Terahertz frequency combs exploiting an on-chip solution processed graphene-quantum cascade laser coupled-cavity architecture
F. P. Mezzapesa, K. Garrasi, J. Schmidt, L. Salemi, V. Pistore, L. Li, A. G. Davies, E. H. Linfield, M. Riesch, C. Jirauschek, T. Carey, F. Torrisi, A. C. Ferrari, M. S. Vitiello
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31 pages, 11 figures, to be published in ACS Photonics
The ability to engineer quantum-cascade-lasers (QCLs) with ultrabroad gain spectra and with a full compensation of the group velocity dispersion, at Terahertz (THz) frequencies, is a fundamental need for devising monolithic and miniaturized optical frequency-comb-synthesizers (FCS) in the far-infrared. In a THz QCL four-wave mixing, driven by the intrinsic third-order susceptibility of the intersubband gain medium, self-lock the optical modes in phase, allowing stable comb operation, albeit over a restricted dynamic range (~ 20% of the laser operational range). Here, we engineer miniaturized THz FCSs comprising a heterogeneous THz QCL integrated with a tightly-coupled on-chip solution-processed graphene saturable-absorber reflector that preserves phase-coherence between lasing modes even when four-wave mixing no longer provides dispersion compensation. This enables a high-power (8 mW) FCS with over 90 optical modes to be demonstrated, over more than 55% of the laser operational range. Furthermore, stable injection-locking is showed, paving the way to impact a number of key applications, including high-precision tuneable broadband-spectroscopy and quantum-metrology.
Hyperspectral imaging is a technique that allows for the creation of multi-color images. At terahertz wavelengths, it has emerged as a prominent tool for a number of applications, ranging from non-ionizing cancer diagnosis and pharmaceutical characterization to non-destructive artifact testing. Contemporary terahertz imaging systems typically rely on non-linear optical down-conversion of a fiber-based near-infrared femtosecond laser, requiring complex optical systems. Here, we demonstrate hyperspectral imaging with chip-scale frequency combs based on terahertz quantum cascade lasers. The dual …
Due to its fast and high resolution characteristics, dual-comb spectroscopy has attracted an increasing amount of interest since its first demonstration. In the terahertz frequency range where abundant absorption lines (finger prints) of molecules are located, multiheterodyne spectroscopy that employs the dual-comb technique shows an advantage in real-time spectral detection over the traditional Fourier transform infrared or time domain spectroscopies. Here, we demonstrate compact terahertz dual-comb spectroscopy based on quantum cascade lasers (QCLs). In our experiment, two free-running QCLs …
Broadband dual-comb spectroscopy has attracted increasing interests due to its unique advantages in high spectral resolution, fast detection, and so on. Although the dual-comb technique is relatively mature in the infrared wavelengths, it is, currently, not commercially capable of practical applications in the terahertz regime due to the lack of high performance broadband terahertz dual-comb sources. In the terahertz frequency range, the electrically pumped quantum cascade laser (QCL) is a suitable candidate for the dual-comb operation. However, free running terahertz QCL dual-comb sources nor…
We demonstrate a terahertz (THz) frequency comb that is flexible in terms of its frequency range and the number and spacing of comb lines. We use a combination of near-infrared laser diodes, phase modulation and opto-electronic frequency conversion. The THz comb lines are characterized to be < 10 MHz by resolving the pressure dependent collisional broadening of an ammonia molecule rotational mode.
