also a known quantum solid. Coherence between the ground and the excited states is prepared by stimulated Raman scattering using two visible laser pulses. The two-photon emission is triggered by another mid-infrared laser pulse. It was observed that the two-photon emission persists even when the trigger pulse is injected long after the excitation. This is due to the long decoherence time of the vibrational states of solid parahydrogen. It is found that the emission intensity increases even after the excitation pulses pass through the target completely. This coherence development is highly suppressed at high target temperatures and high residual orthohydrogen concentrations. Effects of target annealing and laser-induced damage on the target are also observed.