Quantum Cascade Laser Based Hybrid Dual Comb Spectrometer
Luigi Consolino, Malik Nafa, Michele De Regis, Francesco Cappelli, Katia Garrasi, Francesco P. Mezzapesa, Lianhe Li, A. Giles Davies, Edmund H. Linfield, Miriam… 展开作者
Luigi Consolino, Malik Nafa, Michele De Regis, Francesco Cappelli, Katia Garrasi, Francesco P. Mezzapesa, Lianhe Li, A. Giles Davies, Edmund H. Linfield, Miriam S. Vitiello, Saverio Bartalini, Paolo De Natale
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, optically-rectified THz frequency comb. A proof-of-principle application to methanol molecular transitions is presented. The multi-heterodyne molecular spectra retrieved provide state-of-the-art results in line-center determination, achieving the same precision as currently available molecular databases. The devised setup provides a solid platform for a new generation of THz spectrometers, paving the way to more refined and sophisticated systems exploiting full phase control of QCL-FCs, or Doppler-free spectroscopic schemes.
We demonstrate a robust and simple method for measurement, stabilization and tuning of the frequency of cw mid-infrared (MIR) lasers, in particular of quantum cascade lasers. The proof of principle is performed with a quantum cascade laser at 5.4 μm, which is upconverted to 1.2 μm by sum-frequency generation in orientation-patterned GaAs with the output of a standard high-power cw 1.5 μm fiber laser. Both the 1.2 μm and the 1.5 μm waves are measured by a standard Er:fiber frequency comb. Frequency measurement at the 100 kHz-level, stabilization to sub-10 kHz level, controlled frequency tuning …
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 frequ…
We demonstrate the performance of a dual frequency comb QCL spectrometer for the application of vibrational Stark spectroscopy. Measurements performed on fluorobenzene with the dual-comb spectrometer (DCS) were compared to results obtained using a conventional Fourier transform infrared (FTIR) instrument in terms of spectral response, parameter estimation, and signal-to-noise ratio. The dual-comb spectrometer provided similar qualitative and quantitative data as the FTIR setup in 250 times shorter acquisition time. For fluorobenzene, the DCS measurement resulted in a more precise estimation of…
As a potent greenhouse gas and ozone depleting agent, nitrous oxide (N$_2$O) plays a critical role in the global climate. Effective mitigation relies on understanding global sources and sinks which can be supported through isotopic analysis. We present a cross-dispersed spectrometer, coupled with a mid-infrared frequency comb, capable of simultaneously monitoring all singly substituted, stable isotopic variants of N$_2$O. Rigorous evaluation of the instrument lineshape function and data treatment are discussed. Laboratory characterization of the spectrometer demonstrates sub-GHz spectral resol…
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 impossible. Here, we demonstrate an FT spectrometer whose operational principle is based on continuous rotational…
We demonstrate the use of dual-comb spectroscopy for isotope ratio measurements. We show that the analysis spectral range of a free-running near-infrared dual-comb spectrometer can be extended to the mid-infrared by difference frequency generation to target specific spectral regions suitable for such measurements, and especially the relative isotopic ratio $δ{}^{13}$C. The measurements performed present a very good repeatability over several days with a standard deviation below 2$\unicode{x2030}$ for a recording time of a few tens of seconds, and the results are compatible with measurements ob…
Optical frequency combs enable all-solid-state spectrometers that will trigger a breakthrough in miniaturization and on-chip integration of mid-infrared sensing technology. Interband cascade lasers (ICLs) are an ideal candidate for practical implementations due to their low power consumption and zero-bias detection functionality. Here, we demonstrate the generation of self-starting ICL frequency combs. We show that the gain is fast enough to respond to beating of the intracavity field, which hinders the formation of short pulses. Instead, the ICL operates in a comb state, where the phases of t…
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…
Optical frequency-comb-based-high-resolution spectrometers offer enormous potential for spectroscopic applications. Although various implementations have been demonstrated, the lack of suitable mid-infrared comb sources has impeded explorations of molecular fingerprinting. Here we present for the first time a frequency-comb Fourier transform spectrometer operating in the 2100-to-3700-cm-1 spectral region that allows fast and simultaneous acquisitions of broadband absorption spectra with up to 0.0056 cm-1 resolution. We demonstrate part-per-billion detection limits in 30 seconds of integration …
Dual-frequency comb spectroscopy has emerged as a disruptive technique for measuring wide-spanning spectra with high resolution, yielding a particularly powerful technique for sensitive multi-component gas analysis. We present a spectrometer system based on dual electro-optical combs with subsequent conversion to the mid-infrared via tunable difference frequency generation, operating in the range from 3 to 4.7 $μ$m. The simultaneously recorded bandwidth is up to 454(1) GHz and a signal-to-noise ratio of 7.3(2) x 10$^2$ Hz$^{-1/2}$ can be reached. The conversion preserves the coherence of the d…
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…
