Monolithic tunable terahertz quantum cascade laser source based on difference frequency generation

Room-temperature terahertz (THz) quantum cascade laser sources with intracavity difference-frequency nonlinear mixing are electrically pumped monolithic semiconductor laser sources operating in the 0.6–6 THz spectral range. We report widely tunable, low-frequency THz quantum cascade laser sources using a lens-coupled Cherenkov waveguide scheme. Based on a watt-class high-power, λ ∼ 13.7 μm quantum cascade laser, the monolithic THz source is strongly coupled with a high-resistivity silicon lens, which causes a major increase in the THz coupling efficiency and demonstrates significant performance improvements. A room-temperature 1.5 THz device produces a 0.2 mW peak output power with a high-quality beam pattern. Improved THz outcoupling efficiency using the lens-coupled scheme enabled the demonstration of a high-performance external-cavity semiconductor THz source that is tunable from 420 GHz to 2 THz. The external-cavity, lens-coupled device configuration can technically be assembled into a butterfly-style package for a thumb-sized, widely frequency tunable THz semiconductor source.

This paper aims to integrate AlInAs/InGaAs quantum well structures with high second-order nonlinear susceptibility into a dual-wavelength quantum cascade laser (QCL) for difference frequency generation (DFG) of THz radiation. The QCL active region contains two sections: a section with 30 cascades of bound-to-continuum design with integrated optical nonlinearity emitting at 8.7 mum and a section with 20 cascades of two-phonon design emitting at 7.6 mum. The nonlinear susceptibility for the DFG process is found to have a value of chi <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">(2)</sup> ~4times10 <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">5</sup> pm/V.

Terahertz sources based on intracavity difference-frequency generation in mid-infrared quantum cascade lasers (THz DFG-QCLs) have recently emerged as the first monolithic electrically pumped semiconductor sources capable of operating at room temperature across the 1- to 6-THz range. Despite tremendous progress in power output, which now exceeds 1 mW in pulsed and 10 μW in continuous-wave regimes at room temperature, knowledge of the major figure of merits of these devices for high-precision spectroscopy, such as spectral purity and absolute frequency tunability, is still lacking. By exploiting a metrological grade system comprising a terahertz frequency comb synthesizer, we measure, for the first time, the free-running emission linewidth (LW), the tuning characteristics, and the absolute center frequency of individual emission lines of these sources with an uncertainty of 4 × 10-10. The unveiled emission LW (400 kHz at 1-ms integration time) indicates that DFG-QCLs are well suited to operate as local oscillators and to be used for a variety of metrological, spectroscopic, communication, and imaging applications that require narrow-LW THz sources.

We present the recent development of high performance compact THz sources based on intracavity nonlinear frequency mixing in mid-infrared quantum cascade lasers. Significant performance improvements of our THz sources with respect to the continuous wave THz power output, monolithic THz tuning, and widely frequency are achieved by systematic optimization of the device's active region, waveguide design, and chip bonding strategy. Room temperature continuous wave THz power of more than 10 μW at 3.4 THz is demonstrated at room temperature. Monolithic THz tuning of a chip-based THz source from 2.6 to 4.2 THz with power up to 0.1 mW is achieved. Surface emission from the substrate via a diffraction grating with THz power up to 0.5 mW is also obtained. The developing characteristics show the potential for these THz sources as local oscillators for many astronomical and medical applications.

Mid-infrared lasers, emitting in the spectral region of 3–12 μm that contains strong characteristic vibrational transitions of many important molecules, are highly desirable for spectroscopy sensing applications. High-efficiency quantum cascade lasers have been demonstrated with up to watt-level output power in the mid-infrared region. However, the wide wavelength tuning that is critical for spectroscopy applications still largely relies on incorporating external gratings, which have stability issues. Here, we demonstrate a monolithic, broadly tunable quantum cascade laser source emitting between 6.1 and 9.2 μm through an on-chip integration of a sampled grating distributed feedback tunable laser array and a beam combiner. High peak power up to 65 mW has been obtained through a balanced high-gain active region design, efficient waveguide layout, and the development of a broadband antireflection coating. Nearly fundamental transverse-mode operation is achieved for all emission wavelengths with a pointing stability better than 1.6 mrad (0.1°). The demonstrated laser source opens new opportunities for mid-infrared spectroscopy.

We demonstrate a compact, single-mode quantum cascade laser source continuously tunable over 8% of its center wavelength of 9 mum. We integrate the source into a compact mid-infrared spectrometer for absorption spectroscopy of liquids and gases.

We present a semi-automated point-of-care (POC) sensor approach for the simultaneous and reagent-free determination of clinically relevant parameters in blood plasma. The portable sensor system performed direct mid-infrared (MIR) transmission measurements of blood plasma samples using a broadly tunable external-cavity quantum cascade laser source with high spectral power density. This enabled the use of a flow cell with a long path length (165μm) which resulted in high signal-to-noise ratios and a rugged system, insensitive to clogging. Multivariate calibration models were built using well established Partial-Least-Squares (PLS) regression analysis. Selection of spectral pre-processing procedures was optimized by an automated evaluation algorithm. Several analytes, including glucose, lactate, triglycerides, cholesterol, total protein as well as albumin, were successfully quantified in routinely taken blood plasma samples from 67 critically ill patients. Although relying on a spectral range from 1030cm(-1) to 1230cm(-1), which is optimal for glucose and lactate but rather unusual for protein analysis, it was possible to selectively determine the albumin and total protein concentrations with sufficient accuracy for POC application.

