Continuous-wave quantum cascade lasers absorption spectrometers for trace gas detection in the atmosphere

Mid infra-red absorption spectrometry based on continuous-wave distributed feedback (DFB) quantum cascade laser (QCL) is more and more widely used for trace gas detection and pollution monitoring. The main advantages of this technique are high sensitivity, high selectivity and a potential for extreme compactness. Various examples of trace gas detection for atmospheric detection will be presented in this paper. Commercial QCLs available on the shelves were first implemented. A cryogenic QCL emitting at 6.7 μm was used to demonstrate the detection of water vapor and its isotopes. A room-temperature QCL was then used to simultaneously detect methane and nitrous oxide at 7.9 μm. Recently, we have developed a room-temperature top grating DFB QCL designed around 4.5 μm for the demonstration of N₂O detection in the ppb range. Atmospheric applications of these spectrometers will be presented. The improvements of QCL performances make it now possible to develop instruments that are more and more compact and therefore compatible with in situ applications.     

Photoacoustic spectroscopy for trace gas detection with cryogenic and room-temperature continuous-wave quantum cascade lasers

The main characteristics that a sensor must possess for trace gas detection and pollution monitoring are high sensitivity, high selectivity and the capability to perform in situ measurements. The photacoustic Helmholtz sensor developed in Reims, used in conjunction with powerful Quantum Cascade Lasers (QCLs), fulfils all these requirements. The best cell response is # 1200 V W⁻¹ cm and the corresponding ultimate sensitivity is j 3.3 × 10⁻¹⁰ W cm⁻¹¹ Hz^−11/2. This efficient sensor is used with mid-infrared QCLs from Alpes Lasers to reach the strong fundamental absorption bands of some atmospheric gases. A first cryogenic QCL emitting at 7.9 μm demonstrates the detection of methane in air with a detection limit of 3 ppb. A detection limit of 20 ppb of NO in air is demonstrated using another cryogenic QCL emitting in the 5.4 μm region. Real in-situ measurements can be achieved only with room-temperature QCLs. A room-temperature QCL emitting in the 7.9 μm region demonstrates the simultaneous detection of methane and nitrous oxide in air (17 and 7 ppb detection limit, respectively). All these reliable measurements allow the estimated detection limit for various atmospheric gases using quantum cascade lasers to be obtained. Each gas absorbing in the infrared may be detected at a detection limit in the ppb or low-ppb range.     

太赫兹量子级联激光器研究进展

太赫兹技术涉及电磁学、光电子学、半导体物理学、材料科学以及微加工技术等多个学科,它在信息科学、生物学、医学、天文学、环境科学等领域有重要的应用价值.太赫兹辐射源是太赫兹频段应用的关键器件.本文简要介绍了太赫兹电磁波的研究背景、重要特点以及潜在应用,重点讨论了太赫兹半导体量子级联激光器的工作原理和研究进展等.     

太赫兹量子级联激光器研究进展

太赫兹技术涉及电磁学、光电子学、半导体物理学、材料科学以及微加工技术等多个学科，它在信息科学、生物学、医学、天文学、环境科学等领域有重要的应用价值．太赫兹辐射源是太赫兹频段应用的关键器件．本文简要介绍了太赫兹电磁波的研究背景、重要特点以及潜在应用，重点讨论了太赫兹半导体量子级联激光器的工作原理和研究进展等．     

Application of step-scan FTIR to the research of quantum cascade lasers

The principle of step-scan Fourier transform infrared (FTIR) spectroscopy is introduced. Double modulation step-scan FTIR technique is used to obtain the quantum cascade laser's stacked emission spectra in the time domain. Optical property and thermal accumulation of devices due to large drive current are analyzed.     

ZnO-based terahertz quantum cascade lasers

High-power terahertz sources operating at room-temperature are promising for many applications such as explosive materials detection, non-invasive medical imaging, and high speed telecommunication. Here we report the results of a simulation study, which shows the significantly improved performance of room-temperature terahertz quantum cascade lasers (THz QCLs) based on a ZnMgO/ZnO material system employing a 2-well design scheme with variable barrier heights and a delta-doped injector well. We found that by varying and optimizing constituent layer widths and doping level of the injector well, high power performance of THz QCLs can be achieved at room temperature: optical gain and radiation frequency is varied from 108 cm^?1 @ 2.18 THz to 300 cm^?1 @ 4.96 THz. These results show that among II–VI compounds the ZnMgO/ZnO material system is optimally suited for high-performance room-temperature THz QCLs.     

