Intensity Correlations in Quantum Cascade Laser Harmonic Frequency Combs

Optical frequency comb synthesizers, operating in the harmonic regime, are metrological sources in which the emitted optical power is concentrated in a few modes, spaced by several multiples of the cavity free spectral range (FSR). This behavior reflects in a large correlation degree and, in principle, in an increased optical power per mode. In miniaturized quantum cascade lasers (QCLs), harmonic frequency combs (HFCs) are hence particularly attracting to explore quantum correlation effects between adjacent harmonic modes, enabled by the inherently large gain media third-order χ (3) Kerr nonlinearity, even if controlled generation of stable HFCs of predefined order, is typically demanding in such electrically pumped sources. Here, we demonstrate stable2nd order and 3rd order HFC emission in terahertz frequency QCLs by respectively patterning an individual or a couple of equally spaced distributed multilayer graphene absorbers on the top metallic waveguides.

Quantum cascade laser (QCL) harmonic state frequency combs (HFCs) have recently attracted considerable interest for applications ranging from the generation of tones of high spectral purity, high data rate wireless communication networks, radiofrequency arbitrary waveform synthesis, and for fundamental light-matter investigations in quantum physics. However, a detailed knowledge of the nature of the electronic and thermal energy distribution in these devices is of paramount importance for the refinement of their thermal management and quantum efficiency, which are key to the widespread adoption of QCL HFC technology in a new generation of integrated optical quantum platforms. Here, we perform a comparative study of the thermal and electronic properties of Fabry–Perot and micro-ring HFC QCLs, operating in the terahertz frequency range, using micro-probe band-to-band photoluminescence. By monitoring the lattice temperature and the electron cooling above the threshold for stimulated emission, we extract the device thermal resistances and the internal quantum efficiencies, highlighting the key role of the resonator architecture.

Quantum cascade (QC) lasers opens new prospects for powerful sources operating at THz frequencies. Up to now the best THz QC lasers are based on intersubband emission in GaAs/AlGaAs quantum well (QW) heterostructures. The maximum operating temperature is 200 K, which is too low for wide-spread applications. This is due to the rather low LO-phonon energy (36 meV) of GaAs-based materials. Indeed, thermal activation allows non-radiative path through electron-phonon interaction which destroys the population inversion. Wide band gap materials such as ZnO have been predicted to provide much higher operating temperatures because of the high value of their LO-phonon energy. However, despite some observations of intersubband absorption in c-plane ZnO/ZnMgO quantum wells, little is known on the fundamental parameters such as the conduction band offset in such heterostructures. In addition the internal field inherent to c-plane grown heterostuctures is an handicap for the design of QC lasers and detectors. In this talk, we will review a systematic investigation of ZnO/ZnMgO QW heterostructures with various Mg content and QW thicknesses grown by plasma molecular beam epitaxy on low-defect m-plane ZnO substrates. We will show that most samples exhibit TM-polarized intersubband absorption at room temperature linked either to bound-to-quasi bound inter-miniband absorption or to bound-to bound intersubband absorption depending on the Mg content of the barrier material. This systematic study allows for the first time to estimate the conduction band offset of ZnO/ZnMgO heterostructures, opening prospects for the design of QC devices operating at THz frequencies. This was supported by the European Union’s Horizon 2020 research and innovation programme under grant agreement #665107.

Terahertz quantum cascade lasers (QCLs) with a broadband gain medium could play an important role for sensing and spectroscopy since then distributed-feedback schemes could be utilized to produce laser arrays on a single semiconductor chip with wide spectral coverage. QCLs can be designed to emit at two different frequencies when biased with opposing electrical polarities. Here, terahertz QCLs with bidirectional operation are developed to achieve broadband lasing from the same semiconductor chip. A three-well design scheme with shallow-well GaAs/Al0.10Ga0.90As superlattices is developed to achieve high-temperature operation for bidirectional QCLs. It is shown that shallow-well heterostructures lead to optimal quantum-transport in the superlattice for bidirectional operation compared to the prevalent GaAs/Al0.15Ga0.85As material system. Broadband lasing in the frequency range of 3.1–3.7 THz is demonstrated for one QCL design, which achieves maximum operating temperatures of 147 K and 128 K respectively in opposing polarities. Dual-color lasing with large frequency separation is demonstrated for a second QCL, that emits at ~3.7 THz and operates up to 121 K in one polarity, and at ~2.7 THz up to 105 K in the opposing polarity. These are the highest operating temperatures achieved for broadband terahertz QCLs at the respective emission frequencies, and could lead to commercial development of broadband terahertz laser arrays.