Room-temperature, narrow-linewidth terahertz quantum cascade laser sources based on intracavity Cherenkov difference-frequency generation with emission at 3.5 THz, nearly 60µW power output, and conversion efficiency of approximately 0.55 mW/W2 are reported.

Mass spectrometry using matrix-assisted laser desorption/ionization (MALDI) technique is one of the most widely used method to analyze proteins in biological research fields. However, it is difficult to analyze insoluble proteins which have important roles in researches on disease mechanisms or in developments of drugs by using ultraviolet (UV) lasers which have commonly been used for MALDI. Recently, a significant improvement in MALDI process of insoluble proteins using a combination of a UV nitrogen laser and a tunable mid-infrared (MIR) free electron laser (FEL) was reported. Since the FEL is a very large and expensive equipment, we have developed a tabletop laser source which can generate both UV and tunable MIR lasers. A tunable MIR laser (5.5–10 µm) was obtained by difference frequency generation (DFG) between a Nd:YAG and a tunable Cr:forsterite lasers using two AgGaS 2 crystals. The MIR laser can generate pulses with an energy of up to 1.4 mJ at a repetition rate of 10 Hz. A UV laser was obtained by third harmonic generation of a Nd:YAG laser splitted from that used for DFG. A time interval between the UV and the MIR laser pulses can be adjusted with a variable optical delay. Keywords: difference frequency generation, tunable mid-infrared laser, third harmonic generation, mass spectrometry, matrix-assisted laser desorption/ionization

We discuss the design and operation of widely-tunable terahertz sources based on Cherenkov intra-cavity difference-frequency generation in mid-infrared quantum cascade lasers. Laser chips are integrated into a Littrow-type external cavity system. Devices demonstrate continuous terahertz emission tuning at room temperature with a record tuning range from 1.2 THz to 5.9 THz and peak power output varying between 5 and 90 μW, depending on the operating frequency. Beam steering of terahertz Cherenkov emission with frequency is suppressed and mid-infrared-to-terahertz conversion efficiency is improved by bonding devices onto high-resistivity silicon substrates that have virtually no refractive index dispersion and vanishingly-small optical loss in 1–6 THz range.

We report terahertz quantum cascade laser sources based on intra-cavity difference-frequency generation processed into double-metal waveguides with surface-grating outcouplers. Over 112 μW of peak power output is produced at room temperature at 1.9 THz.

A transportable prototype Faraday rotation spectroscopic system based on a tunable external cavity quantum cascade laser has been developed for ultrasensitive detection of nitric oxide (NO). A broadly tunable laser source allows targeting the optimum Q(3/2)(3/2) molecular transition at 1875.81 cm(-1) of the NO fundamental band. For an active optical path of 44 cm and 1-s lock-in time constant minimum NO detection limits (1sigma) of 4.3 parts per billion by volume (ppbv) and 0.38 ppbv are obtained by using a thermoelectrically cooled mercury-cadmium-telluride photodetector and liquid nitrogen-cooled indium-antimonide photodetector, respectively. Laboratory performance evaluation and results of continuous, unattended monitoring of atmospheric NO concentration levels are reported.

Broadly tunable hetero-cascading quantum cascade lasers: Design, growth, and external cavity operation

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.

Recently we investigated cascaded schemes for down-conversion to the mid-IR spectral range above 5 μm by implementing the second stage based on a non-oxide nonlinear crystal inside the cavity of a ns optical parametric oscillator (OPO) based on Rb:PPKTP, pumped by a Q-switched Nd:YAG laser [1-3]. Intracavity difference-frequency generation (DFG) [2, 3] turned out to be more efficient compared to intracavity pumped OPO [1], however wavelength tuning is restricted and a broadband dichroic half-wave plate is needed for either type-I or type-II phase-matching in the studied crystals of AgGaSe2 and BaGa4Se7. Low-symmetry cubic semiconductors, such as orientation-patterned GaAs offer greater variety of phase-matching configurations in which intracavity polarization rotation becomes redundant. With a similar spectral coverage of up to ∼18 μm and 2 to 3 times higher effective nonlinearity, OPGaAs exhibits 50 to 100 times higher thermal conductivity, better damage resistivity, and offers the unique possibility of convenient temperature tuning in both stages in non-critical configurations. These advantages point at possible extensions to much higher repetition rates (1–100 kHz). On one hand such low energy regimes will utilize perfectly the limited aperture of the presently available OPGaAs samples but on the other hand will enable the generation of unprecedented average powers in the mid-IR spectral range. In a first demonstration of such intracavity DFG we implement OPGaAs in the same Rb:PPKTP OPO operated at 100 Hz [1-3], using tighter focusing.