Mid-infrared (mid-IR) frequency combs are powerful tools for molecular sensing, industrial monitoring, and precision spectroscopy, yet their development beyond 5 um remains limited. Electro-optic modulation offers a promising path toward compact, agile comb generation, but extending this approach into the mid-infrared has been hindered by the lack of practical, high-performance modulators. Here we present an approach that leads to efficient generation of mid infrared frequency combs around 9 um, by employing ultrafast, room temperature, free space electro optic intensity modulators. By driving a single modulator with short electrical pulse trains, we realize both single- and dual-comb operation from a continuous-wave quantum cascade laser, providing a compact and versatile platform for mid-IR spectroscopy. This scheme produces combs with tunable repetition rates down to the megahertz range with direct observation on an electrical spectrum analyzer without any interferometer. As a proof of concept, we perform single- and dual-comb spectroscopy of a germanium etalon and an ammonia cell, achieving resolution far beyond that of conventional Fourier-transform infrared (FTIR) spectrometers and highlighting the potential of this approach for precise measurements in the long-wavelength molecular-fingerprint region. These results establish high-performance mid-IR modulators as a promising route toward practical, energy-efficient frequency-comb systems for sensing and spectroscopy.
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 present an experimental technique to accurately predict the formation of vibro-polaritons from a molecular polymeric film embedded in a resonant mid-infrared cavity. Using simple Fourier-transform reflectance measurement, we extract the complex dielectric function of a polyethylene film using Kramers-Kronig relations. The fitted dielectric function can be plugged into a numerical code to predict the strength and dispersion of the strong light-matter coupling regime between the quantized electromagnetic modes of a microcavity and the vibrational bands of the molecules. As a demonstration, we experimentally resolve the simultaneous formation of multiple vibro-polariton modes issued from the strong coupling of some vibrational bands of the methylene group (CH 2 ) in a 2.5-mu m-thick polyethylene film embedded in a microcavity. We measure a Rabi splitting of 6.3 THz for the stretching doublet around 87.5 THz and a Rabi splitting of 1.1 THz for the scissoring doublet around 43.7 THz, in excellent agreement with numerical predictions.
In mammals, the suprachiasmatic nucleus of the hypothalamus is the master circadian pacemaker that synchronizes the clocks in the central nervous system and periphery, thus orchestrating rhythms throughout the body. However, little is known about how so many cellular clocks within and across brain circuits can be effectively synchronized. In this work, we investigated the implication of two possible pathways: (i) astrocytes-mediated synchronization and (ii) neuronal paracrine factors-mediated synchronization. By taking advantage of a lab-on-a-chip microfluidic device developed in our laboratory, here we report that both pathways are involved. We found the paracrine factors-mediated synchronization of molecular clocks is diffusion-limited and, in our device, effective only in case of a short distance between neuronal populations. Interestingly, interconnecting astrocytes define an active signaling channel that can synchronize molecular clocks of neuronal populations also at longer distances. At mechanism level, we found that astrocytes-mediated synchronization involves both GABA and glutamate, while neuronal paracrine factors-mediated synchronization occurs through GABA signaling. These findings identify a previously unknown role of astrocytes as active cells that might distribute long-range signals to synchronize the brain clocks, thus further strengthening the importance of reciprocal interactions between glial and neuronal cells in the context of circadian circuitry.
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 μm. 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.
We present a mid-IR ($\lambda \approx$ 8.3 μm) quantum well infrared photodetector (QWIP) fabricated on a transparent substrate, allowing photo detection 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) optical cavity. For two different excitation configurations - backside illumination through the substrate and frontside direct illumination - we present passive optical characterizations (reflectivity and transmissivity), electric transport measurements and photocurrent generation, showing similar broadband spectral response for the two detector ports and an experimental $T_{\text{blip}}$ of $\approx$ 200K.
We report on an ultra-low threshold saturable absorber operating in the mid-infrared spectral region (λ ~ 9 μm). The device relies on intersubband transitions in semiconductor quantum wells embedded in metallic microcavities. It operates in the strong light-matter coupling regime. The absorption change stems from the collapse of the polaritons resonances upon bleaching of the transition. We have developed an analytical formalism based on temporal coupled mode theory to model the device non-linear behavior. Using a commercial TEC-cooled quantum cascade laser as source, we demonstrate saturation with a peak pumping power of 150 mW (corresponding to an intensity on the sample of 10 kW.cm -2 ).