The design and operation of quantum cascade (QC) lasers using AlAs/GaAs coupled quantum wells are reported. In this material system, the conduction band offset at the Γ point (∼1 eV) is much higher than in previously reported QC lasers. The use of high band discontinuity allows us to increase the energy separation among the subbands, thus suppressing thermally activated processes which limit device performance at high temperature. The measured thermal characteristics of these promising devices are strongly improved from previously reported GaAs-based QC lasers: The temperature dependence of the threshold current density is described by a very large T0 (320 K) and the laser slope efficiency does not vary for increasing heat sink temperatures. The maximum operating temperature is 230 K, limited by negative differential resistance effects that occur when the applied bias reaches 8 V.

We propose and study the feasibility of a THz GaN/AlGaN quantum cascade laser (QCL) consisting of only five periods with confinement provided by a spoof surface plasmon (SSP) waveguide for room temperature operation. The QCL design takes advantages of the large optical phonon energy and the ultrafast phonon scattering in GaN that allow for engineering favorable laser state lifetimes, and the SSP waveguide provides the optical confinement for the ultrathin QCL. Our analysis has shown that the waveguide loss is sufficiently low for the QCL to reach its threshold at the injection current density around 6 kA/cm2 at room temperature.

Recently, a novel type of molecular THz laser with ∼mW-level output power was demonstrated [1,2]. This laser is optically pumped by a mid-IR Quantum Cascade Laser (QCL), therefore resulting in a much more compact, frequency agile and deployable source compared to standard, CO 2 -laser pumped, far-infrared gas lasers. This achievement has revived the interest for molecular THz lasers, in particular for their exploitation as low-phase noise THz local oscillators (LOs) operating at room temperature. Compared to CO 2 -laser pumping, a QCL pump offers an unrivalled frequency agility that allows accessing an unprecedented number of molecular transitions. On the other hand, its lower frequency stability can potentially impact the frequency noise of the THz laser source [3–5]. Here we report the first measurement of the frequency noise power spectral density (PSD) of a 1.073THz ammonia laser pumped by a 10.3μm QCL. This is achieved by using a commercial harmonic mixer to generate a beating between the ammonia laser frequency and the 1080th harmonic of the 1GHz repetition rate of a custom-made, 1560nm frequency comb (FC). We then exploit a voltage-controlled oscillator to track the beat-note signal and realize the frequency to amplitude conversion [6]. The measured frequency noise PSD is shown in Fig.1. In the range ∼30–100kHz we find a frequency noise 2 -pumped, 2.5THz methanol laser, reaching 0.1Hz2/Hz (−110dBc) at 40kHz from the carrier, limited by the frequency noise of the FC harmonic. Finally, we will show that it is possible to actively phase-lock the QCL-pumped ammonia laser to the FC repetition rate harmonic by controlling the QCL drive current, demonstrating a sub-Hz linewidth. These results pave the way to the development of QCL-pumped molecular lasers as compact, low-phase noise THz sources operating a room temperature.

Stable operation is one of the most important requirements for a laser source for high-precision applications. Many efforts have been made to improve the stability of lasers by employing various techniques, e.g., electrical and/or optical injection and phase locking. However, these techniques normally involve complex experimental facilities. Therefore, an easy implementation of the stability evaluation of a laser is still challenging, especially for lasers emitting in the terahertz (THz) frequency range because the broadband photodetectors and mature locking techniques are limited. In this work, we propose a simple method, i.e., relative phase locking, to quickly evaluate the stability of THz lasers without a need of a THz local oscillator. The THz laser system consists of a THz quantum cascade laser (QCL) frequency comb and a single-mode QCL. Using the single-mode laser as a fast detector, heterodyne signals resulting from the beating between the single-mode laser and the comb laser are obtained. One of the heterodyne beating signals is selected and sent to a phase-locked loop (PLL) for implementing the relative phase locking. Two kinds of locks are performed by feeding the output error signal of the PLL, either to the comb laser or to the single-mode laser. By analyzing the current change and the corresponding frequency change of the PLL-controlled QCL in each phase-locking condition, we, in principle, are able to experimentally compare the stability of the emission frequency of the single-mode QCL (fs) and the carrier envelope offset frequency (fCEO) of the QCL comb. The experimental results reveal that the QCL comb with the repetition frequency injection locked demonstrates much higher stability than the single-mode laser. The work provides a simple heterodyne scheme for understanding the stability of THz lasers, which paves the way for the further locking of the lasers and their high-precision applications in the THz frequency range.

