Ultra-broadband high-resolution microdroplet spectrometers for the near infrared.

By stabilizing the evaporation dynamics of a microliter fluorocarbon droplet, we demonstrate a fast-scan optofluidic Fourier transform (FT) spectrometer on the tip of an optical fiber operating in the 1000-2000 nm window with a resolution of 3.5 cm-1 (i.e., <1 nm at 1560 nm). Compared with other FT near-infrared (NIR) small-scale spectrometers reported in the literature, the fluorocarbon droplet spectrometer shows the largest wavelength span and span/resolution ratio, allowing spectral analysis of broadband or narrowband radiation to be easily performed. Our results open the way for the practical application of droplet spectrometers as advanced optofluidic NIR analyzers with small size and low cost that are capable of operating in harsh environments, even in the absence of electrical power sources.

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.

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.

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.

Mode-splitting cloning in birefringent fiber Bragg grating ring resonators.

In this Letter, we report the theoretical model and the experimental evidence of a mode-splitting cloning effect due to the resonant coupling between modes having different polarizations in weakly birefringent fiber Bragg grating (FBG) ring resonators. This modal coupling depends on the fiber birefringence and the FBG reflectivity. In the ideal case of the absence of birefringence, a single split-mode resonant structure can be observed in the resonator transmission spectrum due to the degeneracy removal of the two counter-propagating modes. In the presence of FBG birefringence, a secondary split doublet resulting in a clone of the initial one is generated. The described effect can be exploited for spectroscopic-sensing applications based on more complex split-mode dynamics.

Fiber Bragg grating laser sensor with direct radio-frequency readout.

A fiber Bragg grating (FBG)-coupled ring laser sensor is demonstrated. In the proposed configuration the interrogating source, the sensing head and the readout instrument are integrated in a single fiber-optic device. An FBG inserted within a bidirectional fiber ring couples the two counterpropagating modes of the cavity, generating a splitting of the resonant wavelengths proportional to the FBG reflectivity. When the cavity gain is brought beyond threshold, the two peaks of the split resonances simultaneously lase, leading to a beat note in the emission spectrum whose frequency tracks any small shift of the FBG reflectivity spectrum. Such a beat note can be simply monitored by a frequency counter, without the need for an optical spectrometer, allowing to significantly reduce size and costs of the sensor setup. The sensing performance compares well to the state-of-the-art thermo-mechanical fiber sensors.

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.

Enhanced spectral response of π-phase shifted fiber Bragg gratings in closed-loop configuration.

The transmission spectrum of a ring resonator enclosing a π-phase shifted fiber Bragg grating (π-FBG) shows a spectral feature at the Bragg wavelength that is much sharper than resonance of the π-FBG alone, and that can be detected with a simple integrated cavity output technique. Hence, the resolution of any sensor based on the fitting of the π-FBG spectral profile can be largely improved by the proposed configuration at no additional fabrication costs and without altering the sensor robustness. A theoretical model shows that the resolution enhancement attainable in the proposed closed-loop geometry depends on the quality factor of the ring resonator. With a commercial grating in a medium-finesse ring, a spectral feature 12 times sharper than the π-FBG resonance is experimentally demonstrated. A larger enhancement is expected in a low-loss, polarization maintaining setup.

Split-mode fiber Bragg grating sensor for high-resolution static strain measurements.

We demonstrate a strain sensor with very high sensitivity in the static and low frequency regime based on a fiber ring cavity that includes a π phase-shifted fiber Bragg grating. The grating acts as a partial reflector that couples the two counter-propagating cavity modes, generating a splitting of the resonant frequencies. The presence of a sharp transition within the π phase-shifted fiber Bragg grating's spectral transmittance makes this frequency splitting extremely sensitive to length, temperature, and the refractive index of the fiber in the region where the grating is written. The splitting variations caused by small mechanical deformations of the grating are tracked in real time by interrogating a cavity resonance with a locked-carrier scanning-sideband technique. The measurable strain range and bandwidth are characterized, and a resolution of 320 pϵ/Hz(1/2) at 0 Hz is experimentally demonstrated, the highest achieved to date with a fiber Bragg grating sensor.

