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.
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 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.
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.
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.
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.
In this thesis I study coherent light-matter interactions via stimulated Raman scattering (SRS) in a gas-filled hollow-core photonic crystal fiber (HC-PCF).The HC-PCF constitutes the foundation of the experimental results presented in this thesis, as without its unique properties realization of these experiments would not have been possible.These unique properties include tight confinement of laser light and matter in the small core of the fiber, which leads to extremely high conversion efficiencies in the SRS, and spectral filtering of unwanted nonlinear waves.This setup creates a clean system of two optical fields interacting via Raman medium inside the core of the fiber.This thesis consists of three parts.The first part (chapter 2) includes a general overview of the different types of HC-PCF, their fabrication techniques and guidance mechanisms.Two types of HC-PCF are considered: photonic bandgap HC-PCF and kagomé-HC-PCF.Guidance mechanisms of these two types of fibers are considered in detail.Of particular interest to me is the broadband guidance in kagomé-HC-PCF.Up to now, the mechanism responsible for this broadband guidance is not understood.A simplified semi-analytical model is derived which accounts for this broadband guidance in kagomé-HC-PCF and explain many of its guidance properties.In particular, using the model, the fiber loss as a function of wavelength is reproduced fairly well.The model also explains an important feature of kagomé-HC-PCF, namely, the insensitivity of its loss to the number of cladding layers.In the second part of the thesis (chapter 3), I set the basic theoretical formalism of SRS to be used in the rest of the thesis.The aim of the chapter is to derive the coupled wave equations that govern the evolution of the pump, Stokes and coherence fields using classical as well as semi-classical approaches.The third part of the thesis (chapters 4, 5, 6 and 7) discusses the results of experimental and theoretical investigations of my studies on SRS in gas-filled HC-PCF.I start with an overview of the already know results about SRS in HC-PCF and explain the mechanism of phase-locking for efficient generation of anti-Stokes SRS.This work clarifies high conversion efficiencies to anti-Stokes frequencies observed in early experiments.Most of these early experiments are focused on lowering the threshold for SRS generation and are done at relatively high pressures.In chapters 5 and 6, I use some of the unique properties of the HC-PCF to explore the coherent light-matter SRS interaction regimes not previously accessible.This includes the first experimental observation of backward superluminal solitary waves and self-similar solutions of SRS coupled-wave equations.These results represent a significant advance in the study of coherent effects and point to a new generation of highly engineerable gas cells for studying complex nonlinear phenomena.In chapter 7, I briefly overview the results presented in previous chapters and conclude my thesis by explaining possible improvements as well as new interesting directions in studying coherent light-matter interactions in gas-filled HC-PCF.In particular, I introduce a simple scheme for generating (purely rotational) broadband coherent frequency comb at low pump pulse energies using a gas-filled HC-PCF.Generation of such a frequency comb is quite interesting for synthesizing ultrashort pulses as well as a broad coherent tunable light source with high spectral brightness.The classic system of education is mainly based on the ability of deductive reasoning and knowledge of the classics.Quite often, in the course of learning that, we lose the joy and excitement of thinking.Scientific research, on the other hand, is not just about knowing and reasoning, but also thinking, creativity and courage of realizing new ideas.For that, I am hugely indebted to my supervisor, Prof. Philip Russell.Philip, thank you for teaching me the divergent way of thinking, to see many solutions to one problem, for giving me the courage to express my ideas and for providing excellent facilities and environment to realize them.I would also like to thank Prof. Curtis Menyuk for very nice discussions and comments about my thesis and specially the work he has done on self-similarity.Your deep insight and understanding of the physics and the beauty of mathematics behind it, is truly amazing and I really hope that in future I would have the opportunity to learn more from you.Many thanks go to Dr. Johannes Nold for who he is and