Rapid Detection of Volatile Organic Compounds by Switch-Scan Tuning of Vernier Quantum-Cascade Lasers.

Volatile organic compounds (VOCs) exhibit typically broad and mutually overlapping ro-vibrational absorption fingerprints. This complexity has so far limited the applicability of laser-based spectroscopy for VOC measurements in complex gas matrices. Here, we exploit a Vernier-type quantum-cascade laser (QCL) as an electrically tunable multiwavelength source for selective and sensitive VOC analysis. This emerging class of lasers provides access to several spectral windows by discrete Vernier tuning ("switching") and continuous coverage within these windows ("scanning"). We present a versatile driving technique that efficiently combines the two tuning mechanisms. Applied to our Vernier QCL, it enables the rapid acquisition (within 360 ms) of high-resolution spectra from six individual spectral windows, distributed over a wide range from 1063 to 1102 cm-1. Gaining access to the broad absorption envelopes of VOCs at multiple frequencies, along with their superimposed fine structure, which are especially pronounced at a reduced sample pressure, offers completely new opportunities in VOC analysis. The potential of this approach is assessed in a direct-laser-absorption setup with acetaldehyde, ethanol, and methanol as benchmark compounds with significant spectral overlaps. A measurement precision of 1-10 ppb is obtained after integration for 10 s at amount fractions below 10 ppm, and excellent linearity is found over at least 3 orders of magnitude. Combined with our dedicated spectral fitting algorithm, we demonstrate highly selective multicompound analyses with less than 3.5% relative expanded uncertainty, even in the presence of a 40× excess of an interfering compound with complete spectral overlap.

Multi-gas quartz-enhanced photoacoustic sensor for environmental monitoring exploiting a Vernier effect-based quantum cascade laser.

We report on a gas sensor based on quartz-enhanced photoacoustic spectroscopy (QEPAS) able to detect multiple gas species for environmental monitoring applications, by exploiting a Vernier effect-based quantum cascade laser as the excitation source. The device emission spectrum consists of ten separated emission clusters covering the range from 2100 up to 2250 cm-1. Four clusters were selected to detect the absorption features of carbon monoxide (CO), nitrous oxide (N2O), carbon dioxide (CO2), and water vapor (H2O), respectively. The sensor was calibrated with certified concentrations of CO, N2O and CO2 in a wet nitrogen matrix. The H2O absorption feature was used to monitor the water vapor within the gas line during the calibration. Minimum detection limits of 6 ppb, 7 ppb, and 70 ppm were achieved for CO, N2O and CO2, respectively, at 100 ms of integration time. As proof of concept, the QEPAS sensor was tested by continuously sampling indoor laboratory air and monitoring the analytes concentrations.

High performance quantum cascade laser frequency combs at λ ∼ 6 µm based on plasmon-enhanced dispersion compensation.

We demonstrate quantum cascade laser (QCL) optical frequency combs emitting at λ ∼ 6 µm. A 5.5 µm-wide, 4.5 mm-long laser exhibits comb operation from -20 °C up to 50 °C. A maximum output power of 300 mW is achieved at 50 °C showing a robustness of the system. The laser output spectrum is ∼80 cm-1 wide at the maximum current, with a mode spacing of 0.334 cm-1, resulting in a total of 240 modes with an average power of 0.8 mW per mode. To achieve frequency comb operation, a plasmonic-waveguide approach is utilized. A thin, highly-doped indium phosphide (InP) layer is inserted in the top cladding design to compensate the positive dispersion of the system (material and waveguide). This approach can be further exploited to design QCL combs at even shorter wavelengths, down to 4 µm. Different ridge widths between 2.8 and 5.5 µm have been fabricated and characterized. All of the devices exhibit frequency comb operation. These observations demonstrate that the plasmonic-waveguide is a robust and reliable method for dispersion compensation of a semiconductor laser systems to achieve frequency comb operation.

Quantum cascade lasers with discrete and non equidistant extended tuning tailored by simulated annealing.

In this work, we report a new superstructure grating design method for broad, non-equidistant discrete tuning in quantum cascade lasers using the Vernier effect. Our approach is applied to a wafer with gain centred at ∼7.8 µm. Measurements of a 3.75 mm long device are presented yielding 3.66% tuning around the central frequency and a peak optical power over 200 mW at 0 ∘C heat sink temperature. In addition, we show that taking into account the optical dispersion of the material is crucial to fulfill narrow specifications. Our device is particularly well suited for multi absorption line spectroscopic measurements requiring high resolution and small form factor for high volume production.

