We present a directly generated on-chip dual-comb source at THz frequencies. The multi-heterodyne beating signal of two free-running THz quantum cascade laser frequency combs is measured electrically using one of the combs as a detector, fully exploiting the unique characteristics of quantum cascade active regions. Up to 30 modes can be detected corresponding to a spectral bandwidth of 630 GHz, being the available bandwidth of the dual comb configuration. The multi-heterodyne signal is used to investigate the equidistance of the comb modes showing an accuracy of $10^{-12}$ at the carrier frequency of 2.5 THz.
The lack of coherent room-temperature sources in the whole terahertz spectral window (0.3-10 THz) has significantly hampered the growth of scientific and technological applications in this range. Among them, high-precision frequency measurements of molecular transitions play a central role but remain an open challenge. Here, room-temperature generation and detection of continuous-wave, broadly tunable, narrow-linewidth THz radiation are presented, and their application to high-resolution spectroscopy in the broad 1-7.5 THz spectral range is demonstrated. This result has been achieved by implem…
Subwavelength-slotted parallel plate waveguides exhibit a localized electromagnetic resonance bound to the slits at a frequency slightly below the transverse electric cutoff [R. Merlin, Phys. Rev. X 2, 031015 (2012)]. The resonance is long-lived and, as opposed to the vanishingly small transmission shown by a single sub-wavelength aperture, it gives perfect transmission for perfectly-conducting plates. We show that the aperture-supported resonances of a pair of slotted copper plates have long lifetimes at THz frequencies. Finite element method calculations show that these bound resonances can …
In this paper we present the outcome of the first international comparison in the terahertz frequency range among three different kinds of spectrometers. A Fourier-Transform infrared spectrometer, a Vector Network Analyzer and a Time-Domain Spectrometer have been employed for measuring the complex refractive index of three travelling standards made of selected dielectric materials in order to offer a wide enough range of parameters to be measured. The three spectrometers have been compared in terms of measurement capability and uncertainty.
We construct a terahertz time-domain spectrometer (THz-TDS) system based on photoconductive antenna (PCA). A 800 nm Ti sapphire femtosecond laser with 80 MHz repetition rate provides the pump and probe laser pulse, which has a 45 fs pulse width (as short as 15 fs is available) and as much as 400 mW power. Two commercial PCAs with 34 um and 6 um gap size are used as the emitter and receiver, respectively. We characterize this system by measuring its absolute radiated THz power, spectral bandwidth, signal-to-noise ratio (SNR), dynamic range and beam profile at the focal plane. We further analyze…
Continuous Wave (CW) Terahertz spectroscopy enabled by photomixing is a promising high precision spectroscopic tool for the examination of a wide variety of samples including biological, chemical, and solid state. However, often it would be of interest to examine isolated samples free from bulk effects that broaden spectral features. In this form samples with low concentrations of absorbers have a reduced cross section making coupling to an external driving field a challenge. By utilising THz metamaterials one can borrow the concepts of surface enhanced Raman spectroscopy to confine and concen…
Highly sensitive terahertz (THz) sensors for a myriad of applications are rapidly evolving. A widespread sensor concept is based on the detection of minute resonance frequency shifts due to a targeted specimen in the sensors environment. Therefore, cutting-edge high resolution continuous wave (CW) THz spectrometers provide very powerful tools to investigate the sensors' performances. However, unpredictable yet non negligible frequency drifts common to state-of-the-art CW THz spectrometers limit the sensors' accuracy for ultra-high precision sensing and metrology. Here, we overcome this deficie…
We demonstrate a single-shot terahertz spectrometer consisting of a modified Mach-Zehnder interferometer and a microbolometer focal plane array. The spectrometer is simple to use and can measure terahertz field autocorrelations and spectral power with no moving parts and no ultrashort-pulsed laser. It can effectively detect radiation at 10$\sim$40 THz when tested with a thermal source. It can be also used to measure the complex refractive index of a sample material. In principle, it can characterize both laser-based and non-laser-based terahertz sources and potentially cover 1$\sim$10 THz with…
