Frequency-modulation spectroscopy with transform-limited nanosecond laser pulses

We demonstrate high-quality FM spectra with nanosecond laser pulses. Transform-limited pulses with FM sidebands are produced by pulsed amplification of a phase-modulated cw laser. The pulses can be shifted to the UV by nonlinear mixing. We report both initial experiments on I(2) and what is to our knowledge the first observation of a far-UV transition by FM spectroscopy, at 214.5 nm. Major advantages of this method include (1) spectral resolution of the order of 0.001 cm(-1), (2) better-defined optical phase, and (3) a much smaller and more easily detected modulation frequency, ~500 MHz. The absorption sensitivity is ~10(-4), and considerable further improvement is expected.