WaterSpy: A High Sensitivity, Portable Photonic Device for Pervasive Water Quality Analysis.

In this paper, we present WaterSpy, a project developing an innovative, compact, cost-effective photonic device for pervasive water quality sensing, operating in the mid-IR spectral range. The approach combines the use of advanced Quantum Cascade Lasers (QCLs) employing the Vernier effect, used as light source, with novel, fibre-coupled, fast and sensitive Higher Operation Temperature (HOT) photodetectors, used as sensors. These will be complemented by optimised laser driving and detector electronics, laser modulation and signal conditioning technologies. The paper presents the WaterSpy concept, the requirements elicited, the preliminary architecture design of the device, the use cases in which it will be validated, while highlighting the innovative technologies that contribute to the advancement of the current state of the art.

Electrically-driven pure amplitude and frequency modulation in a quantum cascade laser.

We present pure amplitude modulation (AM) and frequency modulation (FM) achieved electrically in a quantum cascade laser (QCL) equipped with an integrated resistive heater (IH). The QCL output power scales linearly with the current applied to the active region (AR), but decreases with the IH current, while the emission frequency decreases with both currents. Hence, a simultaneous modulation applied to the current of the AR and IH sections with a proper relative amplitude and phase can suppress the AM, resulting in a pure FM, or vice-versa. The adequate modulation parameters depend on the applied modulation frequency. Therefore, they were first determined from the individual measurements of the AM and FM transfer functions obtained for a modulation applied to the current of the AR or IH section, respectively. By optimizing the parameters of the two modulations, we demonstrate a reduction of the spurious AM or FM by almost two orders of magnitude at characteristic frequencies of 1 and 10 kHz compared to the use of the AR current only.

Frequency stability of a dual wavelength quantum cascade laser.

We characterized the dual wavelength operation of a distributed Bragg reflector (DBR) quantum cascade laser (QCL) operating at 4.5 µm using two independent optical frequency discriminators. The QCL emits up to 150 mW fairly evenly distributed between two adjacent Fabry-Perot modes separated by ≈11.6 GHz. We show a strong correlation between the instantaneous optical frequencies of the two lasing modes, characterized by a Pearson correlation coefficient of 0.96. As a result, we stabilized one laser mode of the QCL to a N2O transition using a side-of-fringe locking technique, reducing its linewidth by a factor 6.2, from 406 kHz in free-running operation down to 65 kHz (at 1-ms observation time), and observed a simultaneous reduction of the frequency fluctuations of the second mode by a similar amount, resulting in a linewidth narrowing by a factor 5.4, from 380 kHz to 70 kHz. This proof-of-principle demonstration was performed with a standard DBR QCL that was not deliberately designed for dual-mode operation. These promising results open the door to the fabrication of more flexible dual-mode QCLs with the use of specifically designed gratings in the future.

Plasmon-enhanced waveguide for dispersion compensation in mid-infrared quantum cascade laser frequency combs.

We demonstrate dispersion compensation in mid-infrared quantum cascade laser frequency combs (FCs) emitting at 7.8 µm using the coupling of a dielectric waveguide to a plasmonic resonance in the top cladding layer of the latter. Devices with group velocity dispersion lower than 110 fs2/mm were fabricated, and narrow beatnotes with FWHM linewidths below 1 kHz were measured on the entire operation range. At -20°C, the optical output power reaches 275 mW, and the optical spectrum spans 60 cm-1. The multi-heterodyne beating spectrum of two devices was measured and spans 46 cm-1, demonstrating the potential of dispersion-engineered waveguides for the fabrication of highly stable and reliable quantum cascade laser FCs with high output power across the mid-infrared.

Mid infrared quantum cascade laser operating in pure amplitude modulation for background-free trace gas spectroscopy.

We present a single mode multi-section quantum cascade laser source composed of three different sections: master oscillator, gain and phase section. Non-uniform pumping of the QCL's gain reveals that the various laser sections are strongly coupled. Simulations of the electronic and optical properties of the laser (based on the density matrix and scattering matrix formalisms, respectively) were performed and a good agreement with measurements is obtained. In particular, a pure modulation of the laser output power can be achieved. This capability of the device is applied in tunable-laser spectroscopy of N2O where background-free quartz enhanced photo acoustic spectral scans with nearly perfect Voigt line shapes for the selected absorption line are obtained.

