This thesis presents how sources of coherent sources extreme ultraviolet (XUV) and soft
X-ray wavelengths can be generated and how these sources may be used to study both the
dynamics and structure of molecular systems.
Developmental work on a beam line designed to generate XUV radiation using high
harmonic generation is presented. In addition to commissioning experimental work using
both a flat-field XUV spectrometer and magnetic bottle electron spectrometer, software
development work towards building a scalable and future proof acquisition framework for
future experiments is presented.
The remainder of the thesis presents results obtained from experiments performed at
the Linac Coherent Light Source (LCLS) X-ray free electron laser (FEL). We demonstrate
that by using a UV femtosecond pulse and a weakly focused X-ray pulse of duration 70
fs, the evolution of UV induced photoisomerisation of 1-3 cyclohexadiene can be tracked.
Over timescales of ≈1 ps after UV excitation, the ion yields of the H+ and C+ species were
observed to increase by 10% and the observed kinetic energy of all fragments is observed
to increase over the same time scale, which can be explained by the structural change of
the molecule into the hexatriene isomers.
There has been a recent focus in FEL science in using tightly focused X-rays to generate
so called hollow atoms, with a completely empty inner shell. Study of the products of the
creation of these states ideally requires a measurement in coincidence of multiple particles.
We demonstrate that by using the technique of partial covariance mapping (PCM) in
conjunction with a high efficiency electron time-of-flight spectrometer, multiple processes
in the core ionisation of neon can be resolved. We also use the scheme to successfully
measure single site double-core hole states in the hydrocarbons of acetylene and ethane.
We discuss how this technique will be a powerful tool in future experiments designed for
chemical analysis of the core hole states of systems.