We report on the engineering of broadband quantum cascade lasers (QCLs) emitting at Terahertz (THz) frequencies, which exploit a heterogeneous active region scheme and have a current density dynamic range (Jdr) of 3.2, significantly larger than the state of the art, over a 1.3 THz bandwidth. We demonstrate that the devised broadband lasers operate as THz optical frequency comb synthesizers in continuous wave, with a maximum optical output power of 4 mW (0.73 mW in the comb regime). Measurement of the intermode beatnote map reveals a clear dispersion-compensated frequency comb regime extending …
In the terahertz frequency range, the quantum cascade laser (QCL) is a suitable platform for the frequency comb and dual-comb operation. Improved comb performances have been always much in demand. In this work, by employing a symmetric thermal dissipation scheme, we report an improved frequency comb and dual-comb operation of terahertz QCLs. Two configurations of cold fingers, i.e., type A and B with asymmetric and symmetric thermal dissipation schemes, respectively, are investigated here. A finite-element thermal analysis is carried out to study the parametric effects on the thermal managemen…
Arising from modulation instability, Turing rolls in optical Kerr microresonators have been used in the generation of optical frequency combs and the synthesis of microwave and terahertz frequencies. In this work, by applying electro-optic modulation on terahertz-frequency Turing rolls, we implement electro-optic frequency division with a microcomb to synthesize variable low-noise microwave signals. We also actively stabilize the terahertz oscillations to a microwave reference via intracavity power modulation, obtaining fractional frequency instabilities that are better than those of the free-…
Real-time measurement of the absolute frequency of continuous-wave terahertz (CW-THz) waves is required for characterization and frequency calibration of practical CW-THz sources. We proposed a method for real-time monitoring of the absolute frequency of CW-THz waves involving temporally parallel, i.e., simultaneous, measurement of two pairs of beat frequencies and laser repetition frequencies based on dual THz combs of photocarriers (PC-THz combs) with different frequency spacings. To demonstrate the method, THz-comb-referenced spectrum analyzers were constructed with a dual configuration bas…
Dual-comb sources with equally spaced and low phase noise frequency lines are of great importance for high resolution spectroscopy and metrology. In the terahertz frequency range, electrically pumped semiconductor quantum cascade lasers (QCLs) are suitable candidates for frequency comb and dual-comb operation. For a single laser frequency comb, the repetition rate can be locked using a microwave injection locking and the carrier frequency can be locked to a highly stable source. However, for the locking of two laser combs, four frequencies (two repetition rates and two carrier offset frequenci…
We present a monolithic solution to extract efficiently light from terahertz quantum cascade lasers with metal-metal waveguides suitable for broadband frequency comb applications. The design is optimized for a bandwidth of 500 GHz around a center frequency of 2.6 THz. A five-fold increase in total output power is observed compared to standard metal-metal waveguides. The extractor features a single-lobed far-field pattern and increases the frequency comb dynamical range to cover more than 50 % of the laser dynamic range. Frequency comb operation up to a spectral bandwidth of 670 GHz is achieved…
We report the coherent generation and detection of terahertz (THz) pulses covering the bandwidth of 0.1-9 THz in a high repetition rate, low pulse energy laser system. In this work we demonstrate the application and evaluation of solid-state biased coherent detection in combination with a spintronic emitter. This combination was used to generate and detect THz pulses in a time-domain spectroscopy (TDS) setup and tested on bulk nonlinear crystals. These results establish a new promising candidate to extend the possibilities for compact, broadband THz TDS systems driven by high repetition rate l…
We demonstrated combination of gapless terahertz (THz) comb with dual-comb spectroscopy, namely gapless dual-THz-comb spectroscopy, to achieve the spectral resolution equal to width of the THz comb tooth. The gapless THz comb was realized by interpolating frequency gaps between the comb teeth with sweeping of a laser mode-locked frequency. The demonstration of low-pressure gas spectroscopy with gapless dual-THz-comb spectroscopy clearly indicated that the spectral resolution was decreased down to 2.5-MHz width of the comb tooth and the spectral accuracy was enhanced to 10-6 within the spectral…
