Heterodyne-assisted pulsed spectroscopy with a nearly Fourier-transform limited, injection-seeded optical parametric oscillator.

Narrowband pulsed 822 nm signal radiation from an injection-seeded optical parametric oscillator (OPO) system is used to record fluorescence-detected sub-Doppler two-photon excitation (TPE) spectra of atomic cesium. An optical-heterodyne technique is used to monitor the frequency chirp as well as the fluctuating central frequency of successive OPO output pulses, thereby providing a novel way to record sub-Doppler TPE spectra. The measured TPE linewidth approaches the ultimate limit imposed by the Fourier transform of the pulse's temporal profile, demonstrating the utility of this system for pulsed laser spectroscopy applications that require the highest possible resolution.