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Physical Review A

Coherent anti-Stokes Raman scattering in isolated air-guided modes of a hollow-core photonic-crystal fiber

Andrei B. Fedotov, Stanislav O. Konorov, V. P. Mitrokhin, Evgenii E. Serebryannikov, Aleksei M. Zheltikov

Published Oct 18, 2004• 60 citations
Publisher

Abstract

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 $2331{\text{\ensuremath{-}}\mathrm{cm}}^{\ensuremath{-}1}$ $Q$-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.

DOI
10.1103/physreva.70.045802

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Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)•Jun 1, 2017•0 citations
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\ensuremath-cm3\text{\ensuremath{-}}\mathrm{cm}3\ensuremath-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\ensuremath-cm\ensuremath−12331{\text{\ensuremath{-}}\mathrm{cm}}^{\ensuremath{-}1}2331\ensuremath-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.
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.
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.
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 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.