Quantum Cascade Laser Frequency Combs Research Articles

Dual‐Comb Interferometry for Coherence Analysis of Tightly Locked Mid‐Infrared Quantum Cascade Laser Frequency Combs

Frequency combs are powerful tools for many applications and high performances are achieved by stabilizing these lasers. For operation in the mid‐infrared, quantum cascade lasers (QCL) are ideal candidates as they present numerous advantages. However, stabilized QCL‐combs lack a detailed characterization of their noise properties due to the sensitivity limits of current analyzing techniques. To overcome these challenges, what is believed to be the first tightly locked dual QCL‐comb system is developed. Its use is twofold. First, phase noise analysis of the dual‐comb signal shows residual phase noise below 600 mrad for all comb lines, and the comb coherence as well as the performances of the repetition frequency locking mechanism is characterized. Second, coherent averaging with a 7 × 105 Hz1/2 figure‐of‐merit system is demonstrated, which is compatible with high‐precision spectroscopy.

Mid-infrared dual-comb spectroscopy with quantum cascade lasers

Since its invention in 1994, the quantum cascade laser (QCL) has emerged as a versatile light source of wavelength 4–12 µm, covering most of the mid- and long-wavelength infrared spectral ranges. Its application range has widened even further since frequency comb operation and its use as a light source for dual-comb spectroscopy (DCS) was demonstrated. In this tutorial, we introduce the unique properties of QCL frequency combs, such as high optical power, multi-GHz repetition rate, and narrow optical linewidths. Implemented in a dual-comb spectroscopy setup, this allows for broadband, low-noise measurements of strongly absorbing samples with sub-microsecond time resolution, and spectral resolution better than 10−3 cm−1/30 MHz. The advantages of QCL DCS will be discussed in the context of its broad range of applications. The high optical power (both total and per comb tooth) is leveraged for measurements in aqueous solution or at large stand-off distances. Microsecond temporal resolution measurements address the demand for probing rapid protein dynamics and combustion diagnostics. MHz-level spectral resolution, in turn, facilitates accurate line parameter studies in low pressure and cold molecular gases. Future development directions of the technology are discussed, including sub-microsecond response DCS, instrument miniaturization, or its expansion toward THz frequencies. Overall, the tutorial aims at giving a broad introduction to QCL DCS and its applications.

Terahertz quantum cascade laser frequency combs with engineered operation frequency around 4.0 THz

Freely engineering the operation frequency of frequency comb sources is crucial for various applications, e.g., high-precision spectroscopy, ranging, communications, and so on. Here, by employing band structure simulations, group velocity dispersion (GVD) analysis, and experimental verifications, we demonstrate that the operation frequency of terahertz (THz) quantum cascade laser frequency combs can be engineered from 4.2 to 4.0 THz. First of all, from the viewpoint of the band structure engineering, we shift the frequency corresponding to the optical transitions in the active region from 4.2 to 4.0 THz by slightly altering the thicknesses of quantum wells. Meanwhile, a GVD analysis is applied to evaluate the potential comb performance. Finally, experimental characterizations, e.g., emission spectra, inter-mode beatnote, dual-comb operation, are performed to validate the exceptional comb operation at 4.0 THz. The advancement in simulations and experimental results present a comprehensive method to customize the desired THz radiative frequency for comb generation, which facilitates the practical development of broadband, high-precision THz comb sources.

Controlled generation of harmonic states in mid-infrared quantum cascade laser frequency combs by external cavity optical feedback.

We demonstrate the implementation of external cavity optical feedback to improve coherence and promote generation of harmonic states by a mid-infrared quantum cascade laser frequency comb. In particular, we present a Vernier-like scheme to realize harmonic comb states that increase the repetition rate of the comb by a factor of up to 6 and broaden spectral coverages from 46 cm-1 to 92 cm-1. Intermode beatnote and dual comb characterization indicate that the coherence of the comb has greatly improved for sub-optimal devices when the comb is operated in these harmonic states. This approach to control the generation of harmonic states and improve comb performance can be readily incorporated to various sensing systems and has great potential in spectroscopic measurements that require high repetition rates and/or broad optical bandwidth.

