Third harmonic generation in liquid core optical fibres

The objective of this thesis is to investigate third harmonic generation in liquid core fibres. Such fibres are formed by injection of liquid into a hollow, solid cladding by capillary forces. Carbon disulphide and tetrachloroethylene are identified as most promising liquid candidates. Such liquids offer a strong nonlinearity whose major contribution is non-instantaneous arising from the molecular structure. The effect of this material response during harmonic generation is investigated numerically by solving coupled evolution equations and causes distinct spectral shifts and broadening of both harmonic and fundamental wave. Both liquids offer excellent transparency and a high index of refraction enabling intermodal phase matching in a step-index geometry without requiring a complex microstructure. Aspects of fibre design and experimental realisation are presented in detail. Using sub-picosecond pump pulses of different duration the harmonic is generated in a higher order fibre mode and resulting signals are analysed in the spectral domain. Modification of the fibre cross-section towards an elliptical core is investigated. Besides the induced birefringence, harmonic generation in further sets of higher order modes is possible due to their transformation of electric fields. Design considerations of spatially modified fibres were confirmed experimentally and adaptive phase matching by controlling fibre temperature could be realised. Feasibility of long term exposure of liquid filled fibres to high average powers of femtosecond pulses is demonstrated underpinning that liquid core fibres withstand practical applications beyond laboratory use. Finally, possible routes to enhance the currently achieved conversion efficiencies for tetrachloroethylen of 2 ∙ 10^-5, and carbon disulphide of 10^-7, are identified and future prospects of this fibre platform are discussed.