Frequency combs based on terahertz quantum cascade lasers feature broadband coverage and high output powers in a compact package, making them an attractive option for broadband spectroscopy. Here, we demonstrate the first multi-heterodyne spectroscopy using two terahertz quantum cascade laser combs. With just 100 $μ$s of integration time, we achieve peak signal-to-noise ratios exceeding 60 dB and a spectral coverage greater than 250 GHz centered at 2.8 THz. Even with room-temperature detectors we are able to achieve peak signal-to-noise ratios of 50 dB, and as a proof-of-principle we use these…
By using two mutually phase-locked optical frequency combs with slightly different repetition rates, we demonstrate asynchronous optical-sampling terahertz time-domain spectroscopy (ASOPS THz-TDS) without using any trigger signals or optical delay lines. Due to a tight stabilization of the repetition frequencies, it was possible to accumulate the data over 48 minutes in a triggerless manner without signal degradation. The fractional frequency stability of the measured terahertz signal is evaluated to be $\sim$8.0$\times$10$^{- 17}$ after 730 s. The frequency accuracy of the obtained terahertz …
Compact and robust waveguide chips are crucial for new integrated terahertz applications, such as high-speed interconnections between processors and broadband short-range wireless communications. Progress on topological photonic crystals shows potential to improve integrated terahertz systems that suffer from high losses around sharp bends. Robust terahertz topological transport through sharp bends on a silicon chip has been recently reported over a relatively narrow bandwidth. Here, we report the experimental demonstration of topological terahertz planar air-channel metallic waveguides which …
The Terahertz or millimeter wave frequency band (300 GHz - 3 THz) is spectrally located between microwaves and infrared light and has attracted significant interest for applications in broadband wireless communications, space-borne radiometers for Earth remote sensing, astrophysics, and imaging. In particular optically generated THz waves are of high interest for low-noise signal generation. In particular optically generated THz waves are of high interest for low-noise signal generation. Here, we propose and demonstrate stabilized terahertz wave generation using a microresonator-based frequenc…
Detailed simulations for Terahertz quantum cascade lasers based on two-well designs are presented. We reproduce the maximal operation temperatures observed and attribute the degradation with temperature to the occupation of parasitic levels and thermal backfilling. Furthermore, we demonstrate that the current injection can be conveniently studied by using EZ states, which combine energy selectivity and spatial localisation. Improving the injection allows to achieve higher maximal operation temperatures around 265 Kelvin.
We report on the first experimental demonstration of terahertz (THz) whispering-gallery modes (WGMs) with an ultra high quality (Q) factor of $1.5 \times {10}^{4}$ at 0.62THz. The WGMs are observed in a high resistivity float zone silicon (HRFZ-Si) spherical resonator coupled to a sub-wavelength silica waveguide. A detailed analysis of the coherent continuous wave (CW) THz spectroscopy measurements combined with a numerical model based on Mie-Debye-Aden-Kerker (MDAK) theory allows to unambiguously identify the observed higher order radial THz WGMs.
We report on the first direct measurement of the emission character of quantum cascade laser based frequency combs, using intensity autocorrelation. The correlation technique is based on fast electro-optic sampling, with a bandwidth optimized to match the emission spectra of the comb laser, centered around 2.5~THz. We find the output light to be amplitude and frequency modulated at the same time, with intensity modulation depth as high as 90\%, occuring on timescales as short as few picoseconds. We compare these findings with intensity autocorrelation measurements of pulsed Terahertz light ori…
Mode-resolved dual-comb spectroscopy (DCS) is an emerging spectroscopic tool with the potential to simultaneously achieve a broad spectral coverage and ultrahigh spectral resolution in terahertz (THz) spectroscopy. However, the need for two independently stabilized ultrafast lasers significantly hampers the potential application of DCS techniques. In this article, we demonstrate mode-resolved DCS in the THz region based on a free-running single-cavity dual-comb fiber laser with adaptive sampling. Low-pressure spectroscopy of acetonitrile gas with absorption features approaching the Doppler lim…
Terahertz plasmons and magnetoplasmons propagating along electrically and chemically doped graphene p-n junctions are investigated. It is shown that such junctions support non-reciprocal magnetoplasmonic modes which get concentrated at the middle of the junction in one direction and split away from the middle of the junction in the other direction under the application of an external static magnetic field. This phenomenon follows from the combined effects of circular birefringence and carrier density non-uniformity. It can be exploited for the realization of plasmonic isolators.
