Coherent heterodyne-assisted pulsed spectroscopy: Sub-Doppler two-photon spectra of krypton, characterizing a tunable nonlinear-optical ultraviolet light source

A chirp-minimized, nanosecond-pulsed system has been developed to generate tunable coherent ultraviolet light at ∼212.5 nm by fourth-harmonic conversion of output from an amplified, injection-seeded optical parametric oscillator (OPO). Our CHAPS (coherent heterodyne-assisted pulsed spectroscopy) method is used to characterize the frequency stability and optical bandwidth of the system's output radiation by recording sub-Doppler two-photon excitation spectra of krypton. In our new scanned-reference variant of CHAPS, the central frequency for each amplified OPO pulse is logged by the optical-heterodyne chirp-analysis software, with the frequency of the seed laser slowly tuned and monitored by a high-resolution wavemeter, unlike our previous implementation of CHAPS where the seed-laser frequency was fixed. For the amplified, up-converted pulses at ∼212.5 nm, our CHAPS measurements indicate an optical bandwidth of ∼100 MHz, consistent with the Fourier-transform limit of their duration (∼4.5 ns).