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The intensity noise of a laser source represents one of the key factors limiting the ultimate sensitivity in laser-based systems for sensing and telecommunication. For advanced applications based on interferometry, the availability of a shot-noise-limited local oscillator is even more important for the effective feasibility of high-precision measurements. This is particularly crucial in quantum optics applications based on homodyne detection schemes to measure non-classical light states, such as squeezed states. This work deeply investigates and analyzes the intensity noise features of the most widely used mid-infrared semiconductor heterostructured lasers: quantum cascade and interband cascade lasers. For this purpose, a comprehensive comparison of three different continuous-wave lasers operating at room temperature around 4.5 {\mu}m wavelength is presented. First, a thorough electro-optical characterization is given, highlighting the differences and the shared common characteristics of the tested devices. Then, a detailed intensity noise analysis is reported, identifying their different noise operations with a particular reference to shot-noise-limited operations. Finally, some perspectives towards advanced applications are discussed., Comment: 17 pages, 5 figures

Many precision applications in the mid-infrared spectral range have strong constraints based on quantum effects that are expressed in particular noise characteristics. They limit, e.g., sensitivity and resolution of mid-infrared imaging and spectroscopic systems as well as the bit-error rate in optical free-space communication. Interband cascade lasers (ICLs) are a class of mid-infrared laser exploiting interband transitions in type-II band alignment geometry. They are currently gaining significant importance for mid-infrared applications from <3 {\mu}m to >6 {\mu}m wavelength, enabled by novel types of high-performance ICLs such as ring-cavity devices. Their noise-behavior is an important feature that still needs to be thoroughly analyzed, including its potential reduction with respect to the shot noise limit. In this work, we provide a comprehensive characterization of {\lambda} = 3.8 {\mu}m-emitting, continuous-wave ring-ICLs operating at room temperature. It is based on an in-depth study of their main physical intensity noise features, such as their bias-dependent intensity noise power spectral density (INPSD) and relative intensity noise (RIN). We obtain shot-noise-limited statistics for Fourier frequencies above 100 kHz. This is an important result for precision applications, e.g. interferometry or advanced spectroscopy, which benefit from exploiting the advantage of using such a shot-noise limited source, enhancing the setup sensitivity. Moreover, it is an important feature for novel quantum optics schemes including testing specific light states below the shot noise level, such as squeezed states.

The recent development of Quantum Cascade Lasers (QCLs) represents one of the biggest opportunities for the deployment of a new class of Free Space Optical (FSO) communication systems working in the mid-infrared (Mid-IR) wavelength range. As compared to more common FSO systems exploiting the telecom range, the larger wavelength employed in Mid-IR systems delivers exceptional benefits in case of adverse atmospheric conditions, as the reduced scattering rate strongly suppresses detrimental effects on the FSO link length given by the presence of rain, dust, fog and haze. In this work, we use a novel FSO testbed operating at \SI{4.7}{\micro m}, to provide a detailed experimental analysis of noise regimes that could occur in realistic FSO Mid-IR systems based on QCLs. Our analysis reveals the existence of two distinct noise regions, corresponding to different realistic channel attenuation conditions, which are precisely controlled in our setup. To relate our results with real outdoor configurations, we combine experimental data with predictions of an atmospheric channel loss model, finding that error-free communication could be attained for effective distances up to 8~km in low visibility conditions of 1 km. Our analysis of noise regimes may have a key relevance for the development of novel, long-range FSO communication systems based on Mid-IR QCL sources

A novel study on harmonic frequency combs emitted by Quantum Cascade Lasers (QCLs) is here presented, demonstrating the presence of intensity correlations between twin modes characterising the emission spectra. These originate from a Four-Wave Mixing (FWM) process driven by the active medium's third-order non-linearity. The study of such correlations is essential for the engineering of a new generation of semiconductor devices with the potential of becoming integrated emitters of light with quantum properties, such as squeezing and entanglement. Starting from experimental results, the limits of state-of-the-art technology are discussed as well as the possible methodologies that could lead to the detection of non-classical phenomena, or alternatively improve the design of QCLs, in the compelling perspective of generating quantum correlations in mid-infrared light., Comment: 14 pages, 6 figures

Photoacoustic spectroscopy (PAS) based gas sensors with high sensitivity, wide dynamic range, low cost, and small footprint are desirable across a broad range of applications in energy, environment, safety, and public health. However, most works have focused on either acoustic resonator to enhance acoustic wave or optical resonator to enhance optical wave. Herein, we develop a gas sensor based on doubly resonant PAS in which the acoustic and optical waves are simultaneously enhanced using combined optical and acoustic resonators in a centimeter-long configuration. Not only the lower detection limit is enhanced by the double standing waves, but also the upper detection limit is expanded due to the short resonators. As an example, we developed a sensor by detecting acetylene (C2H2), achieving a noise equivalent absorption of 5.7*10-13 cm-1 and a dynamic range of eight orders. Compared to the state-of-the-art PAS gas sensors, the developed sensor increases the sensitivity by two orders of magnitude and extends the dynamic range by three orders of magnitude. Besides, a laser-cavity-molecule locking strategy is proposed to provide additional flexibility of fast gas detection.

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 $\mu$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 parallel transmission of an independent digital signal via amplitude modulation at 5 MS/s is also demonstrated., Comment: 17 pages, 13 figures

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.

Quantum cascade lasers (QCLs) are becoming a key tool for plenty of applications, from the mid-infrared (mid-IR) to the THz range. Progress in related areas, such as the development of ultra-low-loss crystalline microresonators, optical frequency standards, and optical fiber networks for time and frequency dissemination, is paving the way for unprecedented applications in many fields. For most demanding applications, a thorough control of QCLs emission must be achieved. In the last few years, QCLs unique spectral features have been unveiled, while multifrequency QCLs have been demonstrated. Ultra-narrow frequency linewidths are necessary for metrological applications, ranging from cold molecules interaction and ultra-high sensitivity spectroscopy to infrared-THz metrology. A review of the present status of research in this field is presented, with a view of perspectives and future applications.

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.

Liquid droplet whispering-gallery-mode microresonators open a new research frontier for optomechanics and photonic devices. At visible wavelengths, where most liquids are transparent, a major contribution to a droplet optical quality factor is expected theoretically from thermal surface distortions and capillary waves. Here, we investigate experimentally these predictions using transient cavity ring-down spectroscopy. In this way, the optical out-coupling and intrinsic loss are measured independently while any perturbation induced by thermal, acoustic and laser-frequency noise is avoided thanks to the ultra-short light-cavity interaction time. The measurements reveal a photon lifetime ten times longer than the thermal limit and suggest that capillary fluctuations activate surface scattering effects responsible for light coupling.

We experimentally demonstrate and theoretically explain the onset of optical frequency combs in a simple cavity-enhanced second-harmonic-generation system, exploiting second-order nonlinear interactions. Two combs are simultaneously generated around the fundamental pump frequency, with a spectral bandwidth up to about 10 nm, and its second harmonic. We observe different regimes of generation, depending on the phase-matching condition for second-harmonic-generation. Moreover, we develop an elemental model which provides a deep physical insight into the observed dynamics. Despite the different underlying physical mechanism, the proposed model is remarkably similar to the description of third-order effects in microresonators, revealing a potential variety of new effects to be explored and laying the groundwork for a novel class of highly efficient and versatile frequency comb synthesizers based on second-order nonlinear materials., Comment: 25 pages, 7 figures