Distributed feedback quantum cascade laser with optically tunable emission frequency

We present the design and the performance of midinfrared distributed feedback (DFB) quantum cascade lasers (QCLs) made of strain balanced Ga <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">x</sub> In <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">1-x</sub> As/Al <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">y</sub> In <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">1-y</sub> As material on InP substrates for sensing CO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> , N <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> O, and NO in the middle wavelength range of mid-IR from 4 to 6 μm. We present the performances of our DFB QCLs at three different aspects: high power, low threshold power consumption, and wide wavelength coverage. We demonstrated a continuous wave (CW) DFB QCL with an output power of 220mW at 20°C, a CW DFB QCL with low threshold voltage of 8V and low-divergent far-field angles of 27.5° × 32.9° by reducing the number of quantum cascaded stages, a CW DFB QCL with a low threshold power consumption of 0.7W by reducing doping density in the active core, and DFB QCLs wide wavelength coverage of 325 cm <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">-1</sup> , 16.9% of center wavelength at 5.2 μm, within one wafer by changing the grating period. 12 DFB QCL chips have being aged for 3000 h under 25°C and a constant quasi-CW current of 0.37 A. No decrease in power was observed.

Quantum cascade lasers are unipolar semiconductor lasers based on intersubband transitions in heterostructures. These lasers, which have demonstrated continuous wave operation at room temperature in the mid-infrared spectral range, are well suited for the realization of compact, ultra-sensitive, trace-gas sensors based on absorption spectroscopy. Up to now, only distributed feedback (DFB) single-mode devices have been used for such applications. DFB quantum cascade lasers have proven to be effective for gas sensing, but their relatively narrow tuning range, smaller or equal to about 1% of the wavelength, makes them not very versatile and limits their usefulness for spectroscopic investigations. In this thesis we developed broadly tunable external cavity quantum cascade lasers. The main advantage of these sources compared with DFBs is their broader tuning range, which is limited only by the spectral bandwidth of the gain element. We particularly studied broad gain bandwidth active regions based on bound-to-continuum designs. With that kind of active region, we have demonstrated a tuning range equal to 15% of the center wavelength at ~ 10 m, which was three times broader than the best values reported in the literature at that time, as well as good performance in pulsed mode at room temperature. Using a strain-compensated bound-to-continuum design emitting near 5.2 m, we have demonstrated for the first time continuous-wave operation of an external cavity quantum cascade laser on a thermoelectric cooler. The tuning range was comparable to that of pulsed devices, but with a much better side-mode suppression ratio and a much narrower linewidth. This continuous-wave device has successfully been applied to the spectroscopy of nitric oxide in collaboration with Prof. Tittel's Laser Science Group at Rice University. High resolution absorption spectra of that gas could be acquired over a large wavelength range. We also studied heterogeneous cascade structures, that is quantum cascade structures in which the various stages emit at several different wavelengths, as a way to increase further the tuning range of external cavity quantum cascade lasers. A pulsed laser tunable from 8.2 to 10.4 m, that is over 24% of the center wavelength has been realized using an active region composed of two substacks of bound-to-continuum designs. We conclude on the feasibility of room temperature, continuous-wave, broadly-tunable external cavity quantum cascade lasers in the mid-infrared spectral range. These devices will be useful for the analysis of multi-component gases, for high resolution spectroscopic investigations in fundamental science, and for the detection of heavy molecules with broad absorption features which DFB quantum cascade lasers cannot scan entirely.

We demonstrate surface-grating distributed feedback quantum cascade lasers (QCLs) with a watt-level power output at 4.75 μm. A device with a 5 mm cavity length exhibits an output power of 1.1 W in room-temperature cw operation. Single-mode operation with a side mode suppression ratio of 30 dB is obtained in the working temperature of 15–105 °C. A double-lobed far field with negligible beam steering is observed. The significance of this demonstration lies in its simplicity and readiness to be applied to standard QCL wafers with the promise of high-power performances.

We demonstrate phase locking of a 4.7 THz distributed feedback quantum cascade laser (QCL) to a stable laboratory synthesizer. The QCL operates at 4747.9 GHz with 1 mW output power, mounted on the first stage of a pulse-tube cryocooler with mechanical dampers. Despite residual mechanical vibrations, the QCL radiation is successfully coupled out through a series of cold and warm mirrors and focused onto a room-temperature superlattice diode (SLD). The SLD is pumped by a 182.6 GHz signal from a diode frequency multiplier chain and generates the 26th harmonic at 4748.2 GHz for harmonic mixing as a phase reference. This produces a 327 MHz intermediate frequency (IF) that is amplified, filtered, and fed to a balanced diode mixer phase detector. The phase-locked loop employs a loop filter to generate correction signals for QCL current adjustment, reducing the unlocked linewidth from approximately 10 MHz to 1 Hz (limited by resolution bandwidth of spectrum analyzer). In addition of providing absolute frequency reference and ability of introducing fine frequency steps, the system demonstrates remarkable robustness, maintaining phase lock for several hours and even under low signal-to-noise conditions such as 1 dB of signal over noise at 3 MHz resolution bandwidth.This robustness comes from tailored PLL design, incorporating a diode ring mixer as phase detector and a linear phase narrow band filter, and proves its suitability for practical heterodyne array receivers targeting the [OI] line at 4.7 THz.