We have developed a dispersive spectrometer using a compact immersion grating for direct frequency comb spectroscopy in the long-wave infrared region of 8-10 μm. A frequency resolution of 463 MHz is achieved, which is the highest reported in this wavelength region with a dispersive direct frequency comb spectrometer. We also demonstrate individual mode-resolved imaging of the frequency comb spectrum by Vernier cavity filtering and apply this to obtain both simple and complex molecular spectra. These results indicate that the immersion grating spectrometer offers the next advancement for sensit…
Optical frequency combs generated by multiple four-wave mixing of two stabilized single-frequency lasers in optical fibers are proposed for use as high precision frequency markers, calibration of astrophysical spectrometers and metrology. Use of highly nonlinear and photonic crystal fibers with very short lengths and small group velocity dispersion, combined with energy and momentum conservation required by the parametric generation, assures negligible phase mismatch between comb frequencies. In contrast to combs from mode-locked lasers or microcavities, the absence of a resonator allows large…
In the current study, a quantum-cascade-laser-based dual-comb spectrometer (DCS) was used to paint a detailed picture of a 1.0 ms high-temperature reaction between propyne and oxygen. The DCS interfaced with a shock tube to provide pre-ignition conditions of 1225 K, 2.8 atm, and 2% p-C3H4/18% O2/Ar. The spectrometer consisted of two free-running, non-stabilized frequency combs each emitting at 179 wavelengths between 1174 and 1233 cm-1. A free spectral range, f_r, of 9.86 GHz and a difference in comb spacing, Δf_r, of 5 MHz, enabled a theoretical time resolution of 0.2 us but the data was time…
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 …
Quantum cascade laser (QCL) frequency combs are a promising candidate for chemical sensing and biomedical diagnostics, requiring only milliseconds of acquisition time to record absorption spectra without any moving parts. They are electrically pumped and have a small footprint, making them an ideal platform for on-chip integration. Until now, optical feedback is fatal for frequency comb generation in QCLs and destroys intermodal coherence. This property imposes strict limits on the possible degree of integration. Here, we demonstrate coherent injection locking of the repetition frequency to a …
Quantum cascade laser (QCL) frequency combs have revolutionized mid-infrared (MIR) spectroscopy by their high brightness and fast temporal resolution, and are a promising technology for fully-integrated and cost-effective sensors. As for other integrated comb sources such as micro-combs and interband cascade laser, QCLs have a comb spacing of several GHz, which is adequate for measurements of wide absorbing structures, typically found in liquid or solid samples. However, high-resolution gas-phase spectra require spectral interleaving and frequency calibration. We developed a frequency calibrat…
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…
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…
We present quantum cascade laser (QCL) frequency comb devices with engineered waveguides for managing the dispersion. The QCL waveguide consists of multiple sections with different waveguide widths. The narrow and wide sections of the waveguide are designed in a way to compensate the group velocity dispersion (GVD) of each other and thereby produce a flat and slightly negative GVD for the QCL. The QCL exhibits continuous comb operation over a large part of the dynamic range of the laser. Strong and narrow-linewidth intermode beatnotes are achieved in more than 300 mA wide operation current ran…
Quantum cascade laser frequency combs are nowadays well-appreciated sources for infrared spectroscopy. Here their applicability for free-space optical communication is demonstrated. The spontaneously-generated intermodal beat note of the frequency comb is used as carrier for transferring the analog signal via frequency modulation. Exploiting the atmospheric transparency window at 4 $μ$m, an optical communication with a signal-to-noise ratio up to 65 dB is realized, with a modulation bandwidth of 300 kHz. The system tolerates a maximum optical attenuation exceeding 35 dB. The possibility of par…
We present gapless, high-resolution absorption and dispersion spectra obtained with quantum cascade laser frequency combs covering 55 cm$^{-1}$. Using phase-sensitive dual comb design, the comb lines are gradually swept over 10 GHz, corresponding to the free spectral range of the laser devices, by applying a current modulation. We show that with interleaving the spectral point spacing is reduced by more than four orders of magnitude over the full spectral span of the frequency comb. The potential of this technique for high-precision gas sensing is illustrated by measuring the low pressure (107…
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 …
The impact of photodetector nonlinearity on dual-comb spectrometers is described and compared to that of Michelson-based Fourier transform spectrometers (FTS). The optical sampling occurring in the dual-comb approach, being the key difference with FTS, causes optical aliasing of the nonlinear spectral artifacts. Measured linear and nonlinear interferograms are presented to validate the model. Absorption lines of H$^{13}$CN are provided to understand the impact of nonlinearity on spectroscopic measurements.