The 1-10 terahertz (THz) spectral window is emerging as a key region for plenty of applications, requiring not yet available continuous-wave room-temperature THz spectrometers with high spectral purity and ultra-broad tunability. In this regard, the spectral features of stabilized telecom sources can actually be transferred to the THz range by difference frequency generation, considering that the width of the accessible THz spectrum generally scales with the area involved in the nonlinear interaction. For this reason, in this paper we extensively discuss the role of Lithium Niobate (LN) channe…
Two frequency combs can be used to measure the full complex response of a sample in a configuration which can be alternatively viewed as the equivalent of a dispersive Fourier transform spectrometer, infrared time domain spectrometer, or a multiheterodyne laser spectrometer. This dual comb spectrometer retains the frequency accuracy and resolution inherent to the comb sources. We discuss, in detail, the specific design of our coherent dual-comb spectrometer and demonstrate the potential of this technique by measuring the first overtone vibration of hydrogen cyanide, centered at 194 THz (1545 n…
Four-wave-mixing-based quantum cascade laser frequency combs (QCL-FC) are a powerful photonic tool, driving a recent revolution in major molecular fingerprint regions, i.e. mid- and far-infrared domains. Their compact and frequency-agile design, together with their high optical power and spectral purity, promise to deliver an all-in-one source for the most challenging spectroscopic applications. Here, we demonstrate a metrological-grade hybrid dual comb spectrometer, combining the advantages of a THz QCL-FC with the accuracy and absolute frequency referencing provided by a free-standing, optic…
Terahertz (THz) emission spectroscopy is a powerful method that allows one to measure the ultrafast dynamics of polarization, current, or magnetization in a material based on THz emission from the material. However, the practical implementation of this method can be challenging, and can result in significant errors in the reconstruction of the quantity of interest. Here, we experimentally and theoretically demonstrate a rigorous method of signal reconstruction in THz emission spectroscopy, and describe the main experimental and theoretical sources of reconstruction error. We identify the linea…
A new approach for image reconstruction in THz computed tomography (THz-CT) is presented. Based on a geometrical optics model containing the THz signal amplitude and phase, a novel algorithm for extracting an average phase from the measured THz signals is derived. Applying the algorithm results in a phase-contrast sinogram, which is further used for image reconstruction. For experimental validation, a fast THz time-domain spectrometer (THz-TDS) in transmission geometry is employed, enabling CT measurements within several minutes. Quantitative evaluation of reconstructed 3D printed plastic prof…
Acquisition of laser frequency with high resolution under continuous and abrupt tuning conditions is important for sensing, spectroscopy and communications. Here, a single microresonator provides rapid and broad-band measurement of frequencies across the optical C-band with a relative frequency precision comparable to conventional dual frequency comb systems. Dual-locked counter-propagating solitons having slightly different repetition rates are used to implement a Vernier spectrometer. Laser tuning rates as high as 10 THz/s, broadly step-tuned lasers, multi-line laser spectra and also molecul…
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.
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…
High resolution (900 Hz full-width at half maximum) frequency domain spectroscopy near 0.2Terahertz is achieved using an exact frequency spacing comb-source in the optical communications band, filtering and photo-mixing in a custom Uni-Travelling-Carrier Photodiode (UTC-PD) for THz signal generation and coherent down-conversion for detection. Via time domain modulation of one of the comb lines, a fully controllable spectrometer can be defined in software, and this principle is demonstrated for magnetic field-free readout of the electronuclear spectrum for the Ho ions in \lihof, a material ofte…
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…
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…
We report on a heterogeneous active region design for terahertz quantum cascade laser based frequency combs. Dynamic range, spectral bandwidth as well as output power have been significantly improved with respect to previous designs. When operating individually the lasers act as a frequency comb up to a spectral bandwidth of 1.1 THz, while in a dispersed regime a bandwidth up to 1.94 THz at a center frequency of 3 THz can be reached. A self-detected dual-comb setup has been used to verify the frequency comb nature of the lasers.
