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We demonstrate a free-space amplitude modulator for mid-infrared radiation (lambda=9.6 um) that operates at room temperature up to at least 20 GHz (above the -3dB cutoff frequency measured at 8.2 GHz). The device relies on the ultra-fast transition between weak and strong-coupling regimes induced by the variation of the applied bias voltage. Such transition induces a modulation of the device reflectivity. It is made of a semiconductor heterostructure enclosed in a judiciously designed array of metal-metal optical resonators, that - all-together - behave as an electrically tunable surface. At negative bias, it operates in the weak light-matter coupling regime. Upon application of an appropriate positive bias, the quantum wells populate with electrons and the device transitions to the strong-coupling regime. The modulator transmission keeps linear with input RF power in the 0dBm - 9dBm range. The increase of optical powers up to 25 mW exhibit a weak beginning saturation a little bit below.

We report the upgrade and operation of a frequency-comb-assisted high-resolution mid-infrared molecular spectrometer allowing us to combine high spectral purity, SI-traceability, wide tunability and high sensitivity. An optical frequency comb is used to transfer the spectral purity of a SI-traceable 1.54 $\mu$m metrology-grade frequency reference to a 10.3 $\mu$m quantum cascade laser (QCL). The near-infrared reference is operated at the French time/frequency metrology institute, calibrated there to primary frequency standards, and transferred to Laboratoire de Physique des Lasers via the REFIMEVE fiber network. The QCL exhibits a line width of $\delta\nu\sim 0.1$ Hz, a sub-$10^{-15}$ relative frequency stability from 0.1 to 10 s and its frequency is traceable to the SI with a total relative uncertainty better than $4\times10^{-14}$ after 1-s averaging time. We have developed the instrumentation allowing comb modes to be continuously tuned over 9 GHz resulting in a QCL of record spectral purity uninterruptedly tunable at the precision of the reference over an unprecedented span of $\Delta\nu$ = 1.4 GHz. We have used our apparatus to conduct sub-Doppler spectroscopy of methanol in a multi-pass cell, demonstrating state-of-art frequency uncertainties down to the few kilohertz level ($\sim10^{-10}$ in relative value). We have observed weak intensity resonances unreported so far, resolved subtle doublets never seen before and brought to light discrepancies with the HITRAN database. This demonstrates the potential of our apparatus for probing subtle internal molecular processes, building accurate spectroscopic models of polyatomic molecules of atmospheric or astrophysical interest, and carrying out precise spectroscopic tests of fundamental physics., Comment: 14 pages, 5 figures

We describe the properties of a continuous-wave room-temperature quantum cascade laser operating at the long wavelength of 17 $\mu$m. Long wavelength mid-infrared quantum cascade lasers offer new opportunities for chemical detection, vibrational spectroscopy and metrological measurements using molecular species. In particular, probing low energy vibrational transitions would be beneficial to the spectroscopy of large and complex molecules, reducing intramolecular vibrational energy redistribution which acts as a decoherence channel. By performing linear absorption spectroscopy of the v2 fundamental vibrational mode of N2O molecules, we have demonstrated the spectral range and spectroscopic potential of this laser, and characterized its free-running frequency noise properties. Finally, we also discuss the potential application of this specific laser in an experiment to test fundamental physics with ultra-cold molecules.

This work presents two distinct approaches to estimating the exponent related to the distribution of optical rogue waves observed in supercontinuum generated in a single-mode fiber, that is, to quantifying the rogueness. The first is a generalization of the well-known Hill estimator, and the second relies on estimating all parameters of a multi-parameter model. We show that the model shows a good correspondence with experimental data, and that the two estimating approaches provide consistent results, which are significantly more accurate than those obtained with earlier methods of estimation. Furthermore, alternative visualization through the tail function revealed the presence of pump depletion as well as detector saturation leading to the breakdown of power-law behavior for the largest observations. We characterized this breakdown via a combination of an exponential and a generalized Pareto distribution. Additionally, we have uncovered a weak memory effect in the data, which can be attributed to changes of the refractive index in the single-mode fiber., Comment: 12 pages, 5 figures