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…
We report the first experimental demonstration of frequency-locking of an extended-cavity quantum-cascade-laser (EC-QCL) to a near-infrared frequency comb. The locking scheme is applied to carry out absolute spectroscopy of N2O lines near 7.87 μm with an accuracy of ~60 kHz. Thanks to a single mode operation over more than 100 cm^{-1}, the comb-locked EC-QCL shows great potential for the accurate retrieval of line center frequencies in a spectral region that is currently outside the reach of broadly tunable cw sources, either based on difference frequency generation or optical parametric oscil…
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 broadband RF channelizer based on an integrated optical frequency Kerr micro-comb source, with an RF channelizing bandwidth of 90 GHz, a high RF spectral slice resolution of 1.04 GHz, and experimentally verify the RF performance up to 19 GHz. This approach to realizing RF channelizers offers reduced complexity, size, and potential cost for a wide range of applications to microwave signal detection.
In this work, a design for a mid-infrared quantum cascade laser (QCL) frequency comb source that enhances the high frequency response and the comb characteristics of the device is presented . A state-of-the-art active region (AR), grown on a heavily n-doped InP:Si substrate, was processed into a buried heterostructure with a microstrip-like line waveguide. As a result, the repetition rate frequency $f_{rep}$, around 11.09 GHz, can be locked to an injected narrow-linewidth radio frequency (RF) signal, over a range of more than 200 kHz with -10 dBm of injected power, which outperforms normal bur…
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 …
Dual comb spectroscopy (DCS) is a broadband technique offering high resolution and fast data acquisition. We describe a hybrid dual comb spectrometer comprising a broadband commercial fiber laser system offering a wide range of sample interrogation, and an actively mode locked semiconductor laser (MLL) having a widely tunable, relatively narrow spectrum. The mutual coherence over 100 seconds has been realized between the two combs. We employed the DCS system to characterize the absorption spectrum of rubidium atoms at 313 K with a high signal to noise ratio. The broadband laser is directly loc…
Mid-infrared (MIR) spectrometers are invaluable tools for molecular fingerprinting and hyper-spectral imaging. Among the available spectroscopic approaches, GHz MIR dual-comb absorption spectrometers have the potential to simultaneously combine the high-speed, high spectral resolution, and broad optical bandwidth needed to accurately study complex, transient events in chemistry, combustion, and microscopy. However, such a spectrometer has not yet been demonstrated due to the lack of GHz MIR frequency combs with broad and full spectral coverage. Here, we introduce the first broadband MIR freque…
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…
The frequency noise power spectral density of a free-running quantum cascade laser frequency comb is investigated. A plateau is observed at high frequencies, attributed to the quantum noise limit set by the Schawlow-Townes formula for the total laser power on all comb lines. In our experiment, a linewidth of 292 Hz is measured for a total power of 25 mW. This result proves that the four-wave mixing process, responsible for the comb operation, effectively correlates the quantum noise of the individual comb lines.
Dual-comb spectroscopy is a rapidly developing technique that enables moving parts-free, simultaneously broadband and high-resolution measurements with microseconds of acquisition time. However, for high sensitivity measurements and extended duration of operation, a coherent averaging procedure is essential. To date, most coherent averaging schemes require additional electro-optical components, which increase system complexity and cost. Instead, we propose an all-computational solution that is compatible with real-time architectures and allows for coherent averaging of spectra generated by fre…
One salient characteristic of Quantum Cascade Laser (QCL) is its very shor gain recovery time that so far thwarted the attempts to achieve self-mode locking of the device into a train of single pulses. We show theoretically that four wave mixing, combined with the short gain recovery time causes QCL to operate in the self-frequency-modulated regime characterized by a constant power in time domain and stable coherent comb in the frequency domain.Coherent frequency comb may enable many potential applications of QCL in sensing and measurement.