Dual terahertz (THz) comb spectroscopy is a promising methods for high accuracy, high resolution, and broadband THz spectroscopy because the mode-resolved THz comb spectrum possesses both characteristics of broadband THz radiation and narrow-linewidth continuous-wave THz radiation and all frequency mode of THz comb can be phase-locked to a microwave frequency standard. However, requirement of stabilized dual femtosecond lasers has often hindered wide use of this method. In this article, we demonstrated the adaptive sampling, dual THz comb spectroscopy, enabling use of free-running dual femtose…
We report on an attempt to generate highly stable continuous terahertz (THz) wave by using optical frequency comb (OFC). About 10-nm wide OFC has been generated through a deep phase modulation of a 852 nm laser line in lithium niobate crystal cavity. The multiple optical modes (side bands) of the OFC, which are equally separated from each other by the modulation frequency (=6 GHz) are taken as the frequency reference. When another semiconductor laser is frequency locked, the stability of the difference frequency between the master laser and the second laser is improved on the same order of the…
Using an affordable ytterbium laser with sub-mJ of energy combined with a novel pulse compression technique, we demonstrate an extremely competitive state-of-the-art terahertz (THz) source with 53 mW of average power and 310 kV/cm at focus from the tilted-pulse front pumping scheme in lithium niobate at room temperature. Key points of this demonstration include the use of a pump pulse duration of 280 fs in combination with an echelon mirror. Our results present unmatched combined characteristics and are highly competitive with the existing THz sources pumped at the mJ range. This demonstration…
Terahertz quantum cascade laser sources based on intra-cavity difference frequency generation from mid-IR devices are an important asset for applications in rotational molecular spectroscopy and sensing, beingthe only electrically pumped device able to operate in the 0.6-6 THz range without the need of bulky andexpensive liquid helium cooling. Here we present comb operation obtained by intra-cavity mixing of adistributed feedback laser at λ = 6.5 μm and a Fabry-Pérot device at around λ = 6.9 μm. The resultingultra-broadband THz emission extends from 1.8 to 3.3 THz, with a total output power of…
The applications of terahertz (THz) radiation for plant water status monitoring require systematic studies on interaction of THz wave and plants. Here, we present theoretical investigations on scattering behavior of THz waves reflected by and transmitting through a plant leaf under different water content. A theoretical model combining integral equation and radiative transfer theory is presented to fit the measured data. Good agreement confirms the availability of the model for water status evaluation when variation of leaf thickness and surface roughness is considered. We investigate the appl…
We present an antipodal Vivaldi antenna for broadband double metal waveguide terahertz quantum cascade lasers and frequency combs. Its exponentially curved flare profile results in an adiabatic in-plane mode expansion, producing an improved far-field with a single-lobed beam of (23°x19°) full width half maximum with an octave-spanning bandwidth. The antenna also acts as a wave retarder, rotating the polarization from vertical toward horizontal polarization by a frequency-dependent angle. The laser's emission spectrum and current-voltage characteristics are not affected, as well as frequency co…
The recent demonstration of a terahertz (THz) molecular gas laser pumped by a mid-infrared quantum cascade laser (QCL) has opened up new perspectives for this family of sources, traditionally relying on CO2-laser pumping. A so far open question concerning QCL-pumped THz molecular lasers (MLs) is related to their spectral purity. Indeed, assessing their frequency/phase noise is crucial for a number of applications potentially exploiting these sources as local oscillators. Here this question is addressed by reporting the measurement of the frequency noise power spectral density (PSD) of a THz ML…
We present an extended study concerning the dynamics of dense and harmonic coherent regimes in quantum cascade lasers (QCLs) in a Fabry--Perot (FP) configuration emitting in the terahertz (THz) spectral region. Firstly, we study the device in free running operation, reproducing the main features of the self-generated of optical frequency combs (OFCs) and harmonic frequency combs (HFCs) in this spectral range, commenting on the points of difference from the mid-infrared region, and finding excellent agreement with the most recent experimental evidences. Then, we analyze the THz-QCL dynamics und…
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 of 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 optical frequency comb (FC) synthesizer over the whole laser operational regime, with up to 36 optically active laser modes delivering ~ 200 uW of optical power per comb tooth, a power level unreached so far in any THz QCL FC. A stable and narrow single beatnote,…