Continuously graded parabolic quantum wells with excellent optical performances are used to overcome the low-frequency and thermal limitations of square quantum wells at terahertz frequencies. The formation of microcavity intersubband polaritons at frequencies as low as 1.8 THz is demonstrated, with a sustained ultra-strong coupling regime up to a temperature of 200K. It is additionally shown that the ultra-strong coupling regime is preserved when the active region is embedded in sub-wavelength resonators, with an estimated relative strength $\eta = \Omega_R / \omega_0 = 0.12$. This represents an important milestone for future studies of quantum vacuum radiation because such resonators can be optically modulated at ultrafast rates, possibly leading to the generation of non-classical light via the dynamic Casimir effect. Finally, with an effective volume of $2.10^{-6} \lambda_0^3$, it is estimated that fewer than 3000 electrons per resonator are ultra-strongly coupled to the quantized electromagnetic mode, proving it is also a promising approach to explore few-electron polaritonic systems operating at relatively high temperatures., Comment: 7 pages, 4 figures

We demonstrate that absorption saturation of a mid-infrared intersubband transition can be engineered to occur at moderate light intensities of the order of 10-20 kW$.$cm$^{-2}$ and at room temperature. The structure consists of an array of metal-semiconductor-metal patches hosting a judiciously designed 253 nm thick GaAs/AlGaAs semiconductor heterostructure. At low incident intensity the structure operates in the strong light-matter coupling regime and exhibits two absorption peaks at wavelengths close to 8.9 $\mu$m. Saturation appears as a transition to the weak coupling regime - and therefore to a single-peaked absorption - when increasing the incident intensity. Comparison with a coupled mode theory model explains the data and permits to infer the relevant system parameters. When the pump laser is tuned at the cavity frequency, the reflectivity decreases with increasing incident intensity. When instead the laser is tuned at the polariton frequencies, the reflectivity non-linearly increases with increasing incident intensity. At those wavelengths the system therefore mimics the behavior of a saturable absorption mirror (SESAM) in the mid-IR range, a technology that is currently missing.

Recently, the concept of strong light-matter coupling has been demonstrated in semiconductor structures, and it is poised to revolutionize the design and implementation of components, including solid state lasers and detectors. We demonstrate an original nanospectroscopy technique that permits to study the light-matter interaction in single subwavelength-sized nano-cavities where far-field spectroscopy is not possible using conventional techniques. We inserted a thin ($\approx$ 150 nm) polymer layer with negligible absorption in the mid-IR (5 $\mu$m < $\lambda$ < 12 $\mu$m) inside a metal-insulator-metal resonant cavity, where a photonic mode and the intersubband transition of a semiconductor quantum well are strongly coupled. The intersubband transition peaks at $\lambda$ = 8.3 $\mu$m, and the nano-cavity is overall 270 nm thick. Acting as a non-perturbative transducer, the polymer layer introduces only a limited alteration of the optical response while allowing to reveal the optical power absorbed inside the concealed cavity. Spectroscopy of the cavity losses is enabled by the polymer thermal expansion due to heat dissipation in the active part of the cavity, and performed using an atomic force microscope (AFM). This innovative approach allows the typical anticrossing characteristic of the polaritonic dispersion to be identified in the cavity loss spectra at the single nano-resonator level. Results also suggest that near-field coupling of the external drive field to the top metal patch mediated by a metal-coated AFM probe tip is possible, and it enables the near-field mapping of the cavity mode symmetry including in the presence of strong light-matter interaction.