Abstract - Non-collinear pump-probe spectroscopy with phase-stable multi-THz pulses reveals the ultrafast scattering dynamics of intersubband polaritons in a dispersive microcavity. For resonant excitation of the lower polariton at a finite in-plane momentum, $k_{||}$, a narrowband maximum emerges in the probe reflectivity at the polaritonic ground state at $k_{||}=0$. A quantum mechanical model reproduces the experimental key results quantitatively and confirms the underlying microscopic process as stimulated polariton-polariton scattering. These results are an important milestone on the way to bosonic lasing in custom tailored polaritonic systems in the multi-THz and THz spectral regions.
The ultrafast scattering dynamics of intersubband polaritons in dispersive cavities embedding GaAs/AlGaAs quantum wells are studied directly within their band structure using a noncollinear pump-probe geometry with phase-stable midinfrared 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 toward quantum control and bosonic lasing in custom-tailored polaritonic systems in the mid and far infrared.
Non-collinear multi-THz pump-probe spectroscopy reveals the intersubband polariton dynamics in a dispersive microcavity. Selective pumping of the lower polariton at finite in-plane momentum leads to coherent polariton-polariton scattering towards the ground state.
A thin layer of a mid-IR transparent polymer is inserted inside a metallic nano-resonator, where a photonic mode and an intersubband transition are strongly coupled. Acting as a non-perturbative transducer, and without essentially modifying the optical response, the polymer allows the detection of absorbed optical power in the form of thermal expansion due to heat dissipation. This innovative approach permits to identify - at the nano-resonator level - the typical anti crossing characteristic of the polaritonic system, and to perform direct imaging of the electromagnetic fields buried within the optical cavity.
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 the study of the light-matter interaction in single subwavelength-sized nanocavities where far-field spectroscopy is not possible using conventional techniques. We inserted a thin (∼150 nm) polymer layer with negligible absorption in the mid-infrared range (5 μm < λ < 12 μm) 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 λ = 8.3 μm, and the nanocavity is overall 270 nm thick. Acting as a nonperturbative 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 atomic force microscopy (AFM). This innovative approach allows the typical anticrossing characteristic of the polaritonic dispersion to be identified in the cavity loss spectra at the single nanoresonator 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 a strong light-matter interaction.
We resolve the dispersion of multiple vibro-polariton modes issued from the coupling of several vibrational bands of the methylene group with a resonant modes of a mid-infrared micro-cavity. The experimental results are in excellent agreement with numerical simulations.
Surface current patterns in single patch antennas are imaged by means of photoexpansion nanospectroscopy performed with an atomic force microscopy probe and a broadly tunable quantum cascade laser system. The local ohmic losses lead to temperature increase of a thin polymer layer positioned in the cavity, which then expands.
The activation of the T cell mediated immune response relies on the fine interaction between the T cell receptor on the immune cell and the antigen-presenting major histocompatibility complex (MHC) molecules on the membrane surface of antigen-presenting cells. Both the distribution and quantity of MHC/peptide complexes and their adequate morphological presentation affect the activation of the immune cells. In several types of cancer the immune response is downregulated due to the low expression of MHC-class I (MHC-I) molecules on the cell's surface, and in addition, the mechanical properties of the membrane seem to play a role. Herein, we investigate the distribution of MHC-I molecules and the related nanoscale mechanical environment on the cell surface of two cell lines derived from colon adenocarcinoma and a healthy epithelial colon reference cell line. Atomic force microscopy (AFM) force spectroscopy analysis using an antibody-tagged pyramidal probe specific for MHC-I molecules and a formula that relates the elasticity of the cell to the energy of adhesion revealed the different population distributions of MHC-I molecules in healthy cells compared to cancer cells. We found that MHC-I molecules are significantly less expressed in cancer cells. Moreover, the local elastic modulus is significantly reduced in cancer cells. We speculate that these results might be related to the proven ability of cancer cells to evade the immune system, not only by reducing MHC-I cell surface expression but also by modifying the local mechanical properties affecting the overall morphology of MHC-I synapse presentation to immune cells.
The strong light-matter coupling is an exotic phenomenon of interest not only for basic physics, but also because it has potential for improving optoelectronic devices. When dealing with conduction band electrons in semiconductor quantum wells (QWs), intersubband (ISB) transitions can couple to the optical resonances of plasmonic antennas. In the case of strong light-matter coupling, a characteristic anticrossing of the "light" and "matter" excitations is observed. It stems from the appearance of new eigenmodes, called cavity polaritons.
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.
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$μ$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.