Optical frequency combs, consisting of well‐controlled equidistant frequency lines, have been widely used in precision spectroscopy and metrology. Terahertz combs have been realized in quantum cascade lasers (QCLs) by employing either an active mode‐locking or phase seeding technique, or a dispersion compensator mirror. However, it remains a challenge to achieve the passive comb formation in terahertz semiconductor lasers due to the insufficient nonlinearities of conventional saturable absorbers. Here, a passive terahertz frequency comb is demonstrated by coupling a multilayer graphene sample into a QCL compound cavity. The terahertz modes are self‐stabilized with intermode beat note linewidths down to a record of 700 Hz and the comb operation of graphene‐coupled QCLs is validated by on‐chip dual‐comb measurements. Furthermore, the optical pulse emitted from the graphene‐coupled QCL is directly measured employing a terahertz pump–probe technique. The enhanced passive frequency comb operation is attributed to the saturable absorption behavior of the graphene‐integrated saturable absorber mirror, as well as the dispersion compensation introduced by the graphene sample. The results provide a conceptually different graphene‐based approach for passive comb formation in terahertz QCLs, opening up intriguing opportunities for fast and high‐precision terahertz spectroscopy and nonlinear photonics.

Coupling of broadband terahertz pulses into metal-metal terahertz quantum cascade lasers is presented. Mode matched terahertz transients are generated on the quantum cascade laser facet of subwavelength dimension. This method provides a full overlap of optical mode and active laser medium. A longitudinal optical-phonon depletion based active region design is investigated in a coupled cavity configuration. Modulation experiments reveal spectral gain and (broadband) losses. The observed gain shows high dynamic behavior when switching from loss to gain around threshold and is clamped at total laser losses.

Frequency combs, spectra of phase-coherent equidistant lines, have revolutionized time and frequency metrology. The recently developed quantum cascade laser (QCL) comb has exhibits great potential with high power and broadband spectrum. However, in the terahertz (THz) range, cryogenic cooling has to be applied for THz QCL combs. We report a room temperature THz frequency comb at 3.0 THz based on difference-frequency generation from a mid-IR QCL comb. A largely detuned distributed-feedback grating is integrated into the QCL cavity to provide the single mode operation as well as enhanced spatial hole-burning effect for multimode comb operation. Multiheterodyne spectroscopy with multiple equally spaced lines by beating it with a reference Fabry-Pérot comb confirms the THz comb operation. This type of THz comb provides a new solution to chip-based high-speed high-resolution THz spectroscopy with compact size at room temperature.

We report a homogeneous quantum cascade laser (QCL) emitting at terahertz (THz) frequencies, with a total spectral emission of about 0.6 THz, centered around 3.3 THz, a current density dynamic range Jdr = 1.53, and a continuous wave output power of 7 mW. The analysis of the intermode beatnote unveils that the devised laser operates as an optical frequency comb (FC) synthesizer over the whole laser operational regime, with up to 36 optically active laser modes delivering ∼200 µW of optical power per optical mode, a power level unreached so far in any THz QCL FC. A stable and narrow single beatnote, reaching a minimum linewidth of about 500 Hz, is observed over a current density range of 240 A/cm2 and even across the negative differential resistance region. We further prove that the QCL FC can be injection locked with moderate radio frequency power at the intermode beatnote frequency, covering a locking range of 1.2 MHz. The demonstration of stable FC operation, in a QCL, over the full current density dynamic range, and without any external dispersion compensation mechanism, makes our proposed homogenous THz QCL an ideal tool for metrological applications requiring mode-hop electrical tunability and a tight control of the frequency and phase jitter.