We present an experimental study of optical frequency comb generation based on cascaded quadratic nonlinearities inside a continuous-wave-pumped optical parametric oscillator. We demonstrate comb states which produce narrow-linewidth intermode beat note signals, and we verify the mode spacing uniformity of the comb at the Hz level. We also show that spectral quality of the comb can be improved by modulating the parametric gain at a frequency that corresponds to the comb mode spacing. We have reached a high average output power of over 4 W in the near-infrared region, at ~2 μm.
Optical cavities provide high sensitivity to dispersion since their resonance frequencies depend on the index of refraction. We present a direct, broadband, and accurate measurement of the modes of a high finesse cavity using an optical frequency comb and a mechanical Fourier transform spectrometer with a kHz-level resolution. We characterize 16000 cavity modes spanning 16 THz of bandwidth in terms of center frequency, linewidth, and amplitude. We retrieve the group delay dispersion of the cavity mirror coatings and pure N${_2}$ with 0.1 fs${^2}$ precision and 1 fs${^2}$ accuracy, as well as t…
A recent publication on arXiv:1905.00668 suggests that the phase relationship within a frequency comb can be reconstructed from a heterodyne measurement using a reference comb. In principle, following this approach, such retrieval of optical phases appears possible, but should give rise to a temporally constant signal. Instead, arXiv:1905.00668 provides experimental evidence for a pronounced relative drift of the phases, which indicates that the modes of the comb are not coherently phase-locked. This temporal drift can be explained if the comb under test is not equidistant. This further means …
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…
Dual comb spectroscopy (DCS) is a powerful technique for broadband spectroscopy with high precision and fast data acquisition. High-frequency resolution requires long data acquisition times, limiting the temporal resolution in time-resolved measurements. Here we overcome this limitation by engineering the DCS pulse train that interacts with the sample. The measurement is performed in steps where the number of pulses interacting with the sample varies in each step. The DCS spectrum is recorded in each stage, and a multi-dimensional spectrum is generated from which the system time evolution is d…
Dual-comb spectroscopy is emerging as one of the most appealing applications of mid-infrared frequency combs for high-resolution molecular spectroscopy, as it leverages on the unique coherence properties of frequency combs combined with the high sensitivities achievable by mid-infrared molecular spectroscopy. Here we present an on-chip dual-comb source based on mid-infrared quantum cascade laser frequency combs, where two frequency combs are integrated on a single chip. Control of the combs repetition and offset frequencies is obtained by integrating micro-heaters next to each laser. We show t…
The cascade of resonant topological structures with $\mathcal{PT}$-symmetry breaking is shown to emit laser light with a frequency-comb spectrum. We consider optically active topological Aubry-André-Harper lattices supporting edge-modes at regularly spaced frequencies. When the amplified resonances in the $\mathcal{PT}$-broken regime match the edge modes of the topological gratings, we predict the emission of discrete laser lines. A proper design enables to engineer the spectral features for specific applications. The robustness of the topological protection makes the system very well suited f…
Quantum cascade lasers are compact sources capable of generating frequency combs. Yet key characteristics - such as optical bandwidth and power-per-mode distribution - have to be improved for better addressing spectroscopy applications. Group delay dispersion plays an important role in the comb formation. In this work, we demonstrate that a dispersion compensation scheme based on a Gires-Tournois Interferometer integrated into the QCL-comb dramatically improves the comb operation regime, preventing the formation of high-phase noise regimes previously observed. The continuous-wave output power …
For the growing demand of frequency combs in mid-infrared (mid-IR), known as the "molecular fingerprint" region of the spectrum [1], down conversion of near-IR frequency combs through half- harmonic generation offers numerous benefits including high conversion efficiency and intrinsic phase and frequency locking to the near-IR pump [2]. Hence cascaded half-harmonic generation promises a simple path towards extending the wavelength coverage of stable frequency combs. Here, we report a two-octave down-conversion of a frequency comb around 1 μm through cascaded half-harmonic generation with ~64% …