Anti-correlation phenomena in quantum cascade laser frequency combs

In quantum cascade laser frequency combs, the intensity distribution of the optical spectrum can be split into two well-separated lobes of longitudinal modes that, even when far apart, have a common phase relation and preserve equal frequency separation. The temporal dynamics of two lasers emitting at 4.4 and 8.1 µm operating in this bilobed regime are here investigated. The laser intensity shows a peculiar temporal behavior associated with the spectral features whereby, every half a round-trip, the total emitted power switches from one lobe to the other, with a perfect temporal anti-correlation. The anti-correlation between the lobes is also observed in the intensity noise figure of the emission. This coherent phenomenon arises from gain nonlinearities induced by spatial hole burning and the extremely fast gain dynamics typical of quantum cascade lasers.

Broadband surface-emitting THz laser frequency combs with inverse-designed integrated reflectors

THz quantum cascade lasers (QCLs) based on double metal waveguides feature broadband and high-temperature devices for their use in spectroscopy and sensing. However, their extreme field confinement produces poor output coupling efficiencies and divergent far-fields. Here, we present a planarized THz QCL with an inverse-designed end facet reflector coupled to a surface-emitting patch array antenna. All the components have been optimized for octave-spanning spectral bandwidths between 2 and 4 THz and monolithically integrated on the same photonic chip. We demonstrate this experimentally on broadband THz QCL frequency combs, with measured devices showing a seven-fold improvement in slope efficiency compared to devices with a cleaved facet. They feature a peak power of up to 13.5 mW with surface emission into a narrow beam with a divergence of (17.0° × 18.5°), while broadband fundamental and harmonic comb states spanning up to 800 GHz are observed.

Coherent control of mid-infrared frequency comb by optical injection of near-infrared light

We demonstrate the use of a low power near-infrared laser illuminating the front facet of a quantum cascade laser (QCL) as an optical actuator for the coherent control of a mid-infrared frequency comb. We show that with appropriate current control of the QCL comb and intensity modulation of the near-infrared laser, a tight phase lock of a comb line to a distributed feedback laser is possible with 2 MHz of locking bandwidth and 200 mrad of residual phase noise. A characterization of the whole scheme is provided, showing the limits of the electrical actuation, which we bypassed using the optical actuation. Both comb degrees of freedom can be locked by performing electrical injection locking of the repetition rate in parallel. However, we show that the QCL acts as a fast near-infrared light detector such that injection locking can also be achieved through modulation of the near-infrared light. These results on the coherent control of a QCL frequency comb are particularly interesting for coherent averaging in dual-comb spectroscopy and for mid-infrared frequency comb applications requiring high spectral purity.

Electro-Optic Sampling of a Free-Running Terahertz Quantum-Cascade-Laser Frequency Comb

Quantum-cascade-laser (QCL) frequency combs are compact semiconductor light sources operating in the mid-IR and terahertz frequencies. Achieving subpicosecond laser pulses with high peak power is of vital importance for performing nonlinear time-resolved spectroscopy as well for exploring nonlinear phenomena. Therefore, investigation and characterization of time-resolved free-running laser emission is a key for further improvement and optimization of these intersubband devices. In this work, we demonstrate a direct electric field measurement of a free-running terahertz QCL frequency comb using electro-optic sampling in combination with computational phase correction, where we retrieve the electric field profile and access the comb parameters. The demonstrated method is of high interest for time-resolved low-power laser emission characterization, typical for ring terahertz QCL frequency combs and investigation of phase-compensated emission via waveguide dispersion engineering for broadband comb operation.