The ultrafast scattering dynamics of intersubband polaritons in dispersive cavities embedding GaAs/AlGaAs quantum wells are studied directly within their band structure using a non-collinear pump-probe geometry with phase-stable mid-infrared pulses. Selective excitation of the lower polariton at a frequency of ~25 THz and at a finite in-plane momentum, $k_{||}$, leads to the emergence of a narrowband maximum in the probe reflectivity at $k_{||}=0$. A quantum mechanical model identifies the underlying microscopic process as stimulated coherent polariton-polariton scattering. These results mark an important milestone towards quantum control and bosonic lasing in custom-tailored polaritonic systems in the mid and far-infrared.

We theoretically study the coherent nonlinear response of electrons confined in semiconductor quantum wells under the effect of an electromagnetic radiation close to resonance with an intersubband transition. Our approach is based on the time-dependent Schr\"odinger-Poisson equation stemming from a Hartree description of Coulomb-interacting electrons. This equation is solved by standard numerical tools and the results are interpreted in terms of approximated analytical formulas. For growing intensity, we observe a redshift of the effective resonance frequency due to the reduction of the electric dipole moment and the corresponding suppression of the depolarization shift. The competition between coherent nonlinearities and incoherent saturation effects is discussed. The strength of the resulting optical nonlinearity is estimated across different frequency ranges from mid-IR to THz with an eye to ongoing experiments on Bose-Einstein condensation of intersubband polaritons and to the speculative exploration of quantum optical phenomena such as single-photon emission in the mid-IR and THz windows.

We present a mid-IR ($\lambda \approx$ 8.3 $\mu$m) quantum well infrared photodetector (QWIP) fabricated on a mid-IR transparent substrate, allowing photodetection with illumination from either the front surface or through the substrate. The device is based on a 400 nm-thick GaAs/AlGaAs semiconductor QWIP heterostructure enclosed in a metal-insulator-metal (MIM) cavity and hosted on a mid-IR transparent ZnSe substrate. Metallic stripes are symmetrically patterned by e-beam lithography on both sides of the active region. The detector spectral coverage spans from $\lambda \approx 7.15$ $\mu$m to $\lambda \approx 8.7$ $\mu$m by changing the stripe width L - from L = 1.0 $\mu$m to L = 1.3 $\mu$m - thus frequency-tuning the optical cavity mode. Both micro-FTIR passive optical characterizations and photocurrent measurements of the two-port system are carried out. They reveal a similar spectral response for the two detector ports, with an experimentally measured T$_{BLIP}$ of $\approx$ 200K., Comment: Copyright 2021 Mario Malerba, Mathieu Jeannin, Stefano Pirotta, Lianhe Li, Alexander Giles Davies, Edmund Linfield, Adel Bousseksou, Jean-Michel Manceau and Raffaele Colombelli. This article is distributed under a Creative Commons Attribution (CC BY) License. The following article has been submitted to APL Photonics. After it is published, it will be found at https://aip.scitation.org/journal/app

We experimentally resolve the dispersion of multiple vibro-polariton modes issued from the strong coupling of different vibrational bands of the methylene group (CH2) in a 2.56$\mu$m thick polyethylene film with the confined modes of a mid-infrared Fabry-Perot micro-cavity. We measure a Rabi frequency of 111 cm$^{-1}$ for the stretching doublet around 2950 cm$^{-1}$ and a Rabi frequency of 29 cm$^{-1}$ for the scissoring doublet around 1460 cm$^{-1}$. This simple experimental approach offers the possibility to accurately fit the measured molecular film dielectric function. We show that the polariton dispersion and Rabi splitting can be precisely predicted from numerical simulations, offering a valuable tool for the design of strongly coupled system and the development of novel molecular films with crystalline organization., Comment: Copyright 2021 Mario Malerba, Mathieu Jeannin, Paul Goulain, Adel Bousseksou, Raffaele Colombelli, Jean-Michel Manceau. This article is distributed under a Creative Commons Attribution (CC BY) License. The following article has been submitted to APL Photonics. After it is published, it will be found at https://aip.scitation.org/journal/app

