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Register a new userDetecting mid-infrared light by molecular frequency upconversion with dual-wavelength hybrid nanoantennas
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Coherent interconversion of signals between optical and mechanical domains is enabled by optomechanical interactions. Extreme light-matter coupling produced by confining light to nanoscale mode volumes can then access single mid-infrared (MIR) photon sensitivity. Here we utilise the infrared absorption and Raman activity of molecular vibrations in plasmonic nanocavities to demonstrate frequency upconversion. We convert {lambda}~10 {mu}m incoming light to visible via surface-enhanced Raman scattering (SERS) in doubly-resonant antennas that enhance upconversion by >10^10. We show >200% amplification of the SERS antiStokes emission when a MIR pump is tuned to a molecular vibrational frequency, obtaining lowest detectable powers ~1 {mu}W/{mu}m^2 at room temperature. These results have potential for low-cost and large-scale infrared detectors and spectroscopic techniques, and bring single-molecule sensing into the infrared
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Frequency upconversion is a cornerstone of electromagnetic signal processing, analysis and detection. It is used to transfer energy and information from one frequency domain to another where transmission, modulation or detection is technically easier or more efficient. Optomechanical transduction is emerging as a flexible approach to coherent frequency upconversion; it has been successfully demonstrated for conversion from radio- and microwaves (kHz to GHz) to optical fields. Nevertheless, optomechanical transduction of multi-THz and mid-infrared signals remains an open challenge. Here, we utilize molecular cavity optomechanics to demonstrate upconversion of sub-microwatt continuous-wave signals at $sim$32~THz into the visible domain at ambient conditions. The device consists in a plasmonic nanocavity hosting a small number of molecules. The incoming field resonantly drives a collective molecular vibration, which imprints an optomechanical modulation on a visible pump laser and results in Stokes and anti-Stokes upconverted Raman sidebands with sub-natural linewidth, indicating a coherent process. The nanocavity offers 13 orders of magnitude enhancement of upconversion efficiency per molecule compared to free space, with a measured phonon-to-photon internal conversion efficiency larger than $10^{-4}$ per milliwatt of pump power. Our results establish a flexible paradigm for optomechanical frequency conversion using molecular oscillators coupled to plasmonic nanocavities, whose vibrational and electromagnetic properties can be tailored at will using chemical engineering and nanofabrication.
Mid-infrared light scatters much less than shorter wavelengths, allowing greatly enhanced penetration depths for optical imaging techniques such as optical coherence tomography (OCT). However, both detection and broadband sources in the mid-IR are technologically challenging. Interfering entangled photons in a nonlinear interferometer enables sensing with undetected photons making mid-IR sources and detectors obsolete. Here we implement mid-infrared frequency-domain OCT based on ultra-broadband entangled photon pairs. We demonstrate 10 ${mu}$m axial and 20 ${mu}$m lateral resolution 2D and 3D imaging of strongly scattering ceramic and paint samples. Together with $10^6$ times less noise scaled for the same amount of probe light and also vastly reduced footprint and technical complexity this technique can outperform conventional approaches with classical mid-IR light.
We present a new method for accurate mid-infrared frequency measurements and stabilization to a near-infrared ultra-stable frequency reference, transmitted with a long-distance fibre link and continuously monitored against state-of-the-art atomic fountain clocks. As a first application, we measure the frequency of an OsO4 rovibrational molecular line around 10 $mu$m with a state-of-the-art uncertainty of 8x10-13. We also demonstrate the frequency stabilization of a mid-infrared laser with fractional stability better than 4x10-14 at 1 s averaging time and a line-width below 17 Hz. This new stabilization scheme gives us the ability to transfer frequency stability in the range of 10-15 or even better, currently accessible in the near-infrared or in the visible, to mid-infrared lasers in a wide frequency range.
We designed and simulated freestanding dielectric optical metasurfaces based on arrays of etched nanoholes in a silicon membrane. We showed $2pi$ phase control and high forward transmission at mid-infrared wavelengths by tuning the dimensions of the holes. We also identified the mechanisms responsible for high forward scattering efficiency and showed that these conditions are connected with the well-known Kerker conditions already proposed for isolated scatterers. A beam deflector was designed and optimized through sequential particle swarm and gradient descent optimization to maximize transmission efficiency and reduce unwanted grating orders. Such freestanding silicon nanohole array metasurfaces are promising for the realization of silicon based mid-infrared optical elements.
A guided-wave chip laser operating in a single longitudinal mode at 2860 nm is presented. The cavity was set in the Littman-Metcalf configuration to achieve single-frequency operation with a side-mode suppression ratio above 33 dB. The chip lasers linewidth was found to be limited by mechanical fluctuations, but its Lorentzian contribution was estimated to be lower than 1 Hz using a heterodyne technique. This demonstration incorporates a high coherence source with the simplicity provided by the compactness of chip lasers.
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