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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 {\lambda} = 6.5 {\mu}m and a Fabry-P\'erot device at around {\lambda} = 6.9 {\mu}m. The resultingultra-broadband THz emission extends from 1.8 to 3.3 THz, with a total output power of 8 {\mu}W at 78K.The THz emission has been characterized by multi-heterodyne detection with a primary frequencystandard referenced THz comb, obtained by optical rectification of near infrared pulses. The down-converted beatnotes, simultaneously acquired, confirm an equally spaced THz emission down to 1 MHzaccuracy. In the next future this setup can be used for Fourier transform based evaluation of the phaserelation among the emitted THz modes, paving the way to room-temperature, compact and field-deployable metrological grade THz frequency combs.

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.

The road towards the realization of quantum cascade laser (QCL) frequency combs (QCL-combs) has undoubtedly attracted ubiquitous attention from the scientific community, as these devices promise to deliver all-in-one (i.e. a single, miniature, active devices) frequency comb (FC) synthesizers in a range as wide as QCL spectral coverage itself (from about 4 microns to the THz range), with the unique possibility to tailor their spectral emission by band structure engineering. For these reasons, vigorous efforts have been spent to characterize the emission of four-wave-mixing multi-frequency devices, aiming to seize their functioning mechanisms. However, up to now, all the reported studies focused on free-running QCL-combs, eluding the fundamental ingredient that turns a FC into a useful metrological tool. For the first time we have combined mode-locked multi-frequency QCL emitters with full phase stabilization and independent control of the two FC degrees of freedom. At the same time, we have introduced the Fourier transform analysis of comb emission (FACE) technique, used for measuring and simultaneously monitoring the Fourier phases of the QCL-comb modes. The demonstration of tailored-emission, miniaturized, electrically-driven, mid-infrared/THz coverage, fully-stabilized and fully-controlled QCL-combs finally enables this technology for metrological-grade applications triggering a new scientific leap affecting several fields ranging from everyday life to frontier-research., Comment: 6 pages, 5 figures, conference proceeding Photonics West 2020

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 implementing a Cherenkov phase-matching scheme into a channel waveguide in a nonlinear crystal. This simple approach, entirely based on robust telecom technology, unprecedently merges in a single source an ultra-broad continuous-wave spectral coverage and a state-of-the-art accuracy (approximately 10-9) in molecular-transition-center determination.

The major development recently undergone by quantum cascade lasers has effectively extended frequency comb emission to longer-wavelength spectral regions, i.e. the mid and far infrared. Unlike classical pulsed frequency combs, their mode-locking mechanism relies on four-wave mixing nonlinear processes, with a temporal intensity profile different from conventional short-pulses trains. Measuring the absolute phase pattern of the modes in these combs enables a thorough characterization of the onset of mode-locking in absence of short-pulses emission, as well as of the coherence properties. Here, by combining dual-comb multi-heterodyne detection with Fourier-transform analysis, we show how to simultaneously acquire and monitor over a wide range of timescales the phase pattern of a generic frequency comb. The technique is applied to characterize a mid-infrared and a terahertz quantum cascade laser frequency comb, conclusively proving the high degree of coherence and the remarkable long-term stability of these sources. Moreover, the technique allows also the reconstruction of electric field, intensity profile and instantaneous frequency of the emission., Comment: 20 pages. Submitted to Nature Photonics

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) channel waveguides in the experimental accomplishment of a room-temperature continuous wave (CW) spectrometer, with uW-range power levels and a spectral coverage of up to 7.5 THz.To this purpose, and looking for further improvements, a thought characterization of specially-designed LN waveguides is presented, whilst discussing its nonlinear efficiency and its unprecedented capability to handle high optical power (10 7 W/cm 2 ), on the basis of a three-wave-mixing theoretical model.

