High Temperature Operating Narrow Period Terahertz Quantum Cascade Laser Designs

Presently, terahertz quantum cascade lasers still suffer from operations below room temperature, which prohibits extensive applications in terahertz spectra. The past continuous contributions to improving the operating temperatures were by clarifying the main thermal degradation process and proposing different designs with the optical gain demonstrating higher temperature cut-offs. Recent designs have attempted to employ a narrow period length with a simplified and clean state system, and reach renewed operating temperatures above 200 K. This study reveals how historic designs approach such narrow-period designs, discus the limitations within those designs, and show further possible designs for higher operating temperatures.

The portion of the electromagnetic spectrum between roughly 300 GHz and 10 THz is nicknamed the "THz Gap" because of the enormous difficulty encountered by researchers to devise practical sources covering it. Still, the quantum cascade laser (QCL) has emerged over recent years as the most promising approach to a practical source in the 1-5 THz range. First developed in the higher-frequency mid-IR, where they are now widely available, QCLs were later extended to the THz where a host of greater design challenges awaited. Lasing in QCLs is based on intersubband optical transitions in semiconductor quantum wells, the energy of which can be chosen by design ("bandstructure engineering"). However, simply building a THz optical transition is insufficient; a good design must also produce significant population inversion by the applied cascading electron current, and this requires deep understanding of the transport physics. So far, no THz QCL has operated above the temperature of 200 K, even though the reasons prohibiting high temperature operation are well known. The goal of this Thesis is to put novel ideas for high-temperature operation of THz QCL active regions through rigorous theoretical testing. The central enabling development is a density-matrix-based model of transport and optical properties tailored for use in QCLs, which is general enough that widely varying design concepts can be tested using the same core principles. Importantly, by simulating QCLs more generally, fewer a priori assumptions are required on part of the researcher, allowing for the true physics to emerge on its own. It will be shown that this gives rise to new and useful insights that will help to guide the experimental efforts towards realization of these devices. One specific application is a quantum dot cascade laser (QDCL), a highly ambitious approach in which the electrons cascade through a series of quantum dots rather than wells. Benefits are expected due to the suppression of nonradiative scattering, brought about by the discrete spectrum of electronic states. However, this in turn leads to a highly different physics of transport and effects that are not well understood, even in the case of perfect materials. This work will show that while the benefits are clear, naive scaling of existing QCL designs to the quantum dot limit will not work. An alternative strategy is given based on a revised understanding of the nature of transport, and is put to a test of practicality in which the effects of quantum dot size inhomogeneity are estimated. Another application is to the already existing method of THz difference frequency generation in mid-IR QCLs, which occurs via a difference-frequency susceptibility $\chi^{(2)}$ in the active region itself. For this purpose, the model is extended to enable a coherent and nonperturbative calculation of optical nonlinearities. First, the generality of the method is displayed through the emergence of exotic nonlinear effects, including electromagnetically-induced transparency, in mock quantum-well systems. Then, the modeling concepts are applied to the real devices, where two new and important mechanisms contributing to $\chi^{(2)}$ are identified. Most importantly, it is predicted that the QCL acts as an extremely fast photodetector of itself, giving rise to a current response to the mid-IR beatnote that provides a better path forward to the generation of frequencies below ~2 THz. Finally, the fundamentals of density matrix transport theory for QCLs are revisited to develop a model for conventional THz QCL designs eliminating the usual phenomenological treatment of scattering. The new theory is fully developed from first principles, and in particular sheds light on the effects of scattering-induced electron localization. The versatility of the model is demonstrated by successful simulation of varying active region designs.

Terahertz Quantum Cascade Lasers (THz QCLs) are arguably the most promising technology today for the compact, efficient generation of THz radiation. Their main limitation is that they require cryogenic cooling, which dominates their ownership cost. Therefore, achieving room-temperature operation is essential for the widespread adoption of THz QCLs. This thesis analyzes the limitations of THz QCL maximum lasing temperature (Tmax) and proposes solutions. THz QCL Tmax is hypothesized to be limited by a fundamental trade-off between gain oscillator strength ful and upper-level lifetime [Tau]. This so-called "ful[Tau] tradeoff" is shown to explain the failure of designs which target [Tau] alone. A solution is proposed in the form of highly diagonal (low ful) active region design coupled with increased doping. Experimental results indicate the strategy to be promising, but heavily doped designs are shown to suffer band-bending effects which may deteriorate performance. In order to treat these band-bending effects, which are typically neglected in previous THz QCL designs, a fast transport simulation tool is developed. Scattering integrals are simplified using the assumption of thermalized sub bands. Results comparable to ensemble Monte Carlo are achieved at a fraction of the computational expense. Carrier leakages to continuum states are also investigated, although they are found to have little effect. Other work in this thesis includes the optimization of double-metal THz waveguides to enable Tmax ~ 200 K, a current world record. Furthermore, laser designs to investigate the leakages of carriers to high-energy subbands and continuum states were fabricated and tested; such parasitic leakages are suggested to be small. Finally, the design of gain media for applications is examined, notably the development of 4.7 THz gain media for OI line detection in astrophysics, and the development of broadband heterogeneous gain media for THz comb generation.