Self-consistent simulations of intracavity terahertz comb difference frequency generation by mid-infrared quantum cascade lasers

Portable terahertz (THz) frequency comb sources are highly desired for applications in rotational molecular spectroscopy and sensing. To date, direct THz quantum cascade laser (QCL) frequency comb generation is not achievable at room temperature. However, THz comb generation based on intracavity difference frequency generation (DFG) in mid-infrared (mid-IR) QCLs is a promising alternative. Here, we present a numerical study of THz DFG-QCL comb formation in mid-IR QCLs based on a self-consistent multi-domain simulation approach. The dynamical simulations are performed using our open-source software tool mbsolve, which provides a flexible and efficient codebase for solving the generalized full-wave Maxwell–Bloch equations. Here, DFG in the active region of a dual-wavelength mid-IR QCL is considered for the generation of THz radiation. The mixing process and, thus, THz generation require a high second-order intersubband nonlinear susceptibility in the QCL active region and can be obtained by targeted quantum engineering. The associated nonlinear effects are included in the Hamiltonian of our Maxwell–Bloch simulation approach. All necessary input parameters for the description of the quantum system are determined self-consistently using our in-house ensemble Monte Carlo software tool for stationary carrier transport simulations. Notably, such simulations require a full-wave Maxwell–Bloch solver that does not employ the common rotating wave approximation, as a broadband optical field extending from the THz to the mid-IR region is investigated. Our modeling approach and the obtained simulation results for two THz DFG-QCL comb setups are validated against experimental data, showing reasonable agreement. Furthermore, we obtain a locked frequency modulated comb state for mid-IR and THz regimes.

Highly coherent phase-lock of an 8.1 μm quantum cascade laser to a turn-key mid-IR frequency comb

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.

THz optical beat-note detection with a fast superconducting hot electron bolometer operating up to 31 GHz.

We study the performance of a hot-electron bolometer (HEB) operating at THz frequencies based on superconducting niobium nitride films. We report on the voltage response of the detector over a large electrical detection bandwidth carried out with different THz sources. We show that the impulse response of the fully packaged HEB at 7.5 K has a 3 dB cutoff around 2 GHz. Remarkably, detection capability is still observed above 30 GHz in an heterodyne beating experiment using a THz quantum cascade laser frequency comb. Additionally, the HEB sensitivity has been evaluated and an optical noise equivalent power NEP of 0.8 pW/√H z has been measured at 1 MHz.

Frequency chirped Fourier-Transform spectroscopy

Fast (sub-second) spectroscopy with high spectral resolution is of vital importance for revealing quantum chemistry kinetics of complex chemical and biological reactions. Fourier transform (FT) spectrometers can achieve high spectral resolution and operate at hundreds of ms time scales in rapid-scan mode. However, the linear translation of a scanning mirror imposes stringent time-resolution limitations to these systems, which makes simultaneous high spectral and temporal resolution very difficult. Here, we demonstrate an FT spectrometer whose operational principle is based on continuous rotational motion of the scanning mirror, effectively decoupling the spectral resolution from the temporal one. Furthermore, we show that such rotational FT spectrometer can perform Mid-IR dual-comb spectroscopy with a single comb source, since the Doppler-shifted version of the comb serves as the second comb. In our realization, we combine the advantages of dual-comb and FT spectroscopy using a single quantum cascade laser frequency comb emitting at 8.2 μm as a light source. Our technique does not require any diffractive or dispersive optical elements and hence preserve the Jacquinot’s-, Fellgett’s-, and Connes’-advantages of FT spectrometers. By integrating mulitple broadband sources, such system could pave the way for applications where high speed, large optical bandwidth, and high spectral resolution are desired.

Relative phase locking of a terahertz laser system configured with a frequency comb and a single-mode laser

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.

Near-Full Current Dynamic Range THz Quantum Cascade Laser Frequency Comb.

The present study proposes a terahertz quantum cascade laser frequency comb (THz QCL FC) with a semi-insulated surface plasma waveguide characterized by a low threshold current density, high power and a wide current dynamic range. The gain dispersion value and the nonlinear susceptibility were optimized based on the combination of a hybrid bound-to-continuum active region with a semi-insulated surface plasmon waveguide. Without any extra dispersion compensator, stable frequency comb operation within a current dynamic range of more than 97% of the total was revealed by the intermode beat note map. Additionally, a total comb spectral emission of about 300 GHz centered around 4.6 THz was achieved for a 3 mm long and 150 µm wide device. At 10 K, a maximum output power of 22 mW was obtained with an ultra-low threshold current density of 64.4 A·cm-2.