We report on the development, testing, and performance analysis of a bow-tie resonant cavity for terahertz (THz) radiation, injected with a continuous-wave 2.55 THz quantum cascade laser. The bow-tie cavity employs a wire-grid polarizer as input/output coupler and a pair of copper spherical mirrors coated with an unprotected 500 nm thick gold layer. The improvements with respect to previous setups have led to a measured finesse value F=123, and a quality factor Q = 5.1x10^5. The resonator performances and the relevant parameters are theoretically predicted and discussed, and a comparison among simulated and experimental spectra is given.

Optical frequency comb synthesizers (FCs) [1] are laser sources covering a broad spectral range with a number of discrete, equally spaced and highly coherent frequency components, fully controlled through only two parameters: the frequency separation between adjacent modes and the carrier offset frequency. Providing a phase-coherent link between the optical and the microwave/radio-frequency regions [2], FCs have become groundbreaking tools for precision measurements[3,4]. Despite these inherent advantages, developing miniaturized comb sources across the whole infrared (IR), with an independent and simultaneous control of the two comb degrees of freedom at a metrological level, has not been possible, so far. Recently, promising results have been obtained with compact sources, namely diode-laser-pumped microresonators [5,6] and quantum cascade lasers (QCL-combs) [7,8]. While both these sources rely on four-wave mixing (FWM) to generate comb frequency patterns, QCL-combs benefit from a mm-scale miniaturized footprint, combined with an ad-hoc tailoring of the spectral emission in the 3-250 {\mu}m range, by quantum engineering [9]. Here, we demonstrate full stabilization and control of the two key parameters of a QCL-comb against the primary frequency standard. Our technique, here applied to a far-IR emitter and open ended to other spectral windows, enables Hz-level narrowing of the individual comb modes, and metrological-grade tuning of their individual frequencies, which are simultaneously measured with an accuracy of 2x10^-12, limited by the frequency reference used. These fully-controlled, frequency-scalable, ultra-compact comb emitters promise to pervade an increasing number of mid- and far-IR applications, including quantum technologies, due to the quantum nature of the gain media [10]., Comment: 12 pages, 6 figures

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 over a continuous 106 mA current range (current density dynamic range of 1.24), significantly larger than the state of the art reported under similar geometries, with a corresponding emission bandwidth of 1.05 THz ans a stable and narrow (4.15 KHz) beatnote detected with a signal-to-noise ratio of 34 dB. Analysis of the electrical and thermal beatnote tuning reveals a current-tuning coefficient ranging between 5 MHz/mA and 2.1 MHz/mA and a temperature-tuning coefficient of -4 MHz/K. The ability to tune the THz QCL combs over their full dynamic range by temperature and current paves the way for their use as powerful spectroscopy tool that can provide broad frequency coverage combined with high precision spectral accuracy.

Terahertz sources based on intra-cavity difference-frequency generation in mid-infrared quantum cascade lasers (THz DFG-QCLs) have recently emerged as the first monolithic electrically-pumped semiconductor sources capable of operating at room-temperature (RT) across the 1-6 THz range. Despite tremendous progress in power output, that now exceeds 1mW in pulsed and 10 {\mu}W in continuous-wave regime at room-temperature, knowledge of the major figure of merits of these devices for high precision spectroscopy, such as spectral purity and absolute frequency tunability, is still lacking. Here, by exploiting a metrological grade system comprising a terahertz frequency comb synthesizer, we measure, for the first time, the free-running emission linewidth (LW), the tuning characteristics, and the absolute frequency of individual emission lines of these sources with an uncertainty of 4 x 10-10. The unveiled emission LW (400 kHz at 1ms integration time) indicates that DFG-QCLs are well suited to operate as local oscillators and to be used for a variety of metrological, spectroscopic, communication, and imaging applications requiring narrow-linewidth THz sources.

We investigate the propagation of a coherent probe light pulse through a three-level atomic medium (in the $\Lambda$--configuration) in the presence of a pump laser under the conditions for gain without inversion. When the carrier frequency of the probe pulse and the pump laser are in a Raman configuration, we show that it is possible to amplify a slow propagating pulse. We also analyze the regime in which the probe pulse is slightly detuned from resonance where we observe anomalous light propagation., Comment: 7 pages, 10 figures. To be published in Europhysics Letters