S. Borri

Observing the intrinsic linewidth of a quantum-cascade laser: beyond the Schawlow-Townes limit.

A comprehensive investigation of the frequency-noise spectral density of a free-running midinfrared quantum-cascade laser is presented for the first time. It provides direct evidence of the leveling of this noise down to a white-noise plateau, corresponding to an intrinsic linewidth of a few hundred hertz. The experiment is in agreement with the most recent theory on the fundamental mechanism of line broadening in quantum-cascade lasers, which provides a new insight into the Schawlow-Townes formula and predicts a narrowing beyond the limit set by the radiative lifetime of the upper level.

Saturated-absorption cavity ring-down spectroscopy.

A novel approach to cavity ring-down spectroscopy with the sample gas in saturated- absorption regime allows to decouple and simultaneously retrieve empty-cavity background and absorption signal, improving both measurement sensitivity and resolution. OCIS codes: 300.6340 Spectroscopy, infrared; 300.6390 Spectroscopy, molecular; 300.6460 Spectroscopy, saturation The availability of a molecular-spectroscopy technique, able to combine the ultimate performance in terms of sensitivity, resolution and frequency accuracy, can be crucial in many fundamental physical measurements. Indeed, profiting from the strength and ease of saturation of many mid-IR ro-vibrational transitions, this technique could provide new insights in elusive quantum-mechanical effects encoded in molecules. Such a technique could also represent a major step forward in trace-gas sensing. Cavity ring-down (CRD) spectroscopy has already proven to be a good technique to directly provide a sensitive and quantitative measurement of gas absorption coefficient with a simple experimental set-up. In principle, it is not limited by amplitude noise of the laser source, but only by detection shot noise. However, variations of the empty-cavity decay rate always prevent to achieve this ultimate limit and to average measurements over long times. Other techniques (e.g. CRD heterodyne spectroscopy and NICE-OHMS) are even more sensitive than standard CRD, but they are more complex (frequency modulations and/or lockings are needed), less quantitative (calibration procedures are needed) and require fast and sensitive detectors, generally unavailable in the mid IR. We present a new spectroscopic technique, namely saturated-absorption cavity ring-down (SCaR), that improves the CRD sensitivity (1). We show that the progressive decrease of the saturation level during each SCaR event makes our technique very effective in identifying and decoupling any variation of the empty-cavity decay rate. Saturated absorption induces a deviation of the SCaR signal from the perfectly exponential behavior, making a detailed treatment of non-linear effects needed to fit experimental data to the underlying physics of matter-radiation interaction. We developed and tested a new model which is very effective in exploiting the SCaR spectroscopic technique. The experimental set-up (2) is based on a difference-frequency-generated CW coherent source widely tunable in the mid IR, with the near-IR pump/signal lasers phase-locked one another through a fs Ti:sapphire optical frequency comb (OFC). The 1-m-long cavity is formed by 2 high-reflectivity mirrors with 6-m radius of curvature and optical losses of 440 ppm around 2340 cm -1 . With this set-up we performed several spectroscopic measurements to test both sensitivity and resolution using the newly developed model.

Part-per-trillion level SF6 detection using a quartz enhanced photoacoustic spectroscopy-based sensor with single-mode fiber-coupled quantum cascade laser excitation.

A sensitive spectroscopic sensor based on a hollow-core fiber-coupled quantum cascade laser (QCL) emitting at 10.54 μm and quartz enhanced photoacoustic spectroscopy (QEPAS) technique is reported. The design and realization of mid-IR fiber and coupler optics has ensured single-mode QCL beam delivery to the QEPAS sensor. The collimation optics was designed to produce a laser beam of significantly reduced beam size and waist so as to prevent illumination of the quartz tuning fork and microresonator tubes. SF(6) was selected as the target gas. A minimum detection sensitivity of 50 parts per trillion in 1 s was achieved with a QCL power of 18 mW, corresponding to a normalized noise-equivalent absorption of 2.7×10(-10) W·cm(-1)/Hz(1/2).

