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We report a study of high-order multi-photon absorption, nonlinear refraction, and their anisotropy in four notable mid-infrared \c{hi}(2) crystals: GaP, ZnSe, GaSe and ZGP using the Z- scan method and 2.35-{\mu}m femtosecond pulses with peak intensity in excess of 200 GW/cm2. We found that the nonlinear absorption obeys a perturbation model with multi-photon absorption (MPA) orders from N = 4 to 6, in good agreement with the bandgaps of the crystals. A study of the role of free carrier absorption, performed by varying the pulse duration between 30 and 70 fs while maintaining a constant peak intensity showed that at our intensity levels, free carriers generated in the process of MPA absorb much stronger than would be expected from their linear absorption cross section. Possible mechanisms include high-field effects, such as intra-valley scattering in the conduction band and absorption to higher lying bands. Nonlinear refractive indices were measured using (i) closed aperture Z-scan and (ii) spectral broadening due to self-phase modulation, both methods agreeing well with each other., Comment: 10 pages, 5 figures, 3 tables

Mid-infrared (mid-IR) spectroscopy offers unparalleled sensitivity for the detection of trace gases, solids and liquids, which is based on the existence of strong telltale vibrational bands in this part of the spectrum. It was shown more than a decade ago that a dual-comb Fourier spectroscopy could provide superior spectral coverage combined with high resolution and extremely fast data acquisition. Capabilities of this method were limited because of difficulty of producing twins of mutually coherent frequency combs in the mid- IR. Here we report a phase-coherent and broadband dual-comb system that is based on a pair of subharmonic (frequency-divide-by-two) optical parametric oscillators, pumped in turn by two phase-locked thulium fiber lasers at 2-micron wavelength. We demonstrate simultaneous detection of multiple molecular species in the whole band of 3.2-5.3 microns (frequency span 1200 cm^{-1}) augmented by the pump laser band of 1.85-2 microns (span 400 cm^{-1}), with spectral resolution 0.01-0.07 cm^{-1} and acquisition speed of up to 160,000 resolution elements in few seconds., Comment: 9 pages, 4 figures

Ultrasensitive detection of methane, isotopic carbon dioxide, carbon monoxide, formaldehyde, acetylene and ethylene is performed in the spectral range 2.5 - 5 \mu m using intracavity spectroscopy in broadband optical parametric oscillators (OPOs). The OPOs were operated near degeneracy and synchronously pumped either by a mode-locked erbium (1560 nm) or thulium (2050 nm) fiber laser. A large instantaneous bandwidth of up to 800 cm$^{-1}$ allows for simultaneous detection of several gases. We observe an effective path length enhancement due to coherent interaction inside the OPO cavity and achieve part-per-billion sensitivity levels. The measured spectral shapes are in good agreement with a model that takes into account group delay dispersion across the broad OPO frequency band., Comment: 25 pages, 17 figures

We demonstrate mid-infrared (mid-IR) supercontinuum generation (SCG) with instantaneous bandwidth from 2.2 to 5 {\mu}m at 40 dB below the peak, covering the wavelength range desirable for molecular spectroscopy and numerous other applications. The SCG occurs in a tapered As2S3 fiber prepared by in-situ tapering and is pumped by femtosecond pulses from the subharmonic of a mode-locked Er-doped fiber laser. Interference with a narrow linewidth c.w. laser verifies that the coherence properties of the near-IR frequency comb have been preserved through these cascaded nonlinear processes. With this approach stable broad mid-IR frequency combs can be derived from commercially available near-IR frequency combs without an extra stabilization mechanism.

True random number generators (RNGs) are desirable for applications ranging from cryptogra- phy to computer simulations. Quantum phenomena prove to be attractive for physical RNGs due to their fundamental randomness and immunity to attack [1]- [5]. Optical parametric down conversion is an essential element in most quantum optical experiments including optical squeezing [9], and generation of entangled photons [10]. In an optical parametric oscillator (OPO), photons generated through spontaneous down conversion of the pump initiate the oscillation in the absence of other inputs [11, 12]. This quantum process is the dominant effect during the oscillation build-up, leading to selection of one of the two possible phase states above threshold in a degenerate OPO [13]. Building on this, we demonstrate a novel all-optical quantum RNG in which the photodetection is not a part of the random process, and no post processing is required for the generated bit sequence. We implement a synchronously pumped twin degenerate OPO, which comprises two identical independent OPOs in a single cavity, and measure the relative phase states of the OPO outputs above threshold as a bit value. We show that the outcome is statistically random with 99% confidence. With the use of micro- and nanoscale OPO resonators, this technique offers a promise for simple, robust, and high-speed on-chip all-optical quantum random number generators.