Learn how the rapidly expanding area of mid-infrared and terahertz photonics has been revolutionized in this comprehensive overview. State-of-the-art practical applications are supported by real-life examples and expert guidance. Also featuring fundamental theory enabling you to improve performance of both existing and future devices.

The terahertz or the far-infrared frequency range of the electromagnetic spectrum (...) has historically been technologically underdeveloped despite having many potential applications, primarily due to lack of suitable sources of coherent radiation. Following on the remarkable development of mid-infrared (...) quantum-cascade lasers (QCLs) in the past decade, this thesis describes the development of electrically-pumped terahertz quantum-cascade lasers in GaAs/AlsGal_. As heterostructures that span a spectral range of 1.59 - 5.0 THz (...). A quantum-cascade laser (QCL) emits photons due to electronic intersubband transitions in the quantum-wells of a semiconductor heterostructure. The operation of terahertz QCLs at frequencies below the Reststrahlen band in the semiconductor (...), is significantly more challenging as compared to that of the mid-infrared QCLs. Firstly, due to small energy separation between the laser levels various intersubband scattering mechanisms are activated, which make it difficult to selectively depopulate the lower laser level. Additionally, as electrons gain enough kinetic energy in the upper laser level thermally activated longitudinal-optical (LO) phonon scattering reduces the level lifetime and makes it difficult to sustain population inversion at higher temperatures. Secondly, waveguide design for terahertz mode confinement is also more challenging due to higher free-carrier losses in the semiconducting doped regions at the terahertz frequencies. For successful designs reported in this work, the lower radiative state depopulation is achieved by a combination of resonant-tunneling and fast LO phonon scattering, which allow robust operation even at relatively high temperatures. An equally important enabling mechanism for these lasers is the development of metal-metal waveguides, which provide low waveguides losses, and strong mode confinement due to subwavelength mode localization in the vertical dimension. With these techniques some record performances for terahertz QCLs are demonstrated including the highest pulsed operating temperature of 169 K, the highest continuous-wave (cw) operating temperature of 117 K, and the highest optical power output (248 mW in pulsed and 138 mW in cw at 5 K) for any terahertz QCL. Towards the bigger goal of realizing a 1-THz solid-state laser to ultimately bridge the gap between electronic and optical sources of electromagnetic radiation, QCLs with a unique one-well injection scheme, which minimizes intersubband absorption losses that occur at longer wavelengths, are developed. Based on this scheme a QCL operating at 1.59 THz (A - 189 ym) is realized, which is amongst the lowest frequency solid-state lasers that operate without the assistance of a magnetic field. This thesis also reports on the development of distributed-feedback lasers in metal-metal waveguides to obtain single-mode operation, with greater output power and better beam quality. The subwavelength vertical dimension in these waveguides leads to a strongly coupled DFB action and a large reflection from the end-facets, and thus conventional coupled-mode theory is not directly applicable to the DFB design. A design technique with precise control of phase of reflection at the end-facets is developed with the aid of finite-element analysis, and with some additional unique design and fabrication methods, robust DFB operation has been obtained. Single-mode surface-emitting terahertz QCLs operating up to - 150 K are demonstrated, with different grating devices spanning a range of approximately 0.35 THz around v - 3 THz using the same gain medium. A single-lobed far-field radiation pattern, higher output power due to surface-emission, and a relatively small degradation in temperature performance compared to the Fabry-Perot ridge lasers makes these DFB lasers well suited for practical applications that are being targeted by the terahertz quantum-cascade lasers.