Terahertz quartz enhanced photo-acoustic sensor

A quartz enhanced photo-acoustic sensor employing a single-mode quantum cascade laser emitting at 3.93 Terahertz (THz) is reported. A custom tuning fork with a 1 mm spatial separation between the prongs allows the focusing of the THz laser beam between them, while preventing the prongs illumination. A methanol transition with line-strength of 4.28 × 10−21 cm has been selected as target spectroscopic line. At a laser optical power of ∼ 40 μW, we reach a sensitivity of 7 parts per million in 4s integration time, corresponding to a 1σ normalized noise-equivalent absorption of 2 × 10−10 cm−1W/Hz½.

Frequency-comb-referenced quantum-cascade laser at 4.4 μm

We report what we believe to be the first absolute frequency measurement performed using a quantum-cascade laser (QCL) referenced to an optical frequency comb synthesizer (OFCS). A QCL at 4.43 microm has been used for producing near-infrared radiation at 858 nm by means of sum-frequency generation with a Nd:YAG source in a periodically poled lithium niobate nonlinear crystal. The absolute frequency of the QCL source has been measured by detecting the beat note between the sum frequency and a diode laser at the same wavelength, while both the Nd:YAG and the diode laser were referenced to the OFCS. Doppler-broadened line profiles of (13)CO(2) molecular transitions have been recorded with such an absolute frequency reference.

Measuring frequency noise and intrinsic linewidth of a room-temperature DFB quantum cascade laser

The frequency-noise power spectral density of a room-temperature distributed-feedback quantum cascade laser emitting at λ = 4.36 μm has been measured. An intrinsic linewidth value of 260 Hz is retrieved, in reasonable agreement with theoretical calculations. A noise reduction of about a factor 200 in most of the frequency interval is also found, with respect to a cryogenic laser at the same wavelength. A quantitative treatment shows that it can be explained by a temperature-dependent mechanism governing the transport processes in resonant tunnelling devices. This confirms the predominant effect of the heterostructure in determining shape and magnitude of the frequency noise spectrum in QCLs.

Lamb-dip-locked quantum cascade laser for comb-referenced IR absolute frequency measurements

The frequency of a DFB quantum cascade laser (QCL) emitting at 4.3 microm has been long-term stabilized to the Lamb-dip center of a CO2 ro-vibrational transition by means of first-derivative locking to the saturated absorption signal. Thanks to the non-linear sum-frequency generation (SFG) process with a fiber-amplified Nd:YAG laser, the QCL mid-infrared (IR) radiation has been linked to an optical frequency-comb synthesizer (OFCS) and its absolute frequency counted with a kHz-level precision and an overall uncertainty of 75 kHz.

Intracavity quartz-enhanced photoacoustic sensor

We report on a spectroscopic technique named intracavity quartz-enhanced photoacoustic spectroscopy (I-QEPAS) employed for sensitive trace-gas detection in the mid-infrared spectral region. It is based on a combination of QEPAS with a buildup optical cavity. The sensor includes a distributed feedback quantum cascade laser emitting at 4.33 μm. We achieved a laser optical power buildup factor of ∼500, which corresponds to an intracavity laser power of ∼0.75 W. CO2 has been selected as the target molecule for the I-QEPAS demonstration. We achieved a detection sensitivity of 300 parts per trillion for 4 s integration time, corresponding to a noise equivalent absorption coefficient of 1.4 × 10−8 cm−1 and a normalized noise-equivalent absorption of 3.2 × 10−10 W cm−1 Hz−1/2.

Intrinsic stability of quantum cascade lasers against optical feedback

We study the time dependence of the optical power emitted by terahertz and mid-IR quantum cascade lasers in presence of optical reinjection and demonstrate unprecedented continuous wave (CW) emission stability for strong feedback. We show that the absence of coherence collapse or other CW instabilities typical of diode lasers is inherently associated with the high value of the photon to carrier lifetime ratio and the negligible linewidth enhancement factor of quantum cascade lasers.

Comb-assisted subkilohertz linewidth quantum cascade laser for high-precision mid-infrared spectroscopy

We report on the linewidth narrowing of a room-temperature mid-infrared quantum cascade laser by phase-locking to a difference-frequency-generated radiation referenced to an optical frequency comb synthesizer. A locking bandwidth of 250 kHz, with a residual rms phase-noise of 0.56 rad, has been achieved. The laser linewidth is narrowed by more than 2 orders of magnitude below 1 kHz, and its frequency is stabilized with an absolute traceability of 2×10−12. This source has allowed the measurement of the absolute frequency of a CO2 molecular transition with an uncertainty of about 1 kHz.