We report on an optical frequency comb with 14nm (~1.8 THz) spectral bandwidth at -3 dB level that is generated using a passively mode-locked quantum-well (QW) laser in photonic integrated circuits (PICs) fabricated through an InP generic photonic integration technology platform. This 21.5-GHz colliding-pulse mode-locked laser cavity is defined by on-chip reflectors incorporating intracavity phase modulators followed by an extra-cavity SOA as booster amplifier. A 1.8-THz-wide optical comb spectrum is presented with ultrafast pulse that is 0.35-ps-wide. The radio frequency beat note has a 3-dB …
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…
Optical injection locking is implemented to faithfully transfer the phase noise of a dissipative Kerr microresonator soliton comb in addition to the amplification of the Kerr comb. Unlike Er-doped fiber and semiconductor optical amplifiers, the optical injection locking amplifies the comb mode without degrading the optical signal-to-noise ratio. In addition, we show that the residual phase noise of the optical injection locking is sufficiently small to transfer the relative phase noise of comb modes (equivalent to the repetition frequency) of low phase noise Kerr combs, concluding that the opt…
Harmonic comb state has proven to be emerging in quantum cascade lasers and promoted by an interplay between parametric gain and spatial hole burning. We report here on robust, pure, self-starting harmonic mode locking in Copper-based double-metal THz quantum cascade lasers. Different harmonic orders can be excited in the same laser cavity depending on the pumping condition and stable harmonic combs spanning more than 600 GHz bandwidth at 80 K are reported. Such devices can be RF injected and the free running coherence is assessed by means of self-mixing technique performed at 50 GHz. A theore…
Octave-wide frequency combs in microresonators are essential for self-referencing. However, it is difficult for the small-size and high-repetition-rate microresonators to achieve perfect soliton modelocking over the broad frequency range due to the detrimental impact of dispersion. Here we examine the stability of the soliton states consisting of one hundred modes in silicon-nitride microresonators with the one-THz free spectral range. We report the coexistence of fast and slow solitons in a narrow detuning range, which is surrounded on either side by the breather states. We decompose the brea…
We demonstrate a high-accuracy dual-comb spectrometer centered at 3.4 μm. The amplitude and phase spectra of the P, Q, and partial R-branch of the methane ν3 band are measured at 25 MHz to 100 MHz point spacing with ~kHz resolution and a signal-to-noise ratio of up to 3500. A fit of the absorbance and phase spectra yield the center frequency of 132 rovibrational lines. The systematic uncertainty is estimated to be 300 kHz, which is 10-3 of the Doppler width and a tenfold improvement over Fourier transform spectroscopy. These data are the first high- accuracy molecular spectra obtained with a d…
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 dual-comb spectrometer based on two passively mode-locked waveguide lasers integrated in a single Er-doped ZBLAN chip. This original design yields two free-running frequency combs having a high level of mutual stability. We developed in parallel a self-correction algorithm that compensates residual relative fluctuations and yields mode-resolved spectra without the help of any reference laser or control system. Fluctuations are extracted directly from the interferograms using the concept of ambiguity function, which leads to a significant simplification of the instrument that will …
A new difference-frequency method based on electro-optic phase modulators and two free-running lasers is reported to perform THz dual-comb spectroscopy.
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
THz oscillators generated via frequency-multiplication of microwaves are facing difficulty in achieving low phase noise. Photonics-based techniques, in which optical two tones are translated to a THz wave through opto-electronic conversion, are promising if the relative phase noise between the two tones is well suppressed. Here, a THz ($\approx$ 560 GHz) wave with a low phase noise is provided by a frequency-stabilized, dissipative Kerr microresonator soliton comb. The repetition frequency of the comb is stabilized to a long fiber in a two-wavelength delayed self-heterodyne interferometer, sig…
Ultraviolet frequency combs enable applications ranging from precision spectroscopy to atomic clocks by addressing the electronic transitions of atoms and molecules. Access to ultraviolet light via integrated nonlinear optics is usually hampered by the strong material dispersion and large waveguide attention in the ultraviolet region. Here we demonstrate a simple route to chip-scale ultraviolet comb generators, simultaneously showing a gap-free frequency span of ~128 terahertz and supercontinuum sourced by an ultrafast fiber laser. The simultaneous cubic and quadratic nonlinear processes are i…
Fourier transform spectroscopy based on incoherent light sources is a well-established tool in research fields from molecular spectroscopy and atmospheric monitoring to material science and biophysics. It provides broadband molecular spectra and information about the molecular structure and composition of absorptive media. However, the spectral resolution is fundamentally limited by the maximum delay range (Δ$_{max}$) of the interferometer, so acquisition of high-resolution spectra implies long measurement times and large instrument size. We overcome this limit by combining the Fourier transfo…
Room Temperature Terahertz Spectrometer with Quantum-Level Sensitivity
University of California Los Angeles（加州大学洛杉矶分校）；University of Michigan, Ann Arbor（密歇根大学安娜堡分校）；Jet Propulsion Laboratory, California Institute of Technology（加州理工学院喷气推进实验室）