Gain-guided broad area quantum cascade lasers emitting 23.5 W peak power at room temperature.

We report gain-guided broad area quantum cascade lasers at 4.55 µm. The devices were processed in a buried heterostructure configuration with a current injector section much narrower than the active region. They demonstrate 23.5 W peak power at a temperature of 20°C and duty cycle of 1%, while their far field consists of a single symmetric lobe centered on the optical axis. These experimental results are supported well by 2D numerical simulations of electric currents and optical fields in a device cross-section.

High power and single mode quantum cascade lasers.

We present a single mode quantum cascade laser with nearly 1 W optical power. A buried distributed feedback reflector is used on the back section for wavelength selection. The laser is 6 mm long, 3.5 µm wide, mounted episide-up and the laser facets are left uncoated. Laser emission is centered at 4.68 µm. Single-mode operation with a side mode suppression ratio of more than 30 dB is obtained in whole range of operation. Farfield measurements prove a symmetric, single transverse-mode emission in TM00-mode with typical divergences of 41° and 33° in the vertical and horizontal direction respectively. This work shows the potential for simple fabrication of high power lasers compatible with standard DFB processing.

Extended tuning of mid-ir quantum cascade lasers using integrated resistive heaters.

We present single mode quantum cascade lasers including a microscopic heater for spectral emission tuning. Through the use of a buried heater element, the active region temperature can be modified without changing the submount one. Emission frequency tuning in continuous-wave as large as 9 cm(-1) at 1270 cm(-1) and 14 cm(-1) at 2040 cm(-1) are observed, corresponding to an increase of the active region temperatures of ∼ 90 K. Due to the proximity of the heaters to the active region, emission can be modulated at several kHz range and the absence of moving parts guarantees the mechanical stability of the system. This method can be successfully applied to all buried heterostructure lasers, becoming an attractive solution for molecular spectroscopy in the IR. Using the presented devices, molecular absorptions of N(2)O have been measured between 1270 cm(-1) and 1280 cm(-1) and are in agreement with data from the HITRAN database.

High performance, low dissipation quantum cascade lasers across the mid-IR range.

In this work, we present the development of low consumption quantum cascade lasers across the mid-IR range. In particular, short cavity single-mode lasers with optimised facet reflectivities have been fabricated from 4.5 to 9.2 µm. Threshold dissipated powers as low as 0.5 W were obtained in continuous wave operation at room temperature. In addition, the beneficial impact of reducing chip length on laser mounting yield is discussed. High power single-mode lasers from the same processed wafers are also presented.

Broadband superluminescence, 5.9 µm to 7.2 µm, of a quantum cascade gain device.

The broadband electroluminescence of a quantum cascade device based on a multi-color active region covering the wavelengths 5.9 µm - 7.2 µm was measured. Anti-reflection coatings were applied on both cleaved facets to remove the Fabry-Pérot cavity and prevent the device from lasing. This allows the latter to be studied either as a superluminescent diode or a single-pass amplifier in order to determine its suitability as a source for low speckle imaging applications. At 243 K, the amplified spontaneous emission has a peak power of 38 µW that agrees well with a simple model of spontaneous emission intensity. The light of a similar structure could be modulated up to 1 GHz, limited by the RC constant of the device. The peak gain was measured from high-resolution luminescence spectra and determined to be 6.3 cm⁻¹, corresponding to a single-pass gain of 1.89.

All-electrical frequency noise reduction and linewidth narrowing in quantum cascade lasers.

A novel all-electrical method of frequency noise reduction in quantum cascade lasers (QCLs) is proposed. Electrical current through the laser was continuously adjusted to compensate for fluctuations of the laser internal resistance, which led to an active stabilization of the optical emission frequency. A reduction of the linewidth from 1.7 MHz in the standard constant current mode of operation down to 480 kHz is demonstrated at 10-ms observation time when applying this method to a QCL emitting at 7.9 µm.

Dual-comb spectroscopy based on quantum-cascade-laser frequency combs.

