Mid-infrared Ring Interband Cascade Laser: Operation at the Standard Quantum Limit.

Many precision applications in the mid-infrared spectral range have strong constraints based on quantum effects that are expressed in particular noise characteristics. They limit, e.g., sensitivity and resolution of mid-infrared imaging and spectroscopic systems as well as the bit-error rate in optical free-space communication. Interband cascade lasers (ICLs) are a class of mid-infrared lasers exploiting interband transitions in type-II band alignment geometry. They are currently gaining significant importance for mid-infrared applications from < 3 to > 6 µm wavelength, enabled by novel types of high-performance ICLs such as ring-cavity devices. Their noise behavior is an important feature that still needs to be thoroughly analyzed, including its potential reduction with respect to the shot-noise limit. In this work, we provide a comprehensive characterization of λ = 3.8 µm-emitting, continuous-wave ring ICLs operating at room temperature. It is based on an in-depth study of their main physical intensity noise features such as their bias-dependent intensity noise power spectral density and relative intensity noise. We obtained shot-noise-limited statistics for Fourier frequencies above 100 kHz. This is an important result for precision applications, e.g., interferometry or advanced spectroscopy, which benefit from exploiting the advantage of using such a shot-noise-limited source, enhancing the setup sensitivity. Moreover, it is an important feature for novel quantum optics schemes, including testing specific light states below the shot-noise level, such as squeezed states.

Cavity-enhanced photoacoustic dual-comb spectroscopy.

Photoacoustic dual-comb spectroscopy (DCS), converting spectral information in the optical frequency domain to the audio frequency domain via multi-heterodyne beating, enables background-free spectral measurements with high resolution and broad bandwidth. However, the detection sensitivity remains limited due to the low power of individual comb lines and the lack of broadband acoustic resonators. Here, we develop cavity-enhanced photoacoustic DCS, which overcomes these limitations by using a high-finesse optical cavity for the power amplification of dual-frequency combs and a broadband acoustic resonator with a flat-top frequency response. We demonstrate high-resolution spectroscopic measurements of trace amounts of C2H2, NH3 and CO in the entire telecommunications C-band. The method shows a minimum detection limit of 0.6 ppb C2H2 at the measurement time of 100 s, corresponding to the noise equivalent absorption coefficient of 7 × 10-10 cm-1. The proposed cavity-enhanced photoacoustic DCS may open new avenues for ultrasensitive, high-resolution, and multi-species gas detection with widespread applications.

Time/frequency-domain characterization of a mid-IR DFG frequency comb via two-photon and heterodyne detection.

Mid-infrared frequency combs are nowadays well-appreciated sources for spectroscopy and frequency metrology. Here, a comprehensive approach for characterizing a difference-frequency-generated mid-infrared frequency comb (DFG-comb) both in the time and in the frequency domain is presented. An autocorrelation scheme exploiting mid-infrared two-photon detection is used for characterizing the pulse width and to verify the optimal compression of the generated pulses reaching a pulse duration (FWHM) as low as 196 fs. A second scheme based on mid-infrared heterodyne detection employing two independent narrow-linewidth quantum cascade lasers (QCLs) is used for frequency-narrowing the modes of the DFG-comb down to 9.4 kHz on a 5-ms timescale.

Parts-per-billion-level detection of hydrogen sulfide based on doubly resonant photoacoustic spectroscopy with line-locking.

We report on the development of a highly sensitive hydrogen sulfide (H2S) gas sensor exploiting the doubly resonant photoacoustic spectroscopy technique and using a near-infrared laser emitting at 1578.128 nm. By targeting the R(4) transition of H2S, we achieved a minimum detection limit of 10 part per billion in concentration and a normalized noise equivalent absorption coefficient of 8.9 × 10-12 W cm-1 Hz-1/2. A laser-cavity-molecule locking strategy is proposed to enhance the sensor stability for fast measurement when dealing with external disturbances. A comparison among the state-of-the-art H2S sensors using various spectroscopic techniques confirmed the record sensitivity achieved in this work.

