Light pressure in droplet micro-resonators excited by free-space scattering.

A droplet optical resonator is a unique environment to investigate light-matter interaction and optomechanics in liquids. Here, we report on light pressure effects derived from whispering gallery modes excited in a liquid-polymer droplet micro-resonator by free-space laser scattering. From the nonlinear resonance spectrum observed in the visible, we provide evidence of photon pressure exerted at the liquid-air boundary and quantify it with a coherent physical model. Our findings pave the way to studies on micro-rheology and nonlinear optofluidics, where droplets serve as miniature liquid laboratories.

A self-operating broadband spectrometer on a droplet.

Small-scale Fourier transform spectrometers are rapidly revolutionizing infrared spectro-chemical analysis, enabling on-site and remote sensing applications that were hardly imaginable just few years ago. While most devices reported to date rely on advanced photonic integration technologies, here we demonstrate a miniaturization strategy which harnesses unforced mechanisms, such as the evaporation of a liquid droplet on a partially reflective substrate. Based on this principle, we describe a self-operating optofluidic spectrometer and the analysis method to retrieve consistent spectral information in spite of the intrinsically non-reproducible droplet formation and evaporation dynamics. We experimentally realize the device on the tip of an optical fiber and demonstrate quantitative measurements of gas absorption with a 2.6 nm resolution, in a 100 s acquisition time, over the 250 nm span allowed by our setup's components. A direct comparison with a commercial optical analyzer clearly points out that a simple evaporating droplet can be an efficient small-scale, inexpensive spectrometer, competitive with the most advanced integrated photonic devices.

Approaching the transit time limit for high-precision spectroscopy on metastable CO around 6 µm.

As molecular spectroscopy makes its comeback to the limelight of fundamental sciences, scientists need ever better coherent light sources and diagnostic methods. Of particular importance for molecular spectroscopy is the mid infrared spectral region, where strong and narrow ro-vibrational excitations have their fundamental transition frequencies. Unfortunately, much technology in some portions of this spectral region is still rather pioneering. Here we present a high-resolution spectroscopy experiment, based on a molecular beam setup, which pushes the measured linewidth close to the transit time limit, on the order of 100 kHz. Moreover, we discuss the issue of frequency-noise characterization and the linewidth measurement of the ultrastable infrared laser used in the experiment.

Modulation Instability Induced Frequency Comb Generation in a Continuously Pumped Optical Parametric Oscillator.

Continuously pumped passive nonlinear cavities can be harnessed for the creation of novel optical frequency combs. While most research has focused on third-order "Kerr" nonlinear interactions, recent studies have shown that frequency comb formation can also occur via second-order nonlinear effects. Here, we report on the formation of quadratic combs in optical parametric oscillator (OPO) configurations. Specifically, we demonstrate that optical frequency combs can be generated in the parametric region around half of the pump frequency in a continuously driven OPO. We also model the OPO dynamics through a single time-domain mean-field equation, identifying previously unknown dynamical regimes, induced by modulation instabilities, which lead to comb formation. Numerical simulation results are in good agreement with experimentally observed spectra. Moreover, the analysis of the coherence properties of the simulated spectra shows the existence of correlated and phase-locked combs. Our results reveal previously unnoticed dynamics of an apparently well assessed optical system, and can lead to a new class of frequency comb sources that may stimulate novel applications by enabling straightforward access to elusive spectral regions, such as the midinfrared.

Opto-mechanical oscillator in a nanoliter droplet.

Droplets are very simple physical systems, whereby surface tension shapes liquids into ideal opto-mechanical devices. This has recently enabled low-viscosity liquid samples to serve as miniature acoustic resonators harnessing optical generation of bulk vibrations, capillaries, or surface waves. Uniquely, a simple room-temperature pendant droplet can be activated as a hypersound-laser emitter when illuminated by a free-space, low-power visible laser thanks to stimulated Brillouin scattering of optical and acoustic whispering-gallery modes. Here, we demonstrate continuous operation of a liquid polymer opto-mechanical resonator and characterize its quality factor and long-term frequency stability. Our results point to the feasibility of all-liquid micro-mechanical oscillators working in the 50-100 MHz range. The stimulated generation of high-quality surface waves on nanoliter droplets gives momentum to new optical schemes for characterization of material viscous-elastic properties, laboratory investigation of atmospheric phenomena, and mass sensing for direct analysis of biological fluids based on ultrasound-hypersound coherent generation and detection.

Stimulated Brillouin Cavity Optomechanics in Liquid Droplets.

Liquid droplets are ubiquitous in nature wherein surface tension shapes them into perfect spheres with atomic-scale smooth surfaces. Here, we use stable droplets that cohost equatorial acoustical and optical resonances phase matched to enable the exchange of energy and momentum between sound and light. Relying on free-space laser excitation of multiple whispering-gallery modes, we harness a triple-resonant forward Brillouin scattering to stimulate optomechanical surface waves. Nonlinear amplification of droplet vibrations in the 60-70 MHz range is realized with spectral narrowing beyond the limit of material loss, thereby activating the droplet as hypersound-laser emitter.

