xiv, 138 p. : ill. (some col.) / In this dissertation, we demonstrate the generation of optical Raman frequency combs by a single laser pump pulse traveling in hydrogen-filled hollow-core optical fibers. This comb generation process is a cascaded stimulated Raman scattering effect, where higher-order sidebands are produced by lower orders scattered from hydrogen molecules. We observe more than 4 vibrational and 20 rotational Raman sidebands in the comb. They span more than three octaves in optical wavelength, largely thanks to the broadband transmission property of the fiber. We found that there are phase correlations between the generated Raman comb sidebands (spectral lines), although their phases are fluctuating from one pump pulse to another due to the inherit spontaneous initiation of Raman scattering. In the experiment, we generated two Raman combs independently from two fibers and simultaneously observed the single-shot interferences between Stokes and anti-Stokes components from the two fibers. The experimental results clearly showed the strong phase anti-correlation between first-order side bands. We also developed a quantum theory to describe this Raman comb generation process, and it predicts and explains the phase correlations we observe. The phase correlation that we found in optical Raman combs may allow us to synthesize single-cycle optical pulse trains, creating attosecond pulses. However, the vacuum fluctuation in stimulated Raman scattering will result in the fluctuation of carrier envelope phase of the pulse trains. We propose that we can stabilize the comb by simultaneously injecting an auxiliary optical beam, mutually coherent with the main Raman pump laser pulse, which is resonant with the third anti-Stokes field. / Committee in Charge: Dr. Steven van Enk, Chair; Dr. Michael G. Raymer; Dr. Daniel A. Steck; Dr. David M. Strom; Dr. Andrew H. Marcus

Les lasers à fibre de haute puissance constituent depuis une dizaine d’année un outil pertinent pour un nombre croissant d’applications. Dans le cadre d’un contrat CIFRE entre la société Eolite Systems et le laboratoire Xlim (UMR 7252 du CNRS et de l’Université de Limoges), mon projet de thèse a consisté à développer les briques technologiques de futures sources lasers / High-power fiber lasers adress an increasing number of applications since ten years. In the frame of a CIFRE contract between the company Eolite Systems and Xlim (joint laboratory between CNRS and the University of Limoges), the goal of this PhD project was to develop the technological blocs to achieve all-fibre high-power lasers emiting out of the conventional spectral band covered by existing lasers.Modal instabilities in large mode area (LMA) fibers are currently the main limitation of the fiber lasers power scaling. We have experimentally demonstrated the relevance of inner cladding aperiodic structures to efficiently delocalize higher order modes outside the gain region. A systematic study of passive fibers based on such structures has shown the single propagation of the fundamental mode over a wide wavelength range from 1 to 2 µm for dimension of core up to 85 µm. This effective mode delocalization even extends up to a core dimension of 140 µm at a 2 µm wavelength.The combination of high power picosecond fiber laser with an average power of 22.7 W and a hydrogen-filled inhibited coupling Kagome fiber allowed us to generate two Raman combs over five frequency octaves from 321 nm to 12.5 µm. These two combs are controlled by the laser pump polarization and generated an average power of 10.1 W displayed over 70 laser lines for circular pump polarization and 8.6 W over 30 lines for linear polarization. Some laser lines within these combs have been generated for the first time from high-power fiber source in the mid-infrared range. We have also demonstrated the generation of high-power line by optimizing the first vibrational Stokes at 1.8 µm with an average power of 9.3 W and a quantum efficiency of the frequency conversion stage close to 80%.