| Summary: | The generation of few-cycle pulses at near-infrared wavelengths is now a robust technology, as is their application to the efficient production of high-order harmonics in the extreme ultraviolet region with temporal confinement to hundreds of attoseconds. Recent years have seen considerable efforts directed to the study of electron dynamics in complex molecules in real time, with relevance to processes such as photosynthesis and radiation damage of proteins and DNA. This work describes the development of new and unique sources suited for the study of such dynamics, together with novel instrumentation and experimental methodology. This includes a pair of synchronised attosecond pulses at different photon energies in the VUV and XUV regions, which we have generated via high harmonic generation from a few-cycle NIR source and characterised with attosecond streaking. We have also explored the possibilities of sub-cycle control of these attosecond pulses by adding a second harmonic field to the high- harmonic generation process, and simultaneously characterised this second harmonic field with a novel characterisation technique known as ARIES, capable of waveform sampling at arbitrary optical wavelengths. In parallel, we have developed a few-cycle short-wavelength IR source for a UK user facility, to take advantage of the favourable wavelength scaling of the maximum photon energy achievable via high-harmonic generation. Using a commercial optical parametric amplifier and a hollow-core fibre compression system, we have generated sub-2-cycle pulses at 1750 nm, characterised via third-harmonic autocorrelation and a novel implementation of the dispersion scan technique. We have commissioned a beamline for attosecond pump-probe studies in the gas phase, including a purpose-built dual spectrometer with capabilities for simultaneous measurement of mass spectra of ions and velocity-map imaging of electrons. We have performed initial VUV-NIR pump-probe experiments on a small organic molecule, namely isopropanol, and identified a time- dependent signature as an IR-induced coupling. Finally, we have considered perspectives for future studies in attosecond pump-probe experiments with the demonstration of a two-VUV-photon process in helium performed with a moderate energy, high repetition rate attosecond source.
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