Measuring molecular frequencies in the 1-10 µm range at 11-digits accuracy.

High-resolution spectroscopy in the 1-10 µm region has never been fully tackled for the lack of widely-tunable and practical light sources. Indeed, all solutions proposed thus far suffer from at least one of three issues: they are feasible only in a narrow spectral range; the power available for spectroscopy is limited; the frequency accuracy is poor. Here, we present a setup for high-resolution spectroscopy, whose approach can be applied in the whole 1-10 µm range. It combines the power of quantum cascade lasers (QCLs) and the accuracy achievable by difference frequency generation using an orientation patterned GaP crystal. The frequency is measured against a primary frequency standard using the Italian metrological fibre link network. We demonstrate the performance of the setup by measuring a vibrational transition in a highly-excited metastable state of CO around 6 µm with 11 digits of precision.

Fundamental limits in high-Q droplet microresonators.

Liquid droplet whispering-gallery-mode microresonators open a new research frontier for sensing, 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. With our scheme, 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 at least ten times longer than the thermal limit and indicate that capillary fluctuations activate surface scattering effects responsible for light coupling. This suggests that droplet microresonators are an ideal optical platform for ultra-sensitive spectroscopy of highly transparent liquid compounds in nano-liter volumes.

Super-Resonant Intracavity Coherent Absorption.

The capability of optical resonators to extend the effective radiation-matter interaction length originates from a multipass effect, hence is intrinsically limited by the resonator's quality factor. Here, we show that this constraint can be overcome by combining the concepts of resonant interaction and coherent perfect absorption (CPA). We demonstrate and investigate super-resonant coherent absorption in a coupled Fabry-Perot (FP)/ring cavity structure. At the FP resonant wavelengths, the described phenomenon gives rise to split modes with a nearly-transparent peak and a peak whose transmission is exceptionally sensitive to the intracavity loss. For small losses, the effective interaction pathlength of these modes is proportional respectively to the ratio and the product of the individual finesse coefficients of the two resonators. The results presented extend the conventional definition of resonant absorption and point to a way of circumventing the technological limitations of ultrahigh-quality resonators in spectroscopy and optical sensing schemes.

Laser-frequency locking to a whispering-gallery-mode cavity by spatial interference of scattered light.

We present a simple and effective method for frequency locking a laser source to a free-space-coupled whispering-gallery-mode cavity. The scheme relies on the interference of spatial modes contained in the light scattered by the cavity, where low- and high-order modes are simultaneously excited. A dispersion-shaped signal proportional to the imaginary component of the resonant optical field is simply generated by spatial filtering of the scattered light. Locking of a diode laser to the equatorial modes of a liquid droplet resonator is demonstrated using this scheme, and its performance is compared to the Pound-Drever-Hall technique. This new approach makes laser-frequency locking straightforward and shows a number of advantages, including robustness, low cost, and no need for sophisticated optical and electronic components.

Sub-kilohertz linewidth narrowing of a mid-infrared optical parametric oscillator idler frequency by direct cavity stabilization.

We stabilize the idler frequency of a singly resonant optical parametric oscillator directly to the resonance of a mid-infrared Fabry-Perot reference cavity. This is accomplished by the Pound-Drever-Hall locking scheme, controlling either the pump laser or the resonant signal frequency. A residual relative frequency noise power spectral density below 10(3) Hz(2)/Hz is reached on average, with a Gaussian linewidth of 920 Hz over 100 ms, which reveals the potential for reaching spectral purity down to the hertz level by locking the optical parametric oscillator against a mid-infrared cavity with state-of-the-art superior performance.

High-Q resonant cavities for terahertz quantum cascade lasers.

We report on the realization and characterization of two different designs for resonant THz cavities, based on wire-grid polarizers as input/output couplers, and injected by a continuous-wave quantum cascade laser (QCL) emitting at 2.55 THz. A comparison between the measured resonators parameters and the expected theoretical values is reported. With achieved quality factor Q ≈ 2.5 × 10(5), these cavities show resonant peaks as narrow as few MHz, comparable with the typical Doppler linewidth of THz molecular transitions and slightly broader than the free-running QCL emission spectrum. The effects of the optical feedback from one cavity to the QCL are examined by using the other cavity as a frequency reference.

Widely-tunable mid-infrared fiber-coupled quartz-enhanced photoacoustic sensor for environmental monitoring.

A compact widely-tunable fiber-coupled sensor for trace gas detection of hydrogen sulfide (H2S) in the mid infrared is reported. The sensor is based on an external-cavity quantum cascade laser (EC-QCL) tunable between 7.6 and 8.3 µm wavelengths coupled into a single-mode hollow-core waveguide. Quartz-enhanced photoacoustic spectroscopy has been selected as detecting technique. The fiber coupling system converts the astigmatic beam exiting the laser into a TEM(00) mode. During a full laser scan, we observed no misalignment between the optical beam and the tuning fork, thus making our system applicable for multi-gas or broad absorber detections. The sensor has been tested on N2:H2S gas mixtures. The minimum detectable H2S concentration is 450 ppb in ~3 s integration time, which is the best value till now reported in literature for H2S optical sensors.