Asynchronous Upconversion Sampling of Frequency Modulated Combs

AbstractIn recent years, optical frequency combs with a frequency modulated output have attracted considerable attention. While first observed decades ago in externally modulated lasers, a whole class of semiconductor lasers has since been identified to spontaneously enter such a regime of self frequency modulation. However, the temporal properties of these sources could so far only be measured indirectly via phase‐resolved frequency domain measurements. In this work, an asynchronous optical sampling technique which operates directly in time domain is demonstrated. On the basis of a mid‐infrared quantum cascade laser frequency comb, both its instantaneous intensity and optical frequency are measured. The results confirm a quasi‐constant intensity output alongside a close to linear frequency chirp, in accordance with phase‐resolved spectral measurements. Contrary to previous works, stable phase‐locking is achieved in a regime of positive intracavity dispersion resulting in an inversion of the observed frequency modulation.

Gapless tuning of quantum cascade laser frequency combs with external cavity optical feedback.

We present the operation of quantum cascade laser frequency combs in an external cavity configuration. Experimental observations show dependence of comb repetition rate and optical spectrum on the external cavity length. The low phase-noise comb regime is extended to a broader range of bias currents, enabling gapless frequency tuning of the comb modes. Dual-comb measurements also confirm improved comb stability in the presence of unwanted optical feedback when operating in an external cavity configuration. These observations indicate that aside from the continuing efforts to assure low and uniform dispersion characteristics of quantum cascade laser frequency combs, the proposed simple approach of adding a broadband external cavity can significantly enhance operation of sub-optimal devices for spectroscopic applications.

Broadband THz quantum cascade laser frequency combs with surface emission and inverse-designed facet reflectors

We present a planarized waveguide cavity with an integrated broadband output coupler that improves both the output power and far-field properties of THz quantum cascade laser frequency combs. The laser mirror reflectivity can be tuned by the shape of the end facet, which is obtained with an efficient inverse design algorithm, where the structure is iteratively updated to match the desired figure of merit. Surface emission is achieved with a broadband patch-array antenna, and all the components have been optimized for octave-spanning emission spectra (2-4 THz). Experimentally, we demonstrate a broadband surface-emitting THz quantum cascade laser frequency comb with optical bandwidths of up to 800 GHz, surface emission into a narrow beam with divergence below (20° x 20°) and a peak power of 13 mW.

Quantum cascade laser frequency comb locked with 200 mrad residual phase noise

Using near-infrared light, we tightly-lock a mid-infrared quantum cascade laser frequency comb to another laser, achieving a residual integrated phase noise of 200 mrad. This high coherence is pertinent for highly-sensitive dual-comb spectroscopy and metrology.

Surface-emitting THz quantum cascade laser frequency comb with tunable external mirror dispersion compensation

We present a surface emitting THz quantum cascade laser frequency comb with an adjustable chromatic dispersion compensation via a mechanically tunable GTI cavity. Surface emission and high optical feedback into the laser cavity are achieved by a planarized ridge waveguide design with low reflectivity facets and two broadband patch array antennas for coupling to an external mirror (back side) and for power extraction (front side). We demonstrate direct and reproducible manipulation of the frequency comb state, specifically the comb stability and beatnote frequency tuning, by controlling the position of an external movable mirror.

Self‐Induced Phase Locking of Terahertz Frequency Combs in a Phase‐Sensitive Hyperspectral Near‐Field Nanoscope (Adv. Sci. 28/2022)

Hyperspectral Nanoimaging A hyperspectral terahertz near field optical microscope comprising a miniaturized quantum cascade laser frequency comb, acting simultaneously as a source and as a detector is presented. Quantum nanomaterials and related collective mode excitations can be probed at the nanoscale. More details can be found in article number 2200410 by Miriam Serena Vitiello and co-workers.