Optical feedback cavity-enhanced absorption spectroscopy (OF CEAS) has been demonstrated with a thermoelectrically cooled continuous wave distributed feedback quantum cascade laser (QCL) operating at wavelengths around 7.84 μm. The QCL is coupled to an optical cavity which creates an absorption pathlength greater than 1000 m. The experimental design allows optical feedback of infra-red light, resonant within the cavity, to the QCL, which initiates self-locking at each TEM00 cavity mode frequency excited. The QCL linewidth is narrowed to below the mode linewidth, greatly increasing the efficiency of injection of light into the cavity. At the frequency of each longitudinal cavity mode, the absorption coefficient of an intracavity sample is obtained from the transmission at the mode maximum, measured with a thermoelectrically cooled detector: spectral line profiles of CH4 and N2O in ambient air were recorded simultaneously and with a resolution of 0.01386 cm−1. A minimum detectable absorption coefficient of 5.5×10−8 cm−1 was demonstrated after an averaging time of 1 s for this completely thermoelectrically cooled system. The bandwidth-normalised limit for a single cavity mode is 5.6×10−9 cm−1 Hz−1/2 (1σ).

We report on an application of a pulsed distributed feedback quantum cascade laser (QCL) for long open path readout system of multiple passive temperature, pressure, humidity or other sensors. Unlike the usually used active sensors, containing radio or optical data transmitters, the presented system does not contains any active transmitters at the sensors side. The QCL and the receiver are displaced on one side of the path. On the opposite path side, a modified Michelson interferometer, based on corner cube retroreflectors, is placed. One retroreflector is fixed and another one is attached to the appropriate sensor, which moves it when the measured parameter is changed. The useful travel range of the movable retroreflector is less than lambda/2 (4.8 mum) to obtain a monotonic transfer function between the measured parameters and the received signals. This system measures distances in the micrometer and sub-micrometer range but displaced up to a few kilometers from the transmitter/receiver station. A relatively long laser pulse of 150-200 ns is used to scan the interferometers and to read out the information. During the pulse, the QCL frequency is swept within a 40 GHz range. This frequency sweeping allows decreasing significantly the influence of the atmospheric turbulence over the accuracy of the data transfer. When the swept radiation illuminates the interferometer, oscillations in the received signal occur due to the interference between the different parts of the beam. The period of the oscillations and the oscillation phase depend on the distance between retroreflectors and the changes in this distance, respectively. The main advantage of the system proposed is that a single transmitter-receiver pair allows reading out multiple sets of completely passive sensors offering high level of data protection due to the low beam divergency

A non-invasive CO2 gas temperature sensing technique at or close to the room temperature range based on quantum cascade laser absorption spectroscopy is presented. The method probes thermally populated ground state and hot-band rotational-vibrational transitions of CO2 in the frequency range from 2349 to 2351 cm−1 from which the gas temperature is obtained from Boltzmann statistics. Transmission spectra are recorded by injection-current driven frequency-scans, the so-called inter pulse mode, of a pulsed distributed feedback quantum cascade laser. The statistical uncertainty (1σ) in temperature for single frequency scans with time resolution of 10 ms is 4 K and can be further reduced down to ∼50 mK by long-time averaging of about 1 min. The technique is evaluated with particular emphasis on implementation, data acquisition, data analysis and potential improvements.

We have performed high resolution spectroscopy of rotational lines of <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">12</sup> CH <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3</sub> <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">16</sup> OH in a THz spectrometer based on a 2.5 THz distributed feedback quantum cascade laser (QCL). The absolute frequency was determined simultaneously with the absorption measurement by mixing part of the radiation from the QCL with the radiation from a THz gas laser in a Schottky diode.

A continuous wave, distributed feedback quantum cascade laser based absorption system was developed and demonstrated for simultaneous atmospheric CH 4 , N 2 O and H 2 O detection, with minimum detection limits below 2% of their typical atmospheric concentrations.

Two-segment distributed feedback (DFB) GaAs/AlGaAs bound-to-continuum quantum cascade lasers emitting at ∼10.8 µm were fabricated and investigated. Reversible switching between two different DFB modes by current injection control yielding sidemode suppression ratios up to >23 dB is reported. Two different devices were fabricated for which the distance between the different DFB modes is 1.5 and 2.5 cm−1, respectively, and quasi-continuous tuning over a range of >9 cm−1 (105 nm) between 120 and 250 K was observed.