基于中红外分布反馈量子级联激光器的光声光谱技术用于痕量甲烷气体检测

由于工业监控和环境检测的需要,甲烷气体检测日益得到人们的关注。研究了基于中红外分布反馈量子级联激光器(DFB-QCL)的光声光谱技术,并应用于痕量甲烷的检测。自主研发的DFB-QCL室温工作时的激射波长在7.6μm附近,覆盖了甲烷的特征吸收谱线1 316.83cm-1。待测甲烷气体充入亥姆霍兹光声谐振腔中,DFB-QCL的工作频率为234Hz、室温脉冲工作时峰值功率为80mW。中红外光经过甲烷吸收后,产生的声波信号经麦克风检测,由锁相放大器对信号进行采集并输入计算机进行处理。按信噪比为1计算,得到甲烷的探测极限为189nmol.mol-1。     

Comparison between semiclassical and full quantum transport analysis of THz quantum cascade lasers

We implement and compare two theoretical models for stationary electron transport in quantum cascade lasers and Stark ladders. The first one, the nonequilibrium Green's function method is a very general scheme to include coherent quantum mechanics and incoherent scattering with phonons and device imperfections self-consistently. However, it is numerically very demanding and cannot be used for systematic device parameter scans. For this reason, we also implement the approximate, numerically efficient ensemble Monte Carlo method and assess its applicability on the above mentioned transport problems. We identify a transport regime in which results of both methods quantitatively agree. In this regime, the ensemble Monte Carlo method is well suited to propose design improvements.     

Third-order photonic-crystal distributed-feedback quantum cascade lasers

We demonstrate room-temperature operation of broad-area edge-emitting photonic-crystal distributed-feedback quantum cascade lasers at λ ～ 4.6 μm. The lasers use a weak-index perturbed third-order photonic-crystal lattice to control the optical mode in the wafer plane. Utilizing this coupling mechanism, the near-diffraction-limited beam quality with a far-field profile normal to the facet can be obtained. Single-mode operation with a signal-to-noise ratio of about 20 dB is achieved in the temperature range of 85–290 K. The single-facet output power is above 1 W for a 55 μm × 2.5 mm laser bar at 85 K in pulsed mode.     

Nonlinear optics with quantum cascade lasers

We discuss new approaches to monolithic integration of quantum cascade lasers with resonant intersubband nonlinearities. We show that the proposed approaches can greatly enhance the performance of quantum cascade lasers and give rise to new functionalities. Examples considered include extreme frequency up-or down-conversion and wide-range electric tuning.     

Absorption spectroscopy with quantum cascade lasers

Novel pulsed and cw quantum cascade distributed feedback (QC-DFB) lasers operating near lambda=8 micrometers were used for detection and quantification of trace gases in ambient air by means of sensitive absorption spectroscopy. N2O, 12CH4, 13CH4, and different isotopic species of H2O were detected. Also, a highly selective detection of ethanol vapor in air with a sensitivity of 125 parts per billion by volume (ppb) was demonstrated.     

Applications of quantum cascade lasers for sensitive trace gas measurements of CO, CH4, N2O and HCHO

We describe here a sensitive quantum cascade laser absorption spectrometer (QCLAS) employed for aircraft based measurements during the GABRIEL 2005 and HOOVER 2006 and 2007 campaigns. This 3-channel instrument measures CO, HCHO, CH₄ and N₂O using a 64-m path double corner cube White cell. Performance of the instrument was examined for the four species and precisions for CO, N₂O and CH₄ were measured in the field to be 0.5, 0.5 and 0.7% respectively (2σ). The 1σ detection limit for HCHO was ∼500 pptv for a 2 s average, while signal averaging of the HCHO over a 2 min time interval resulted in a 150 pptv detection limit with a duty cycle of 60%. PACS  82.80.Gk; 07.88.+y; 42.62.-b; 92.60.H-     

Photoacoustic spectroscopy with quantum cascade distributed-feedback lasers

We present photoacoustic (PA) spectroscopy measurements of carbon dioxide, methanol, and ammonia. The light source for the excitation was a single-mode quantum cascade distributed-feedback laser, which was operated in pulsed mode at moderate duty cycle and slightly below room temperature. Temperature tuning resulted in a typical wavelength range of 3cm(-1)at a linewidth of 0.2cm(-1). The setup was based on a Herriott multipass arrangement around the PA cell; the cell was equipped with a radial 16-microphone array to increase sensitivity. Despite the relatively small average laser power, the ammonia detection limit was 300 parts in 10(9)by volume.     

Free-running frequency stability of mid-infrared quantum cascade lasers

The intrinsic frequency fluctuations of two single-mode quantum cascade (QC) distributed-feedback lasers operating continuously at a wavelength of 8.5 mum are reported. A Doppler-limited rovibrational resonance of nitrous oxide is used to transform the frequency noise into measurable intensity fluctuations. The QC lasers, along with recently improved current controllers, exhibit a free-running frequency stability of 150 kHz over a 15-ms time interval.     

