Broadening the optical bandwidth of quantum cascade lasers using RF noise current perturbations.

We report on the broadening of the optical bandwidth of a distributed feedback quantum cascade laser (QCL) caused by the application of radio frequency (RF) noise to the injection current. The broadening is quantified both via Lamb-dip spectroscopy and the frequency noise power spectral density (PSD). The linewidth of the unperturbed QCL (emitting at ∼5.3 µm) determined by Lamb-dip spectroscopy is 680±170 kHz, and is in reasonable agreement with the linewidth of 460±40 kHz estimated by integrating the PSD measured under the same laser operating conditions. Measurements with both techniques reveal that by mixing the driving current with broadband RF noise the laser lineshape was reproducibly broadened up to ca 6 MHz with an increasing Gaussian contribution. The effects of linewidth broadening are then demonstrated in the two-color coherent transient spectra of nitric oxide.

Enhancing the sensitivity of mid-IR quantum cascade laser-based cavity-enhanced absorption spectroscopy using RF current perturbation.

The sensitivity of mid-IR quantum cascade laser (QCL) off-axis cavity-enhanced absorption spectroscopy (CEAS), often limited by cavity mode structure and diffraction losses, was enhanced by applying a broadband RF noise to the laser current. A pump-probe measurement demonstrated that the addition of bandwidth-limited white noise effectively increased the laser linewidth, thereby reducing mode structure associated with CEAS. The broadband noise source offers a more sensitive, more robust alternative to applying single-frequency noise to the laser. Analysis of CEAS measurements of a CO(2) absorption feature at 1890 cm(-1) averaged over 100 ms yielded a minimum detectable absorption of 5.5×10(-3) Hz(-1/2) in the presence of broadband RF perturbation, nearly a tenfold improvement over the unperturbed regime. The short acquisition time makes this technique suitable for breath applications requiring breath-by-breath gas concentration information.

Pump and probe spectroscopy with continuous wave quantum cascade lasers.

This paper details infra-red pump and probe studies on nitric oxide conducted with two continuous wave quantum cascade lasers both operating around 5 µm. The pump laser prepares a velocity selected population in a chosen rotational quantum state of the v = 1 level which is subsequently probed using a second laser tuned to a rotational transition within the v = 2 ← v = 1 hot band. The rapid frequency scan of the probe (with respect to the molecular collision rate) in combination with the velocity selective pumping allows observation of marked rapid passage signatures in the transient absorption profiles from the polarized vibrationally excited sample. These coherent transient signals are influenced by the underlying hyperfine structure of the pump and probe transitions, the sample pressure, and the coherent properties of the lasers. Pulsed pump and probe studies show that the transient absorption signals decay within 1 µs at 50 mTorr total pressure, reflecting both the polarization and population dephasing times of the vibrationally excited sample. The experimental observations are supported by simulation based upon solving the optical Bloch equations for a two level system.

Coherent transient spectroscopy with continuous wave quantum cascade lasers.

A high power continuous wave quantum cascade laser operating around 1900 cm(-1) has been used to conduct Lamb dip spectroscopy on a low pressure sample of NO. The widths of the Lamb dips indicate that the laser linewidth is 800 ± 60 kHz and the power sufficient to induce significant population transfer of up to 35%. While the Lamb dip signals are symmetric at low laser chirp rates, they become increasingly asymmetric as the chirp rate increases, further confirming the significant degree of population transfer. In addition rapid passage structure on the Lamb dip signal is observed after the weak probe beam is swept through the line center. This structure is sensitive to both the probe chirp rate and the underlying hyperfine structure of the rovibrational transition, and is accurately modeled using the optical Bloch equations.