Characterization of noise regimes in mid-IR free-space optical communication based on quantum cascade lasers.

The recent development of Quantum Cascade Lasers (QCLs) represents one of the biggest opportunities for the deployment of a new class of Free Space Optical (FSO) communication systems working in the mid-infrared (mid-IR) wavelength range. As compared to more common FSO systems exploiting the telecom range, the larger wavelength employed in mid-IR systems delivers exceptional benefits in case of adverse atmospheric conditions, as the reduced scattering rate strongly suppresses detrimental effects on the FSO link length given by the presence of rain, dust, fog, and haze. In this work, we use a novel FSO testbed operating at 4.7 µm, to provide a detailed experimental analysis of noise regimes that could occur in realistic FSO mid-IR systems based on QCLs. Our analysis reveals the existence of two distinct noise regions, corresponding to different realistic channel attenuation conditions, which are precisely controlled in our setup. To relate our results with real outdoor configurations, we combine experimental data with predictions of an atmospheric channel loss model, finding that error-free communication could be attained for effective distances up to 8 km in low visibility conditions of 1 km. Our analysis of noise regimes may have a key relevance for the development of novel, long-range FSO communication systems based on mid-IR QCL sources.

Doubly resonant sub-ppt photoacoustic gas detection with eight decades dynamic range.

Photoacoustic spectroscopy (PAS) based gas sensors with high sensitivity, wide dynamic range, low cost, and small footprint are desirable in energy, environment, safety, and public health. However, most works have focused on either acoustic resonator to enhance acoustic wave or optical resonator to enhance optical wave. Herein, we develop a gas sensor based on doubly resonant PAS in which the acoustic and optical waves are simultaneously enhanced using combined optical and acoustic resonators in a centimeter-long configuration. Not only the lower detection limit is enhanced by the double standing waves, but also the upper detection limit is expanded due to the short resonators. As an example, we developed a sensor by detecting acetylene (C2H2), achieving a noise equivalent absorption of 5.7 × 10-13 cm-1 and a dynamic range of eight orders. Compared to the state-of-the-art PAS gas sensors, the developed sensor achieves a record sensitivity and dynamic range.

Mid-infrared homodyne balanced detector for quantum light characterization.

We present the characterization of a novel balanced homodyne detector operating in the mid-infrared. The challenging task of revealing non-classicality in mid-infrared light, e. g. in quantum cascade lasers emission, requires a high-performance detection system. Through the intensity noise power spectral density analysis of the differential signal coming from the incident radiation, we show that our setup is shot-noise limited. We discuss the experimental results with a view to possible applications to quantum technologies, such as free-space quantum communication.

Difference frequency generation in the mid-infrared with orientation-patterned gallium phosphide crystals.

We report on the generation of coherent mid-infrared radiation around 5.85 µm by difference frequency generation (DFG) of a continuous-wave Nd:YAG laser at 1064 nm and a diode laser at 1301 nm in an orientation-patterned gallium phosphide (OP-GaP) crystal. We provide the first characterization of the linear, thermo-optic, and nonlinear properties of OP-GaP in a DFG configuration. Moreover, by comparing the experimental efficiency to Gaussian beam DFG theory, we derive an effective nonlinear coefficient d=17(3) pm/V for first-order quasi-phase-matched OP-GaP. The temperature and signal wavelength tuning curves are in qualitative agreement with theoretical modeling.

Tunable Microcavity-Stabilized Quantum Cascade Laser for Mid-IR High-Resolution Spectroscopy and Sensing.

The need for highly performing and stable methods for mid-IR molecular sensing and metrology pushes towards the development of more and more compact and robust systems. Among the innovative solutions aimed at answering the need for stable mid-IR references are crystalline microresonators, which have recently shown excellent capabilities for frequency stabilization and linewidth narrowing of quantum cascade lasers with compact setups. In this work, we report on the first system for mid-IR high-resolution spectroscopy based on a quantum cascade laser locked to a CaF2 microresonator. Electronic locking narrows the laser linewidth by one order of magnitude and guarantees good stability over long timescales, allowing, at the same time, an easy way for finely tuning the laser frequency over the molecular absorption line. Improvements in terms of resolution and frequency stability of the source are demonstrated by direct sub-Doppler recording of a molecular line.