Passive synthesis rules of coupled-cavity quantum cascade lasers

A new approach to passive electromagnetic modelling of coupled–cavity quantum cascade lasers is presented in this paper. One of challenges in the rigorous analysis of such eigenvalue problem is its large size as compared to wavelength and a high quality factor, which prompts for substantial computational efforts. For those reasons, it is proposed in this paper to consider such a coupled-cavity Fabry-Perot resonant structure with partially transparent mirrors as a two-port network, which can be considered as a deterministic problem. Thanks to such a novel approach, passive analysis of an electrically long laser can be split into a cascade of relatively short sections having low quality factor, thus, substantially speeding up rigorous electromagnetic analysis of the whole quantum cascade laser. The proposed method allows to determine unequivocally resonant frequencies of the structure and the corresponding spectrum of a threshold gain. Eventually, the proposed method is used to elaborate basic synthesis rules of coupled–cavity quantum cascade lasers.     

Very low threshold operation of quantum cascade lasers

A strain-compensated InP-based quantum cascade laser(QCL) structure emitting at 4.6 μm is demonstrated,based on a two-phonon resonant design and grown by solid-source molecular beam epitaxy(MBE).By optimizing the growth parameters,a very high quality heterostructure with the lowest threshold current densities ever reported for QCLs was fabricated.Threshold current densities as low as 0.47 kA/cm~2 in pulsed operation and 0.56 kA/cm~2 in continuous-wave(cw) operation at 293 K were achieved for this state-of-the-art QCL.A minimum power consumption of 3.65 W was measured for the QCL,uncooled,with a high-reflectivity(HR) coating on its rear facet.     

Solid source MBE growth of quantum cascade lasers

High material quality is the basis of quantum cascade lasers (QCLs). Here we report the solid source molecular beam epitaxy (MBE) growth details of realizing high quality of InGaAs/InAlAs QCL structures. Accurate control of material compositions, layer thickness, doping profile, and interface smoothness can be realized by optimizing the growth conditions. Double crystal x-ray diffraction discloses that our grown QCL structures possess excellent periodicity and sharp interfaces. High quality laser wafers are grown in a single epitaxial run. Room temperature continuous-wave (cw) operation of QCLs is demonstrated.     

Kilohertz linewidth from frequency-stabilized mid-infrared quantum cascade lasers

Frequency stabilization of mid-IR quantum cascade (QC) lasers to the kilohertz level has been accomplished by use of electronic servo techniques. With this active feedback, an 8.5-microm QC distributed-feedback laser is locked to the side of a rovibrational resonance of nitrous oxide (N(2) O) at 1176.61cm (-1) . A stabilized frequency-noise spectral density of 42Hz/ radicalHz has been measured at 100 kHz; the calculated laser linewidth is 12 kHz.     

External-cavity quantum cascade lasers with fast wavelength scanning

Fast wavelength scanning of an external-cavity quantum cascade laser (EC-QCL) has been developed using a modified Littrow-type cavity configuration. Scan rates up to 5 kHz and tuning ranges up to 7 cm⁻¹ have been realized using folded cavity arrangement with a fast piezoactuated intracavity mirror to vary the effective diffraction grating angle. High-resolution molecular spectroscopy, limited primarily by the effective laser linewidth, has been demonstrated in pulsed and CW mode using direct absorption spectroscopy of ammonia and ethylene in the 10-μm wavelength region. A high-resolution broadband spectral scan employing mode-hop-free tuning of a set of discrete laser modes within the fast frequency scan has been developed. The method has been demonstrated by performing high-resolution broadband spectrum of ethylene under atmospheric and reduced pressures.     

Theory of single-mode lasing in coherent quantum cascade lasers

A theory is developed for steady-state single-mode lasing in coherent quantum-well cascade lasers. This laser model is an example of a strictly quantum mechanical problem in which approximate kinetic approaches are not used to account for dissipative scattering processes. Exact wave functions are found for the system in weak and strong electromagnetic fields, so that the output power and frequency can be determined as functions of the coherent pump current and system parameters. It is shown that for pumping by monoenergetic electrons the power has a nonlinear (root) dependence and tends to saturate in strong fields. It is predicted that the coherent pumping efficiency may be increased by adjusting the energy of the pump electrons, which will lead to a linear power dependence, a high efficiency, and low threshold currents. A population inversion is found not be a necessary condition for lasing in the coherent laser. In particular, in the high field regime the population of the lower level exceeds that of the upper, while in the optimally adjusted regime they are the same. Zh. éksp. Teor. Fiz. 112, 483–498 (August 1997)