Dual-comb generation from a single laser cavity provides a simple and high-performance solution to time sampling applications. We demonstrate a compact single-cavity dual-comb laser operating at gigahertz repetition rates and high repetition rate differences up to more than 100 kHz with sub-100 fs pulse duration. The single cavity approach leads to passive common noise suppression resulting in ultra-low relative timing jitter and fully resolvable comb lines in free-running operation. We showcase the laser performance with two application demonstrations: (a) time-domain spectroscopy of acetylen…
The quest for extrasolar planets and their characterisation as well as studies of fundamental physics on cosmological scales rely on capabilities of high-resolution astronomical spectroscopy. A central requirement is a precise wavelength calibration of astronomical spectrographs allowing for extraction of subtle wavelength shifts from the spectra of stars and quasars. Here, we present an all-fibre, 400 nm wide near-infrared frequency comb based on electro-optic modulation with 14.5 GHz comb line spacing. Tests on the high-resolution, near-infrared spectrometer GIANO-B show a photon-noise limit…
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,…
Beginning with a continuous wave laser at 1064 nm, we generate a 30 GHz electro-optic frequency comb which contains 100 lines spanning 3 THz. The initial comb is subsequently amplified, spectrally broadened in normal dispersion photonic crystal fiber, and then temporally compressed to provide 74 fs pulses with average power of up to 2.6 W. When launched into a second photonic crystal fiber with anomalous dispersion, a supercontinuum spanning 800-1350 nm is generated. Second harmonic generation allows for extension of the 30 GHz comb into the visible, yielding greater than 300 THz of total spec…
Frequency combs have revolutionized time and frequency metrology and in recent years, new frequency comb lasers that are highly compact or even on-chip have been demonstrated in the mid-infrared and THz regions of the electromagnetic spectrum. The emerging technologies include electrically pumped quantum and interband cascade semiconductor devices, as well as high-quality factor microresonators. In this guest editorial, the authors summarize recent advances in the field, the potential for rapid broadband spectroscopy, as well as the challenges and prospects for use in molecular gas sensing.
We report on the generation of frequency combs from the recently-discovered phenomenon of high-order sideband generation (HSG). A near-band gap continuous-wave (cw) laser with frequency $f_\text{NIR}$ was transmitted through an epitaxial layer containing GaAs/AlGaAs quantum wells that were driven by quasi-cw in-plane electric fields $F_\text{THz}$ between 4 and 50 kV/cm oscillating at frequencies $f_\text{THz}$ between 240 and 640 GHz. Frequency combs with teeth at $f_\text{sideband}=f_\text{NIR}+nf_\text{THz}$ ($n$ even) were produced, with maximum reported $n>120$, corresponding to a maximum…
Laser frequency combs are coherent light sources that simultaneously provide pristine frequency spacings for precision metrology and the fundamental basis for ultrafast and attosecond sciences. Recently, nonlinear parametric conversion in high-Q microresonators has been suggested as an alternative platform for optical frequency combs, though almost all in 100 GHz frequencies or more. Here we report a low-phase-noise on-chip Kerr frequency comb with mode spacing compatible with high-speed silicon optoelectronics. The waveguide cross-section of the silicon nitride spiral resonator is designed to…
We present homogeneous quantum cascade lasers (QCLs) emitting around 3 THz which display bandwidths up to 950 GHz with a single stable beatnote. Devices are spontaneously operating in a harmonic comb state, and when in a dense mode regime they can be injection locked at the cavity roundtrip frequency with very small RF powers down to -55 dBm. When operated in the electrically unstable region of negative differential resistance, the device displays ultra-broadband operation exceeding 1.83 THz ($Δf/f=50\%$) with high phase noise, exhibiting self-sustained, periodic voltage oscillations. The low …
Full phase control of THz emitting quantum cascade laser (QCL) combs has recently been demonstrated, opening new perspectives for even the most demanding applications. In this framework, simplifying the set-ups for control of these devices will help to accelerate their spreading in many fields. We report a new way to control the emission frequencies of a THz QCL comb by small optical frequency tuning (SOFT), using a very simple experimental setup, exploiting the incoherent emission of an ordinary white light emitting diode. The slightly perturbative regime accessible in these condition allows …
An electro-optic dual comb system based on chirped-pulse waveforms is used to simultaneously acquire temporally magnified rapid passage signals and normal spectral line shapes from the back-transformation to the time domain. Multi-heterodyne THz wave generation and detection is performed with the difference frequency mixing of two free-running lasers. The method is used to obtain THz spectra of formic acid in the 10 cm-1 to 20 cm-1 (300 GHz to 600 GHz) region over a range of pressures. The method is widely applicable across other spectral regions for investigations of the transient dynamics an…
High-order nonlinear light-matter interactions in gases enable generation of x-ray and attosecond light pulses, metrology, and spectroscopy. Optical nonlinearities in solid-state materials are particularly interesting for combining optical and electronic functions for high-bandwidth information processing. Third-order nonlinear optical processes in silicon have been used to process optical signals with greater than 1 GHz bandwidths. Fundamental physical processes for a Si-based optical modulator in the THz bandwidth range, however, have not yet been explored. Here we demonstrate ultrafast phon…