Dual-comb spectroscopy performed in the mid-infrared-where molecules have their strongest rotovibrational absorption lines-offers the promise of high spectral resolution broadband spectroscopy with very short acquisition times (µs) and no moving parts. Recently, we demonstrated frequency comb operation of a quantum-cascade-laser. We now use that device in a compact, dual-comb spectrometer. The noise properties of the heterodyne beat are close to the shot noise limit. Broadband (15 cm(-1)) high-resolution (80 MHz) absorption spectroscopy of both a GaAs etalon and water vapour is demonstrated, showing the potential of quantum-cascade-laser frequency combs as the basis for a compact, all solid-state, broadband chemical sensor.

Mid-infrared frequency comb based on a quantum cascade laser.

Optical frequency combs act as rulers in the frequency domain and have opened new avenues in many fields such as fundamental time metrology, spectroscopy and frequency synthesis. In particular, spectroscopy by means of optical frequency combs has surpassed the precision and speed of Fourier spectrometers. Such a spectroscopy technique is especially relevant for the mid-infrared range, where the fundamental rotational-vibrational bands of most light molecules are found. Most mid-infrared comb sources are based on down-conversion of near-infrared, mode-locked, ultrafast lasers using nonlinear crystals. Their use in frequency comb spectroscopy applications has resulted in an unequalled combination of spectral coverage, resolution and sensitivity. Another means of comb generation is pumping an ultrahigh-quality factor microresonator with a continuous-wave laser. However, these combs depend on a chain of optical components, which limits their use. Therefore, to widen the spectroscopic applications of such mid-infrared combs, a more direct and compact generation scheme, using electrical injection, is preferable. Here we present a compact, broadband, semiconductor frequency comb generator that operates in the mid-infrared. We demonstrate that the modes of a continuous-wave, free-running, broadband quantum cascade laser are phase-locked. Combining mode proliferation based on four-wave mixing with gain provided by the quantum cascade laser leads to a phase relation similar to that of a frequency-modulated laser. The comb centre carrier wavelength is 7 micrometres. We identify a narrow drive current range with intermode beat linewidths narrower than 10 hertz. We find comb bandwidths of 4.4 per cent with an intermode stability of less than or equal to 200 hertz. The intermode beat can be varied over a frequency range of 65 kilohertz by radio-frequency injection. The large gain bandwidth and independent control over the carrier frequency offset and the mode spacing open the way to broadband, compact, all-solid-state mid-infrared spectrometers.

Room-temperature continuous-wave operation of an external-cavity quantum cascade laser.

Room-temperature, continuous-wave operation of an external-cavity quantum cascade laser (EC-QCL) is reported. Single-mode tuning range of 120 cm(-1) was achieved, from 7.96 to 8.84 microm. The gain chips utilized are based on the bound to continuum design and were fabricated as buried heterostructure lasers. Gap-free tuning (mode hops only on the external-cavity modes) is demonstrated for an antireflection-coated laser, just by grating rotation. The EC-QCL was implemented in a Littrow setup and an average power of 1.5 mW was obtained at 20 degrees C, while a peak power of 20 mW was obtained for a modified Littrow setup with the back extraction of light.

Characterization of a near-room-temperature, continuous-wave quantum cascade laser for long-term, unattended monitoring of nitric oxide in the atmosphere.

We report on power, spectral linewidth, and mode purity for a cw 5.3 microm quantum cascade laser operated on a thermo-electric cooler. A totally noncryogenic nitric oxide monitor was constructed by integrating this laser with an astigmatic multipass cell and a thermo-electrically cooled infrared detector. The resulting instrument is capable of continuous unattended monitoring of ambient, atmospheric nitric oxide for several weeks with no operator intervention. The detection method was rapid sweep, direct absorption spectroscopy. A detection sensitivity of 0.03 parts in 10(9) is achieved with 30 s averaging time with a path length of 210 m, corresponding to an absorbance path length product of 1.5 x 10(-10) cm(-1).

Terahertz emission from quantum cascade lasers in the quantum Hall regime: evidence for many body resonances and localization effects.

A terahertz quantum cascade laser, operating at lambda=159 microm and exploiting the in-plane confinement arising from perpendicular magnetic field, is used to investigate the physics of electrons confined on excited subbands in the regime of a large ratio of the magnetic field confinement energy to the photon energy. As the magnetic field is increased above about 6 T, and the temperature lowered below 20 K, the devices are characterized by a very low threshold current density, with values as low as J(th)=1A/cm(2), and an increase of gain by five times the low field value. We show that, as with the quantum Hall effect, the key physical process is the localization of the carriers. Evidences for resonant electron-electron scattering processes are directly obtained from light intensity and transport measurements.