Two-tone frequency-modulation stimulated Rayleigh spectroscopy

We have demonstrated two-tone frequency-modulation (FM) stimulated Rayleigh spectroscopy. This method can provide high spectral resolution (∼1  MHz), excellent pump/probe detuning accuracy, and near-shot-noise-limited signal-to-noise ratios using a single narrowband laser as the master oscillator. Pump/probe detuning and FM sideband generation are produced with an electro-optic modulator. A double-pass two-rod Nd:YAG amplifier provides peak powers near 1 kW for the pump beam. Unlike with two-tone FM absorption spectroscopy, the phase signal is retained for two-tone FM Rayleigh spectroscopy. Measurements confirm that the shape of the phase component of the stimulated thermal Rayleigh peak agrees with theory.