High-sensitivity ring-down evanescent-wave sensing in fiber resonators.

We report on optical-fiber cavity ring-down spectroscopy (CRDS) in the liquid phase using a laser emitting at telecommunication wavelengths. A fiber-ring cavity, comprising a short evanescent-wave coupler for radiation-matter interaction, is used as a sensor while its resonance modes are frequency locked to the laser. Exploiting the intrinsic sensitivity and noise immunity of the CRDS technique, we show that liquid absorption can be detected down to a level that is nearly a factor of 20 above the shot noise limit. We provide a thorough comparison between the experimental results and various noise contributions and address different expressions that can be used to calculate the shot noise equivalent absorbance. As a proof of principle, polyamine detection in aqueous solutions is carried out demonstrating a minimum detectable absorbance of 1.8×10(-7) Hz(-1/2), which, to our knowledge, is the best sensitivity limit reported to date for evanescent-wave sensors.

Mid-infrared digital holography and holographic interferometry with a tunable quantum cascade laser.

Mid-infrared digital holography based on CO2 lasers has proven to be a powerful coherent imaging technique due to reduced sensitivity to mechanical vibrations, increased field of view, high optical power, and possible vision through scattering media, e.g., smoke. Here we demonstrate a similar and more compact holographic system based on an external cavity quantum cascade laser emitting at 8 µm. Such a setup, which includes a highly sensitive microbolometric camera, allows the acquisition of speckle holograms of scattering objects, which can be processed in real time. In addition, by exploiting the broad laser tunability, we can acquire holograms at different wavelengths, from which we extract phase images not subjected to phase wrapping, at synthetic wavelengths ranging from hundreds of micrometers to several millimeters.

Mid-infrared frequency comb for broadband high precision and sensitivity molecular spectroscopy.

We report on the experimental demonstration of the metrological and spectroscopic performances of a mid-infrared comb generated by a nonlinear downconversion process from a Ti:sapphire-based near-infrared comb. A quantum cascade laser at 4330 nm was phase-locked to a single tooth of this mid-infrared comb and its frequency-noise power spectral density was measured. The mid-infrared comb itself was also used as a multifrequency highly coherent source to perform ambient air direct comb spectroscopy with the Vernier technique, by demultiplexing it with a high-finesse Fabry-Perot cavity.

Two-tone frequency-modulation spectroscopy in off-axis cavity.

As opposed to a conventional optical resonator, an off-axis-aligned cavity is able to transmit without distortion radiation modulated at a frequency even far above the cavity bandpass. This allows us to implement a simple spectroscopic technique that combines the cavity path-length enhancement of integrated cavity output spectroscopy (ICOS) and the noise reduction associated with radio-frequency modulation (FM). An FM-ICOS spectrometer is demonstrated for the first time using a two-tone modulation technique. The performance is compared to the traditional ICOS by examining the acetylene absorption at 1543.77 nm. A signal-to-noise ratio improvement by a factor 3.5 is found with our proof-of-concept setup. Larger improvements are expected in a more optimized setup.

Surface plasmon resonance optical cavity enhanced refractive index sensing.

We report on a method for surface plasmon resonance (SPR) refractive index sensing based on direct time-domain measurements. An optical resonator is built around an SPR sensor, and its photon lifetime is measured as a function of loss induced by refractive index variations. The method does not rely on any spectroscopic analysis or direct intensity measurement. Time-domain measurements are practically immune to light intensity fluctuations and thus lead to high resolution. A proof of concept experiment is carried out in which a sensor response to liquid samples of different refractive indices is measured. A refractive index resolution of the current system, extrapolated from the reproducibility of cavity-decay time determinations over 133 s, is found to be about 10(-5) RIU. The possibility of long-term averaging suggests that measurements with a resolution better than 10(-7) RIU/√Hz are within reach.

Investigating the resonance spectrum of optical frequency combs in fiber-optic cavities.

We report a detailed theoretical and experimental study of fiber-optic cavities under broadband excitation by mode-locked laser combs. We calculate the effects of fiber dispersion on the cavity transmission. For any integer ratio between the comb repetition rate and cavity free spectral range, the theoretical resonant output spectrum exhibits a narrow group of resonant teeth, surrounded by minor, unevenly spaced resonances. Also, the central resonance can be rapidly and precisely tuned over the entire comb span by only acting on its repetition rate. Experimental observations are provided by a single-mode fiber ring and a telecom-wavelength comb laser. The resulting spectral pattern agrees very well with our theoretical prediction, allowing a thorough characterization of the cavity dispersion and opening new perspectives for comb spectroscopy in dielectric resonators.

High-coherence mid-infrared frequency comb.

We report on the generation of a frequency comb around 4330 nm with an unprecedented coherence of the single teeth. Generating the comb within a Ti:sapphire laser cavity by a difference-frequency process and using a phase-lock scheme based on direct digital synthesis, we achieve a tooth linewidth of 2.0 kHz in a 1-s timescale (750 Hz in 20 ms). The generated per-tooth power of 1 µW ranks this comb among the best ever realized in the mid-infrared in terms of power spectral density.