We report on the development of a heterodyne receiver at mid-infrared wavelength for high-resolution spectroscopy applications. The receiver employs a superconducting NbN hot electron bolometer as a mixer and a room temperature distributed feedback quantum cascade laser operating at 10.6 μm (28.2 THz) as a local oscillator. The stabilization of the heterodyne receiver has been achieved using a feedback loop controlling the output power of the laser. Improved Allan variance times as well as a double sideband receiver noise temperature of 5000 K and a noise bandwidth of 2.8 GHz of the receiver system are demonstrated.

13CO 2/ 12CO 2 isotopic ratio measurements with a continuous-wave quantum cascade laser in exhaled breath

Precise knowledge of the linewidth enhancement factor of a semiconductor laser under actual operating conditions is of prime importance since this parameter dictates various phenomena such as linewidth broadening or optical nonlinearities enhancement. The above-threshold linewidth enhancement factor of a mid-infrared quantum cascade laser structure operated at 10∘C is determined experimentally using two different methods based on optical feedback. Both Fabry-Perot and distributed feedback quantum cascade lasers based on the same active area design are studied, the former by following the wavelength shift as a function of the feedback strength and the latter by self-mixing interferometry. The results are consistent and unveil a clear pump current dependence of the linewidth enhancement factor, with values ranging from 0.8 to about 3.

Complex-coupled edge-emitting photonic crystal distributed feedback quantum cascade lasers at λ ∼ 7.6 μm

&amp;lt;p&amp;gt;Water vapor is the dominant greenhouse gas, and its abundance in the upper tropospheric/lower stratospheric region (UTLS, 8-25&amp;amp;#160;km altitude) is of great importance to the Earth's radiative balance. Reliable predictions of the climate evolution as well as the understanding of cloud-microphysical processes require the accurate and frequent measurement of water vapor concentrations at these altitudes. The only established method for high-accuracy UTLS water vapor measurements aboard of meteorological balloons is cryogenic frost-point hygrometry (CFH). However, the cooling agent required for its operation (CHF&amp;lt;sub&amp;gt;3&amp;lt;/sub&amp;gt;) is to be phased out due to its strong global warming potential. It is, therefore, a major, worldwide challenge to ensure the continuation of the observation of this key Environmental Climate Variable (ECV) of the World Meteorological Organization (WMO). As an alternative method, we present a compact and lightweight instrument based on quantum cascade laser absorption spectroscopy (QCLAS) that reduces systematic errors by contactless and contamination-minimized measurements. Its construction addresses the stringent constraints posed by the harsh environmental conditions found in the UTLS. This is achieved by a fundamental reconsideration of main components of the spectrometer. We developed a highly versatile segmented circular multipass cell (SC-MPC) which supports compact and well-controlled beam folding [1]. The SC-MPC consists of a monolithic aluminum ring with 10.8 cm inner radius, containing 57 quadratic, spherically curved segments, seamlessly shaped into the internal ring surface. The collimated mid-IR beam (&amp;amp;#955; = 6 &amp;amp;#181;m) from the distributed feedback quantum cascade laser (DFB-QCL) is directly coupled to the MPC without the need for additional beam-shaping optics. This leads to a resilient optical setup suitable for mobile applications and rough environmental conditions. Water vapor amount fractions of &amp;lt;10 ppmv can be measured with a precision better than 1% at 1 Hz. Measuring in open-path mode ensures quick response and minimal interference by water desorbing from surfaces. The instrument weighs less than 4 kg (including battery) and has an average power consumption of 15 W. An elaborate thermal management system that comprises phase change materials and thermoelectric cooling ensures excellent internal temperature stability despite an outside temperature difference of up to 80 K. Specifically developed hard- and software guarantee autonomous operation for the duration of flight [2]. Extensive stability assessments in climate chambers as well as validation experiments using dynamically generated, SI-traceable water vapor mixtures were performed in collaboration with the Swiss Federal Institute of Metrology (METAS). In cooperation with the German Weather Service (DWD) in Lindenberg, the instrument was successfully tested and compared to CFH in two consecutive balloon-ascents in December 2019 up to 28 km altitude, experiencing temperatures and pressures as low as &amp;amp;#8211;65&amp;amp;#176;C and 16 hPa, respectively. The drastic reduction in mass and size of a laser absorption-spectrometer and its successful deployment under harshest conditions represents a paradigm change in portable laser spectroscopy and opens the door to previously inaccessible applications.&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;[1] Graf, M.; Emmenegger, L.; Tuzson, B. Opt. Lett. 2018, 43, 2434-2437&amp;lt;/p&amp;gt;&amp;lt;p&amp;gt;[2] Liu, C. et al., L. Rev. Sci. Instrum. 2018, 89 (6), 065107 (9 pp.)&amp;lt;/p&amp;gt;