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.

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.

Localized strain sensing with fiber Bragg-grating ring cavities.

We report the theoretical description and the experimental demonstration of an optical resonator formed by inserting a Fiber Bragg Grating (FBG) in a closed fiber loop. The spectral characteristics of such a resonator strongly depend on the reflectivity of the FBG. In the wavelength region where the FBG reflectivity R is negligible, the system behaves like a conventional ring resonator. On the other hand, when R is not vanishing, a split-mode structure can be observed, associated to the degeneracy removal of two counterpropagating resonant modes. The magnitude of the mode splitting can be used to sense small variations of the FBG physical parameters, such as length, temperature or group index. An example of strain sensing with this setup is reported, showing that the mode splitting is sensitive to a mechanical strain applied to the FBG, while it is almost insensitive to a strain applied to any other point of the resonator. This peculiar feature allows to perform cavity-enhanced, local strain measurements with a reduced sensitivity to environmental perturbations, which represents an important improvement in the framework of the fiber-optic sensors.

Absolute measurement of the S(0) and S(1) lines in the electric quadrupole fundamental band of D(2) around 3µm.

The electric quadrupole fundamental (v=1←0) band of molecular deuterium around 3 µm is accessed by cavity ring-down spectroscopy using a difference-frequency-generation source linked to the Cs-clock primary standard via an optical frequency comb synthesizer. An absolute determination of the line position and strength is reported for the first two transitions (J=2←0 and J=3←1) of the S branch. An accuracy of 6×10(-8) is achieved for the line-center frequencies, which improves by a factor 20 previous experimental results [A. R. W. McKellar and T. Oka, Can. J. Phys. 56, 1315 (1978)]. The line strength values, measured with 1% accuracy, are used to retrieve the quadrupole moment matrix elements which are found in good agreement with previous theoretical calculations [A. Birnbaum and J. D. Poll, J. Atmos. Sci. 26, 943 (1969); J. L. Hunt, J. D. Poll, and L. Wolniewicz, Can. J. Phys. 62, 1719 (1984)].

Non-collinear quasi phase matching and annular profiles in difference frequency generation with focused Gaussian beams.

We present and experimentally test a simple model for difference frequency generation (DFG) in periodically-poled crystals with gaussian pumping beams. Focusing of input beams originates several non-collinear quasi-phase-matching configurations of the interacting wavevectors, which contribute to the idler output field. In this picture, we accurately describe a number of effects, such as the occurrence of annular idler intensity profiles and the asymmetric trend of DFG power vs temperature. Finally, we quantitatively test the model by means of an indirect measurement of the crystal poling period.

Absolute frequency measurement of molecular transitions by a direct link to a comb generated around 3-microm.

A 3-microm continuous-wave difference-frequency source is directly referenced to a mid-infrared optical frequency comb synthesizer by measuring their beat-note signal by a fast HgCdTe detector. Absolute frequency metrology of molecular vibration spectra is demonstrated by locking the 3-microm coherent radiation to the nearest comb tooth and tuning the comb mode spacing across the Doppler-broadened absorption profile of a CH(4) ro-vibrational transition.

Combining a difference-frequency source with an off-axis high-finesse cavity for trace-gas monitoring around 3 microm.

High-sensitivity spectroscopy of methane around 3 microm was carried out by means of a 5.5-mW cw difference-frequency generator in conjunction with a high finesse cavity in off-axis alignment. By cavity-output integration a minimum detectable absorption coefficient of 5.7*10-9 cm-1Hz-1/2 was achieved, which compares well with results already reported in the literature. Detection of methane in natural abundance was also performed in ambient air, for different values of total pressure, allowing direct concentration measurements via evaluation of the integrated absorbance of the spectra. In particular, at atmospheric pressure, a minimum detectable concentration of 850 parts per trillion by volume (pptv)*Hz-1/2 was demonstrated.