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arXiv:1508.06501 · Physical Review Letters

Dramatic Raman Gain Suppression in the Vicinity of the Zero Dispersion Point in a Gas-Filled Hollow-Core Photonic Crystal Fiber

S. T. Bauerschmidt, David Novoa, Philip St.J. Russell

Published Dec 11, 2015• 35 citations
arXivHTMLPDF

Abstract

In 1964 Bloembergen and Shen predicted that Raman gain could be suppressed if the rates of phonon creation and annihilation (by inelastic scattering) exactly balance. This is only possible if the momentum required for each process is identical, i.e., phonon coherence waves created by pump-to-Stokes scattering are identical to those annihilated in pump-to-anti-Stokes scattering. In bulk gas cells, this can only be achieved over limited interaction lengths at an oblique angle to the pump axis. Here we report a simple system that provides dramatic Raman gain suppression over long collinear path lengths in hydrogen. It consists of a gas-filled hollow-core photonic crystal fiber whose zero dispersion point is pressure adjusted to lie close to the pump laser wavelength. At a certain precise pressure, stimulated generation of Stokes light in the fundamental mode is completely suppressed, allowing other much weaker phenomena such as spontaneous Raman scattering to be explored at high pump powers.

DOI
10.1103/physrevlett.115.243901

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In 1964 Bloembergen and Shen predicted that Raman gain could be suppressed if the rates of phonon creation and annihilation (by inelastic scattering) exactly balance. This is only possible if the momentum required for each process is identical, i.e., phonon coherence waves created by pump-to-Stokes scattering are identical to those annihilated in pump-to-anti-Stokes scattering. In bulk gas cells, this can only be achieved over limited interaction lengths at an oblique angle to the pump axis. Here we report a simple system that provides dramatic Raman gain suppression over long collinear path lengths in hydrogen. It consists of a gas-filled hollow-core photonic crystal fiber whose zero dispersion point is pressure adjusted to lie close to the pump laser wavelength. At a certain precise pressure, stimulated generation of Stokes light in the fundamental mode is completely suppressed, allowing other much weaker phenomena such as spontaneous Raman scattering to be explored at high pump powers.
Stimulated Raman scattering is coherently suppressed if the rate of phonon creation is exactly balanced by the rate of phonon annihilation, a prediction first made by Bloembergen and Shen in 1964 [1]. Viewed classically, this occurs when the fringe patterns created by the interference of pump-Stokes and pump-anti-Stokes signals cancel each other out. It has been recently shown that gas-filled hollow-core photonic crystal fiber (HC-PCF), pumped in the vicinity of the zero-dispersion point (ZDP), is an ideal vehicle for observing gain suppression. The ultralong path-lengths and the well-controlled dispersion permit dramatic suppression of the effective intramodal Raman gain for the fundamental core mode [2, 3], resulting in strong enhancement of intermodal scattering from the pump to a Stokes signal in a higher-order core mode.
Backward stimulated Raman scattering in gases provides a promising route to compression and amplification of a Stokes seed-pulse by counter-propagating against a pump-pulse, as has been already demonstrated in various platforms, mainly in free-space. However, the dynamics governing this process when seeded by noise has not yet been investigated in a fully controllable collinear environment. Here we report the first unambiguous observation of efficient noise-seeded backward stimulated Raman scattering in a hydrogen-filled hollow-core photonic crystal fiber. At high gas pressures, when the backward Raman gain is comparable with, but lower than, the forward gain, we report quantum conversion efficiencies exceeding 40% to the backward Stokes at 683 nm from a narrowband 532-nm-pump. The efficiency increases to 65% when the backward process is seeded by a small amount of back-reflected forward-generated Stokes light. At high pump powers the backward Stokes signal, emitted in a clean fundamental mode and spectrally pure, is unexpectedly always stronger than its forward-propagating counterpart. We attribute this striking observation to the unique temporal dynamics of the interacting fields, which cause the Raman coherence (which takes the form of a moving fine-period Bragg grating) to grow in strength towards the input end of the fiber. A good understanding of this process, together with the rapid development of novel anti-resonant-guiding hollow-core fibers, may lead to improved designs of efficient gas-based Raman lasers and amplifiers operating at wavelengths from the ultraviolet to the mid-infrared.
Backward stimulated Raman scattering in gases provides a promising route to the compression and amplification of a Stokes seed pulse by counter-propagating against a pump pulse, as has been demonstrated already in various platforms, mainly in free space. However, the dynamics governing this process when seeded by noise has not yet been investigated in a fully controllable collinear environment. Here we report, to the best of our knowledge, the first unambiguous observation of efficient noise-seeded backward stimulated Raman scattering in a hydrogen-filled hollow-core photonic crystal fiber. At high gas pressures, when the backward Raman gain is comparable to, but lower than, the forward gain, we report quantum conversion efficiencies exceeding 40% to the backward Stokes at 683 nm from a narrowband 532 nm pump. Efficiency increases to 65% when the backward process is seeded by a small amount of back-reflected forward-generated Stokes light. At high pump powers, the backward Stokes signal, emitted in a clean fundamental mode and spectrally pure, is unexpectedly always stronger than its forward-propagating counterpart. We attribute this striking observation to the unique temporal dynamics of the interacting fields, which cause the Raman coherence (which takes the form of a moving fine-period Bragg grating) to grow in strength toward the input end of the fiber. A good understanding of this process, together with the rapid development of novel anti-resonant-guiding hollow-core fibers, may lead to improved designs of efficient gas-based Raman lasers and amplifiers operating at wavelengths from the ultraviolet to the mid-infrared.
Stimulated Raman scattering is investigated in a slightly multimode gas-filled hollow-core photonic crystal fiber. Although, second-order Stokes light appears in the fundamental mode below a certain threshold energy, it is observed to switch to a two-lobed higher order mode above this threshold. Conversion to the higher order mode is made possible by the creation of a two-lobed moving coherence wave in the gas that provides both phase-matching and a strong intermodal pump-Stokes overlap. A theoretical model is developed, based on this physical interpretation that agrees quantitatively with the experimental results. The results suggest new opportunities for all-fiber gas-based nonlinear processes requiring phase-matching, such as coherent anti-Stokes Raman scattering, as well as providing a means (for example) of efficiently converting light from a higher order pump mode to a fundamental Stokes mode.
Anti-Stokes Raman scattering in gas-filled hollow-core photonic crystal fibers is discussed. It is shown that the efficient anti-Stokes generation observed under conditions of significant wave mismatch is caused by phase locking of the interacting fields. This leads to the establishment of a phase difference that is independent of the optical path. An optimization technique, based on the adjustment of the wave mismatch along a gas-filled hollow fiber using pressure control, is proposed. Anti-Stokes conversion efficiencies close to the theoretical maximum of 50% are predicted.
Hollow-core photonic-crystal fibers are shown to offer the unique possibility of coherent excitation and probing of Raman-active vibrations in molecules by isolated air-guided modes of electromagnetic radiation. A $3\text{\ensuremath{-}}\mathrm{cm}$ section of a hollow photonic-crystal fiber is used to prepare isolated air-guided modes of pump and probe fields for a coherent excitation of $2331{\text{\ensuremath{-}}\mathrm{cm}}^{\ensuremath{-}1}$ QQQ-branch vibrations of molecular nitrogen in the gas filling the fiber core, enhancing coherent anti-Stokes Raman scattering through these vibrations by a factor of 15 relative to the regime of tight focusing.