Quantum cascade laser (QCL), as a unipolar semiconductor laser based on intersubband transitions in quantum wells, covers a large portion of the Mid and Far Infrared electromagnetic spectrum. The frequency of the optical transition can be determined by engineering the layer sequence of the heterostructure. The focus of this work is on Terahertz (THz) frequency range (frequency of 1 - 10 THz and photon energy of ~ 4 - 40 meV), which is lacking of high power, coherent, and efficient narrowband radiation sources. THz QCL, demonstrated in 2002, as a perfect candidate of coherent THz source, is still suffering from the empirical operating temperature limiting factor of T [ap] h̳[omega]/kB, which allows this source to work only under a cryogenic system. Most of high performance THz QCLs, including the world record design which lased up to ~ 200 K, are based on a resonant phonon (RP) scheme, whose population inversion is always less than 50%. The indirectly-pumped (IDP) QCL, nicely implemented in MIR frequency, starts to be a good candidate to overcome the aforementioned limiting factor of RP-QCL. A rate equation (RE) formalism, which includes both coherent and incoherent transport process, will be introduced to model the carrier transport of all presented structures in this thesis. The second order tunneling which employed the intrasubband roughness and impurity scattering, was implemented in our model to nicely predict the behavior of the QCL designs. This model, which is easy to implement and fast to calculate, could help us to engineer the electron wavefunctions of the structure with optimization tools. We developed a new design scheme which employs the phonon scattering mechanism for both injecting carrier to the upper lasing state and extracting carrier from lower lasing state. Since there is no injection/extraction state to be in resonance with lasing states, this simple design scheme does not suffer from broadening due to the tunneling. Finally, three different THz IDP-QCLs, based on phonon-photon-phonon (3P) scheme were designed, grown, fabricated, and characterized. The performance of those structures in terms of operating temperature, threshold current density, maximum current density, output optical power, lasing frequency, differential resistance at threshold, intermediate resonant current before threshold, and kBT/h̳[omega] factor will be compared. We could improve the kBT/h̳[omega] factor of the 3P-QCL design from 0.9 in first iteration to 1.3 and the output optical power of the structure from 0.9 mW in first design to 3.4 mW. The performance of the structure in terms of intermediate resonant current and the change in differential resistance at threshold was improved.

Quantum cascade lasers (QCLs) are attractive for high-resolution spectroscopy because they can provide high power and a narrow linewidth. They are particularly promising in the terahertz (THz) range since they can be used as local oscillators for heterodyne detection as well as transmitters for direct detection. However, THz QCL-based technologies are still under development and are limited by the lack of frequency tunability as well as the frequency and output power stability for free-running operation. In this dissertation, frequency tuning and linewidth of THz QCLs are studied in detail by using rotational spectroscopic features of molecular species. In molecular spectroscopy, the Doppler eff ect broadens the spectral lines of molecules in the gas phase at thermal equilibrium. Saturated absorption spectroscopy has been performed that allows for sub-Doppler resolution of the spectral features. One possible application is QCL frequency stabilization based on the Lamb dip. Since the tunability of the emission frequency is an essential requirement to use THz QCL for high-resolution spectroscopy, a new method has been developed that relies on near-infrared (NIR) optical excitation of the QCL rear-facet. A wide tuning range has been achieved by using this approach. The scheme is straightforward to implement, and the approach can be readily applied to a large class of THz QCLs. The frequency and output stability of the local oscillator has a direct impact on the performance and consistency of the heterodyne spectroscopy. A technique has been developed for a simultaneous stabilization of the frequency and output power by taking advantage of the frequency and power regulation by NIR excitation. The results presented in this thesis will enable the routine use of THz QCLs for spectroscopic applications in the near future.

(cont.) The challenges posed by the long THz wavelengths in QCL waveguide design leads to a tradeoff between high temperature operation (