We design the InxGa1-xAs/InyAl1-yAs quantum cascade laser (QCL) structures, based on the four-quantum well active region with vertical transition with strain compensation towards the shorter wavelengths, operating at λ ~2.93–6.6μm. Considering the objective function related to the optical gain, i.e., \({z_{43}^2 (1-\tau_3 /\tau_{43})\tau_4}\), and the escape energy related to the carrier leakage to continuum, the design of QCLs is carried out in double infinite feedback loops. Each barrier/well layer in the active region is optimized towards the lasing wavelength as short as possible under a properly designed injector. For efficient short wavelength emission, the larger conduction band discontinuity (ΔEc) is achieved by changing the indium mole fractions of strain-compensated InxGa1-xAs/InyAl1-yAs layers. The experimentally verified injectors are properly modified for the stronger coupling between the wavefunctions of the ground state in injector and the upper state in active region. Thus the use of strain-compensated In0.72Ga0.28As/In0.3Al0.7As structure (i.e., ΔEc = 857 meV) leads to the shortest wavelength up to λ ~2.93μm with τ43 = 2.13 ps, τ4 = 0.87 ps, τ3 = 1.43 ps and z43 = 1.03 nm under an electric field of 96 kV/cm.

A continuous-wave Fabry–Pérot quantum cascade laser (QCL) emitting at 8.1 μm operating in the single mode regime has been coherently phase locked to a turn-key low-noise commercial mid-Infrared (mid-IR) optical frequency comb. The stability of the comb used as a reference is transferred to the QCL resulting in an integrated residual phase error of 0.4 rad. The laser linewidth is narrowed by more than two orders of magnitude reaching sub-kHz level at 1 ms observation time, limited by the spectral purity of the mid-IR comb. Our experiment is an important step toward the development of both powerful and metrology-grade QCLs and fully stabilized QCL frequency comb and opens perspectives for precision measurements and frequency metrology in the mid-IR.

Recent decade brought a tremendous progress laser-based gas detection techniques. This progress would not be possible without the relentless devotion of the scientific community in developing state-of-the-art sources capable of targeting strong absorption lines of gases localized in the mid-infrared (mid-IR) wavelength region. Although narrowband, semiconductor-based mid-IR lasers offer non-complex implementation their tuning range is usually limited to several cm−1. Therefore designing a sensor capable of simultaneous monitoring of several gas species, even with absorption profiles clustered nearby, requires incorporating individual expensive quantum cascade laser (QCL) or interband cascade laser (ICL) sources into a single platform. Recent development of reliable mid-IR comb sources, combined with clever methods of signal processing allowed for designing gas sensors capable of simultaneous monitoring of several gas analytes in fractions of a second [1]. Obtaining broadband pulsed radiation in the mid-IR region is usually accomplished by utilizing nonlinear conversion or in recently presented on-chip QCL combs [2]. Although QCL combs offer compactness and efficiency they do not allow straightforward control of the repetition frequency (f rep ) or the carrier-envelope offset frequency (f CEo ), which are critical in some particular cavity-enhanced comb-based sensing techniques, e.g. Vernier spectroscopy [3]. Here we present a fully-fiberized, f CEO -free mid-IR optical frequency comb source capable of covering 6–9 μm wavelength region with tunable f rep . The setup of the source is presented in Fig 1. The heart of the source is a ring-cavity graphene mode-locked laser generating sub-250 fs pulses at 1560 nm and f rep of 100 MHz. The pulses are split using a 50/50 coupler and directed to separate sections of the source. In the blue section the source the pulses are amplified to 80 mW in an all-fiber-based chirped pulse amplifier (CPA) and recompressed in a 8 m-long section of PM1550 fiber to ∼200 fs. In the red section a custom manufactured nonlinear fiber with tailored dispersion (PCF) is utilized to soliton-shift the 1.55 μm pulses into the 1.9–2 μm wavelength region. Subsequently the pulses are amplified in a CPA and recompressed to ∼200 fs. Combined 1.55 and 2 μm pulses are focused on a 3 mm-long orientation patterned gallium phosphide (OP-GaP) crystal to generate mid-IR radiation via differential frequency generation (DFG). Since both pulses originated from the same ML source, the generated mid-IR frequency comb is inherently fceo-free and can be used in laser-based gas sensors requiring stable carrier-envelope offset. The source is built entirely from PM single-mode fibers.