We propose a unified description of intersubband absorption saturation for quantum wells inserted in a resonator, both in the weak and strong light-matter coupling regimes. We demonstrate how absorption saturation can be engineered. In particular we show that the saturation intensity increases linearly with the doping in the strong coupling regime, while it remains doping independent in weak coupling. Hence, countering intuition, the most suitable region to exploit low saturation intensities is not the ultra-strong coupling regime, but is instead at the onset of the strong light-matter coupling. We further derive explicit conditions for the emergence of bistability. This work sets the path towards yet unexisting ultrafast mid-infrared semiconductor saturable absorption mirrors (SESAMs) and bistable systems. As an example, we show how to design a mid-infrared SESAM with a three orders of magnitude reduction in saturation intensity, down to about 5 kW/cm2.

Applications relying on mid-infrared radiation (Mid-IR, $\lambda\sim$ 3-30 $\mu$m) have progressed at a very rapid pace in recent years, stimulated by scientific and technological breakthroughs. Mid-IR cameras have propelled the field of thermal imaging. And the invention of the quantum cascade laser (QCL) has been a milestone, making compact, semiconductor-based mid-IR lasers available to a vast range of applications. All the recent breakthrough advances stemmed from the development of a transformative technology. In addition to the generation and detection of light, a key functionality for most photonics systems is the electrical control of the amplitude and/or phase of an optical beam at ultra-fast rates (GHz or more). However, standalone, broadband, integrated modulators are missing from the toolbox of present mid-IR photonics integrated circuits and systems developers. We have developed a free-space amplitude modulator for mid-IR radiation ($\lambda\sim$ 10 $\mu$m) that can operate up to at least 1.5 GHz (-3dB cut-off at $\sim$ 750 MHz) and at room-temperature. The device relies on a semiconductor hetero-structure enclosed in a judiciously designed metal-metal optical resonator. At zero bias, it operates in the strong light-matter coupling regime up to 300K. By applying an appropriate bias, the device transitions to the weak coupling regime. The large change in reflectivity due to the disappearance of the polaritonic states is exploited to modulate the intensity of a mid-IR continuous-wave laser up to speeds of more than 1.5 GHz.

We developed a technique that enables to replace a metallic waveguide cladding with a low-index (n $\sim$ 1.4) material - CaF2 or BaF2 - that in addition is transparent from the mid-IR up to the visible range: elevated confinement is preserved while introducing an optical entryway through the substrate. Replacing the metallic backplane also allows double-side patterning of the active region. Using this approach, we demonstrate strong light-matter coupling between an intersubband transition (lambda $\sim$ 10 microns) and a dispersive resonator, at 300 K and at 78 K. Finally, we evaluate the potential of this approach as a platform for waveguiding in the mid-IR spectral range, with numerical simulations that reveal losses in the 1-10 cm$^{-1}$ range., Comment: just accepted in optics express

The phase uncertainty of an unseeded nonlinear interferometer, where the output of one nonlinear crystal is transmitted to the input of a second crystal that analyzes it, is commonly said to be below the shot-noise level but highly dependent on detection and internal loss. Unbalancing the gains of the first (source) and second (analyzer) crystals leads to a configuration that is tolerant against detection loss. However, in terms of sensitivity, there is no advantage in choosing a stronger analyzer over a stronger source, and hence the comparison to a shot-noise level is not straightforward. Internal loss breaks this symmetry and shows that it is crucial whether the source or analyzer is dominating. Based on these results, claiming a Heisenberg scaling of the sensitivity is more subtle than in a balanced setup., Comment: 11 pages, 4 figures, 1 table

Images of semiconductor `dot in rods' and their small clusters are studied by measuring the second-order correlation function with a spatially resolving ICCD camera. This measurement allows one to distinguish between a single dot and a cluster and, to a certain extent, to estimate the number of dots in a cluster. A more advanced measurement is proposed, based on higher-order correlations, enabling more accurate determination of the number of dots in a small cluster. Nonclassical features of the light emitted by such a cluster are analyzed., Comment: 4 pages, 4 figures