High finesse optical cavity coupled with a quartz-enhanced photoacoustic spectroscopic sensor.

An ultra-sensitive and selective quartz-enhanced photoacoustic spectroscopy (QEPAS) combined with a high-finesse cavity sensor platform is proposed as a novel method for trace gas sensing. We call this technique Intra-cavity QEPAS (I-QEPAS). In the proposed scheme, a single-mode continuous wave quantum cascade laser (QCL) is coupled into a bow-tie optical cavity. The cavity is locked to the QCL emission frequency by means of a feedback-locking loop that acts directly on a piezoelectric actuator mounted behind one of the cavity mirrors. A power enhancement factor of ∼240 was achieved, corresponding to an intracavity power of ∼0.72 W. CO2 was selected as the target gas to validate our sensor. For the P(42) CO2 absorption line, located at 2311.105 cm(-1), a minimum detection limit of 300 parts per trillion by volume at a total gas pressure of 50 mbar was achieved with a 20 s integration time. This corresponds to a normalized noise equivalent absorption of 3.2 × 10(-10) W cm(-1) Hz(-1/2), comparable with the best results reported for the QEPAS technique on much faster relaxing gases. A comparison with standard QEPAS performed under the same experimental conditions confirms that the I-QEPAS sensitivity scales with the intracavity laser power enhancement factor.

A quartz enhanced photo-acoustic gas sensor based on a custom tuning fork and a terahertz quantum cascade laser.

An innovative quartz enhanced photoacoustic (QEPAS) gas sensing system operating in the THz spectral range and employing a custom quartz tuning fork (QTF) is described. The QTF dimensions are 3.3 cm × 0.4 cm × 0.8 cm, with the two prongs spaced by ∼800 µm. To test our sensor we used a quantum cascade laser as the light source and selected a methanol rotational absorption line at 131.054 cm(-1) (∼3.93 THz), with line-strength S = 4.28 × 10(-21) cm mol(-1). The sensor was operated at 10 Torr pressure on the first flexion QTF resonance frequency of 4245 Hz. The corresponding Q-factor was 74 760. Stepwise concentration measurements were performed to verify the linearity of the QEPAS signal as a function of the methanol concentration. The achieved sensitivity of the system is 7 parts per million in 4 seconds, corresponding to a QEPAS normalized noise-equivalent absorption of 2 × 10(-10) W cm(-1) Hz(-1/2), comparable with the best result of mid-IR QEPAS systems.

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).

A frequency-modulated quantum-cascade laser for spectroscopy of CH4 and N2O isotopomers.

We report the development of a novel laser spectrometer for high-sensitivity detection of methane and nitrous oxide. The system relies on a quantum-cascade laser source emitting wavelength of around 8.06 microm, where strong fundamental absorption bands occur for the considered species and their isotopomers. The detection technique is based on audio-frequency and radio-frequency modulation of laser radiation. First experimental tests have been performed to estimate the achievable detection limits and the signal reproducibility levels in view of possible measurements of (13)C/(12)C, (18)O/(16)O, (17)O/(16)O and (15)N/(14)N isotope ratios.

Low-power Lamb-dip spectroscopy of very weak CO(2) transitions near 4.25 mum.

We report saturated-absorption spectra recorded by use of 5 muW of infrared radiation coupled into a build-up cavity. Single-pass generation of difference-frequency radiation tunable near 4.25 mum in a periodically poled LiNbO(3) crystal was used. Lamb dips of weak transitions of the fundamental rovibrational band of CO(2) were observed, for what is believed to be the first time, up to the J=82 level. Application of these results to the extension of frequency-comb-based metrology in the infrared is discussed.