Terahertz (THz) quantum-cascade lasers (QCLs) are an emerging semiconductor source of compact, high-power THz radiation. Though first realized more than 15 years ago, THz QCLs continue to suffer from poor beam quality and outcoupling efficiency due to the subwavelength nature of the semiconductor ridge-waveguides typically used. In this thesis, a new technique is discussed for obtaining high power and good beam quality from THz QCLs, the THz quantum-cascade external cavity surface emitting laser (QC-VECSEL). The concept of the QC-VECSEL is to use THz QC-gain material to design a millimeter-scale reflective amplifying surface, or metasurface, for free space THz waves and incorporate it into a free-space THz resonant cavity to provide feedback to the amplification and form a laser. In this manner, the beam shape is determined by the external cavity, which supports fundamental Gaussian solutions. Further, the metasurface itself is composed of a subwavelength array (to prevent diffraction) of surface-coupled QC-elements whose properties, such as phase and polarization response, can be engineered on a unit cell basis allowing for a variety of unique experiments. The power output power of the QC-VECSEL can be scaled by either increasing the size of the metasurface, or increasing the density (or fill factor) of QC-elements across the surface. In this work, large area metasurfaces with high fill-factor have been studied and demonstrated up to 1.35 W of peak output power for a QC-VECSEL operating at 3.4 THz at a heat sink temperature of 4 K. A peak wall-plug efficiency of ~2% is demonstrated, but observation of self lasing from the metasurface at high bias (when no external cavity is provided) in combination with a simultaneous roll-off in VECSEL output power suggests even higher efficiency can be achieved with improved suppression of self-lasing modes. The output beam is well fit to a Gaussian distribution with a 4 degree full-width half-maximum divergence angle. In addition to power and beam quality, the QC-VECSEL opens the door to many interesting and unique studies via engineering of the metasurface properties and external cavity. Much of this thesis describes frequency tuning of QC-VECSELs based on broadband metasurfaces by varying the length of the external cavity. By making the external cavity extremely short (comparable to the operating wavelength), we are able to push all other external cavity modes outside of the gain bandwidth of the metasurface and demonstrate more than 20% fractional single-mode tuning around a center operating frequency of 3.5 THz. Because there are almost no diffraction losses at such a short cavity, the size of the metasurface could be reduced, allowing for continuous wave lasing with up to 20 milliwatts of output power at a heatsink temperature of 77 K, though the output power is highly variable as the reflectance of the output coupler has a strong frequency dependence. At the time of writing this, these are record performances in both frequency tuning and high-temperature continuous wave operation for lasers based on THz QC-gain material. The amount of tuning that be achieved with this approach is limited by the phase response of the metasurface, which squeezes the external cavity modes closer together in the spectral domain. Development of metasurfaces with lower electrical power consumption and higher conversion efficiency for the purpose of improving continuous wave performance. A sparse, patch-based metasurface with reduced power consumption is demonstrated, though the design was not optimal and only showed a 20% reduction in current draw compared to the previously demonstrated metasurfaces. Routes towards improving the performance are discussed. The last subject discussed is the design of a mid-infrared (IR) QC-VECSEL. Due to the large metal losses at mid-IR frequencies compared to THz, the technique used to develop THz QC-VECSELs cannot be directly extended to the mid-IR. We propose a scheme based on a diffraction grating to provide surface coupling of the QC-gain material. Progress on experimental realization is discussed, but lasing has not yet been observed.

Recent advances in Terahertz Quantum Cascade Laser (THz QCL) development are pushing this technology ever closer to practical application, particularly within the spectroscopic field. For this reason, optimizing the operation of THz QCL frequency combs, which can potentially provide unprecedented accuracy and stability to the optical spectra in a broad frequency band, is of particular interest to the research community. The THz QCLs frequency comb was only recently realized using two separate techniques: either a broad-gain active region or a group velocity dispersion controlled waveguide. However, due to residual optical dispersion from both the gain medium and the cold waveguide, comb formation in these reported THz QCLs can only sustain a limited current injection region and the observed comb frequency range is much narrower than the bandwidth of the designed gain medium. To overcome these limitations, this thesis targets a new THz QCL frequency comb device design that simultaneously exploits the broadband gain active region and a group velocity dispersion (GVD)-compensated waveguide over an octave frequency band of 2-4 THz. In designing a broadband gain active region, two heterogeneous structures are proposed and simulated, with one combining three different bound-to-continuum (BTC) active regions operating at a temperature of 25 K, and another one consisting of four different resonant-phonon (RP) active regions operating at the liquid nitrogen temperature (77 K) or higher. The simulation results show that both active region designs can provide a broadband and 'flat-top' gain profile covering the frequency range from 2 to 4 THz. To design a group velocity dispersion-compensated waveguide, strategies are explored for simulating chirped Distributed Bragg Reflectors (DBRs) that can serve as THz QCL metal-metal waveguides, and one-dimensional (1D) and three-dimensional (3D) modeling approaches are established and verified. A novel two-section chirped DBR is proposed, which provides substantially-improved group delay compensation over a broadband octave frequency range from 2 to 4 THz. Two THz QCL structures are grown using in-house molecular beam epitaxy and THz QCL devices equipped with a metal-metal waveguides are fabricated in the University of Waterloo Quantum-Nano-Centre clean-room fabrication lab. The experimental results demonstrate that the new THz QCL active region design can operate up to a maximum lasing temperature of 111 K, and with a broad lasing spectrum covering frequencies from 2.36 to 2.86 THz under pulse mode, at temperature of 13 K. The combined theoretical and experimental work would ultimately lead to the demonstration of improved THz QCL frequency comb operation over the broadband range from 2 to 4 THz.