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Register a new userA widely tunable 10-$mu$m quantum cascade laser phase-locked to a state-of-the-art mid-infrared reference for precision molecular spectroscopy
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Authors
Papa Lat Tabara Sow
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We report the coherent phase-locking of a quantum cascade laser (QCL) at 10-$mu$m to the secondary frequency standard of this spectral region, a CO2 laser stabilized on a saturated absorption line of OsO4. The stability and accuracy of the standard are transferred to the QCL resulting in a line width of the order of 10 Hz, and leading to our knowledge to the narrowest QCL to date. The locked QCL is then used to perform absorption spectroscopy spanning 6 GHz of NH3 and methyltrioxorhenium, two species of interest for applications in precision measurements.
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We present a new method for accurate mid-infrared frequency measurements and stabilization to a near-infrared ultra-stable frequency reference, transmitted with a long-distance fibre link and continuously monitored against state-of-the-art atomic fountain clocks. As a first application, we measure the frequency of an OsO4 rovibrational molecular line around 10 $mu$m with a state-of-the-art uncertainty of 8x10-13. We also demonstrate the frequency stabilization of a mid-infrared laser with fractional stability better than 4x10-14 at 1 s averaging time and a line-width below 17 Hz. This new stabilization scheme gives us the ability to transfer frequency stability in the range of 10-15 or even better, currently accessible in the near-infrared or in the visible, to mid-infrared lasers in a wide frequency range.
We report the first experimental demonstration of frequency-locking of an extended-cavity quantum-cascade-laser (EC-QCL) to a near-infrared frequency comb. The locking scheme is applied to carry out absolute spectroscopy of N2O lines near 7.87 {mu}m with an accuracy of ~60 kHz. Thanks to a single mode operation over more than 100 cm^{-1}, the comb-locked EC-QCL shows great potential for the accurate retrieval of line center frequencies in a spectral region that is currently outside the reach of broadly tunable cw sources, either based on difference frequency generation or optical parametric oscillation. The approach described here can be straightforwardly extended up to 12 {mu}m, which is the current wavelength limit for commercial cw EC-QCLs.
Dual-frequency comb spectroscopy has emerged as a disruptive technique for measuring wide-spanning spectra with high resolution, yielding a particularly powerful technique for sensitive multi-component gas analysis. We present a spectrometer system based on dual electro-optical combs with subsequent conversion to the mid-infrared via tunable difference frequency generation, operating in the range from 3 to 4.7 $mu$m. The simultaneously recorded bandwidth is up to 454(1) GHz and a signal-to-noise ratio of 7.3(2) x 10$^2$ Hz$^{-1/2}$ can be reached. The conversion preserves the coherence of the dual-comb within 3 s measurement time. Concentration measurements of 5 ppm methane at 3.3 $mu$m, 100 ppm nitrous oxide at 3.9 $mu$m and a mixture of 15 ppm carbon monoxide and 5 % carbon dioxide at 4.5 $mu$m are presented with a relative precision of 1.4 % in average after 2 s measurement time. The noise-equivalent absorbance is determined to be less than 4.6(2) x 10$^{-3}$ Hz$^{-1/2}$.
There is an increasing demand for precise molecular spectroscopy, in particular in the mid-infrared fingerprint window that hosts a considerable number of vibrational signatures, whether it be for modeling our atmosphere, interpreting astrophysical spectra or testing fundamental physics. We present a high-resolution mid-infrared spectrometer traceable to primary frequency standards. It combines a widely tunable ultra-narrow Quantum Cascade Laser (QCL), an optical frequency comb and a compact multipass cell. The QCL frequency is stabilized onto a comb controlled with a remote near-infrared ultra-stable laser, transferred through a fiber link. The resulting QCL frequency stability is below 10-15 from 0.1 to 10s and its frequency uncertainty of 4x10-14 is given by the remote frequency standards. Continuous tuning over ~400 MHz is reported. We use the apparatus to perform saturated absorption spectroscopy of methanol in the low-pressure multipass cell and demonstrate a statistical uncertainty at the kHz level on transition center frequencies, confirming its potential for driving the next generation technology required for precise spectroscopic measurements.
Using a free-running distributed-feedback quantum cascade laser (QCL) emitting at 9.54 $mu$m, the pressure shift parameters of four intense rovibrational transitions in the $ u_3$ fundamental band of ozone induced by oxygen (O$_2$), air and the noble gases helium (He), argon (Ar), and xenon (Xe) are obtained by employing second harmonic detection. The experimental analysis comprises a full uncertainty budget and provides line shift data which are traceable to SI. The high density of transitions in the $ u_3$ spectral region of ozone make this region particularly difficult to study with more commonly used techniques such as Fourier transform spectroscopy. The comparatively high spectral resolution of the QCL in the MHz range, on the contrary, allows to measure molecular shifts at relatively low pressures (from 2 to 70 hPa), thus reducing the impact of spectral congestion due to pressure broadening of molecular lines. The comparison of our results with published data shows that presently recommended values for the pressure shift are too low in this region. This observation is corroborated by semi-classical calculations using the Robert-Bonamy formalism. A slight negative $J$ dependence, already observed in other ozone vibrational bands, is predicted. Systematic use of our technique could be very useful to support this hypothesis and to make up for the lack of shift parameters for ozone $ u_3$ transitions in molecular spectral databases. A subsequent stabilization of the QCL onto an optical frequency comb will open up possibilities to perform metrological measurements of Doppler-free molecular lines.
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