Harmonic detection with tunable diode lasers —two-tone modulation

The minimum absorption detectable by a tunable diode laser spectrometer utilising harmonic techniques is often limited by interference fringes generated by scattered light. The sensitivity of the spectrometer to absorption can be increased by applying a jitter modulation. In this paper, the theory of harmonic response for single- and two-tone modulation over optical fringes and Lorentzian absorption lines is developed and compared to experimental measurements. A simple analytic expression for the two-tone harmonic line shape is derived. This expression provides a physical understanding of the effects of the second modulation, and a means to unravel the effects of the second modulation on the linewidth and line shape. For a specific choice of the jitter frequency and phase, it is possible to simultaneously minimise the fringe signal and increase the harmonic absorption signal. The results of this investigation are applicable to trace gas detection using tunable diode lasers, and to other areas of spectroscopy and magnetic resonance where harmonic techniques are used.