We present an electrically switchable graphene terahertz (THz) modulator with a tunable-by-design optical bandwidth and we exploit it to compensate the cavity dispersion of a quantum cascade laser (QCL). Electrostatic gating is achieved by a metal-grating used as a gate electrode, with an HfO2/AlOx gate dielectric on top. This is patterned on a polyimide layer, which acts as a quarter wave resonance cavity, coupled with an Au reflector underneath. We get 90% modulation depth of the intensity, combined with a 20 kHz electrical bandwidth in the 1.9 _ 2.7 THz range. We then integrate our modulato…
Carrier conversion from terahertz wave to dual-wavelength near-infrared light injection-locking to optical comb using asynchronous nonpolarimetric electro-optic downconversion with electro-optic polymer modulator
Quantum cascade lasers (QCLs) represent a fascinating accomplishment of quantum engineering and enable the direct generation of terahertz (THz) frequency radiation from an electrically-biased semiconductor heterostructure. Their large spectral bandwidth, high output powers and quantum-limited linewidths have facilitated the realization of THz pulses by active mode-locking and passive generation of optical frequency combs (FCs) through intracavity four-wave-mixing, albeit over a restricted operational regime. Here, we conceive an integrated architecture for the generation of high power (10 mW) …
We present a combined theoretical and experimental study of spatio-temporal propagation effects in terahertz (THz) generation in gases using two-color ionizing laser pulses. The observed strong broadening of the THz spectra with increasing gas pressure reveals the prominent role of spatio-temporal reshaping and of a plasma-induced blue-shift of the pump pulses in the generation process. Results obtained from (3+1)-dimensional simulations are in good agreement with experimental findings and clarify the mechanisms responsible for THz emission.
Rapid evolutions of microscopic fields govern the majority of elementary excitations in condensed matter and drive microelectronic currents at increasing frequencies. Beyond nominal "radio frequencies", however, access to local electric waveforms remains a challenge. Several imaging schemes resolve sub-wavelength fields up to multi-Terahertz (THz) frequencies - including scanning-probe techniques, electro-optic sampling or recent ultrafast electron microscopy. Yet, various constraints on sample geometries, acquisition speed and maximum fields limit applications. Here, we introduce ubiquitous f…
We report the development of new terahertz techniques for rapidly measuring the complex Faraday angle in systems with broken time-reversal symmetry using the cyclotron resonance of a GaAs two-dimensional electron gas in a magnetic field as a system for demonstration of performance. We have made polarization modulation, high sensitivity (< 1 mrad) narrow band rotation measurements with a CW optically pumped molecular gas laser, and by combining the distinct advantages of terahertz (THz) time domain spectroscopy and polarization modulation techniques, we have demonstrated rapid broadband rotatio…
We demonstrate a convenient and fast method to measure the spectrally resolved far-fields of multimode terahertz quantum cascade lasers by combining a microbolometer focal plane array with an FTIR spectrometer. Far-fields of fundamental TM0 and higher lateral order TM1 modes of multimode Fabry-Pérot type lasers have been distinguished, which very well fit to the results obtained by a 3D finite-element simulation. Furthermore, multimode random laser cavities have been investigated, analyzing the contribution of each single laser mode to the total far-field. The presented method is thus an impor…
Dual terahertz frequency combs for photonic RF readout of refractive index sensing with frequency multiplication and active-dummy temperature compensation
Graduate School of Sciences and Technology for Innovation, Tokushima University(德岛大学创新科学与技术研究生院);Department of Physics, Toho University(东邦大学物理系);School of System Engineering, Kochi University of Technology(高知工科大学系统工程学部);Institute of Post-LED Photonics (pLED), Tokushima University(德岛大学后LED光子学研究所(pLED));Institute of Photonics and Human Health Frontier (IPHF), Tokushima University(德岛大学光子学与人类健康前沿研究所(IPHF));Graduate School of Engineering Science, The University of Osaka(大阪大学工程科学研究生院)
Phase-locked ultrashort pulses in the rich terahertz (THz) spectral range have provided key insights into phenomena as diverse as quantum confinement, first-order phase transitions, high-temperature superconductivity, and carrier transport in nanomaterials. Ultrabroadband electro-optic sampling of few-cycle field transients can even reveal novel dynamics that occur faster than a single oscillation cycle of light. However, conventional THz spectroscopy is intrinsically restricted to ensemble measurements by the diffraction limit. As a result, it measures dielectric functions averaged over the s…