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X-ray free-electron lasers are sources of coherent, high-intensity X-rays with numerous applications in ultra-fast measurements and dynamic structural imaging. Due to the stochastic nature of the self-amplified spontaneous emission process and the difficulty in controlling injection of electrons, output pulses exhibit significant noise and limited temporal coherence. Standard measurement techniques used for characterizing two-coloured X-ray pulses are challenging, as they are either invasive or diagnostically expensive. In this work, we employ machine learning methods such as neural networks and decision trees to predict the central photon energies of pairs of attosecond fundamental and second harmonic pulses using parameters that are easily recorded at the high-repetition rate of a single shot. Using real experimental data, we apply a detailed feature analysis on the input parameters while optimizing the training time of the machine learning methods. Our predictive models are able to make predictions of central photon energy for one of the pulses without measuring the other pulse, thereby leveraging the use of the spectrometer without having to extend its detection window. We anticipate applications in X-ray spectroscopy using XFELs, such as in time-resolved X-ray absorption and photoemission spectroscopy, where improved measurement of input spectra will lead to better experimental outcomes., Comment: 14 pages, 8 figures

The pulse intensity from X-ray free-electron lasers (FELs) can create extreme excitation densities in solids, entering the regime of non-linear X-ray-matter interactions. We show L3-edge absorption spectra of metallic nickel thin films with fluences entering a regime where several X-ray photons are incident per absorption cross-section. Main features of the observed non-linear spectral changes are described with a predictive rate model for electron population dynamics during the pulse, utilizing a fixed density of states and tabulated ground-state properties., Comment: The main text contains 5 pages and 4 figures, the total length including supplement is 14 pages, 7 figures and one table. See also the simultaneously submitted paper about the rate model

The observation of non-perturbative harmonic emission in solids from ultrashort laser pulses [1] sparked a wave of studies [2,3] as a probe of charge carrier dynamics in solids under strong fields and a route to extreme ultraviolet (XUV) attosecond photonic devices [4]. High harmonic generation (HHG) in liquids [5,6] is far less explored, despite their relevance to biological media, and the mechanism is hotly debated. Using few-cycle pulses below the breakdown threshold, we demonstrate HHG in alcohol with data showing carrier-envelope-phase-dependent XUV spectra extending to 50 eV from isopropanol. We study the mechanism of the harmonic emission through its dependence on the driving field and find it to be consistent with a strong-field recombination mechanism. This maps emitted photon energy to the electron trajectories. We explore the role of the liquid environment in scattering the trajectories and find evidence that information on electron scattering from neighbouring molecules is encoded in the harmonic spectra. Using simulations we exploit this to estimate the scattering cross section and we confirm that the cross-section in liquid isopropanol is significantly reduced compared to vapour. Our findings suggest an \textit{in situ} measurement strategy for retrieving accurate values of scattering cross sections in liquids, and also a pathway to liquid-based attosecond XUV devices., Comment: 12 pages, 4 figures

The dissociation dynamics of the $\tilde{A}$-state of ammonia have been studied using a resonant multiphoton ionisation probe in a photoelectron spectroscopy experiment. The use of a resonant intermediate in the multiphoton ionisation process changes the ionisation propensity, allowing access to different ion states when compared with equivalent single photon ionisation experiments. Ionisation through the $E'$ $^1$A$_1'$ Rydberg intermediate means we maintain overlap with the ion state for an extended period allowing us to monitor the excited state population for several hundred femtoseconds. The vibrational states in the photoelectron spectrum show two distinct timescales, 200 fs and 320 fs, that we assign to the non-adiabatic and adiabatic dissociation processes respectively. The different timescales derive from differences in the wavepacket trajectories for the two dissociation pathways that resonantly excite different vibrational states in the intermediate Rydberg state. The timescales are similar to those obtained from time resolved ion kinetic energy release measurements, suggesting we can measure the different trajectories taken out to the region of conical intersection.

New ab-initio surface hopping simulations of the excited state dynamics of CS$_2$ including spin-orbit coupling are compared to new experimental measurements using a multiphoton ionisation probe in a photoelectron spectroscopy experiment. The calculations highlight the importance of the triplet states even in the very early time dynamics of the dissociation process and allow us to unravel the signatures in the experimental spectrum, linking the observed changes to both electronic and nuclear degrees of freedom within the molecule.

The electronic structure of two-dimensional (2D) semiconductors can be significantly altered by screening effects, either from free charge carriers in the material itself, or by environmental screening from the surrounding medium. The physical properties of 2D semiconductors placed in a heterostructure with other 2D materials are therefore governed by a complex interplay of both intra- and inter-layer interactions. Here, using time- and angle-resolved photoemission, we are able to isolate both the layer-resolved band structure and, more importantly, the transient band structure evolution of a model 2D heterostructure formed of a single layer of MoS$_2$ on graphene. Our results reveal a pronounced renormalization of the quasiparticle gap of the MoS$_2$ layer. Following optical excitation, the band gap is reduced by up to $\sim\!$400 meV on femtosecond timescales due to a persistence of strong electronic interactions despite the environmental screening by the $n$-doped graphene. This points to a large degree of tuneability of both the electronic structure and electron dynamics for 2D semiconductors embedded in a van der Waals-bonded heterostructure., Comment: 22 pages, 5 figures, Published in ACS Nano 2016

The dynamics of excited electrons and holes in single layer (SL) MoS$_2$ have so far been difficult to disentangle from the excitons that dominate the optical response of this material. Here, we use time- and angle-resolved photoemission spectroscopy for a SL of MoS$_2$ on a metallic substrate to directly measure the excited free carriers. This allows us to ascertain a direct quasiparticle band gap of 1.95 eV and determine an ultrafast (50 fs) extraction of excited free carriers via the metal in contact with the SL MoS$_2$. This process is of key importance for optoelectronic applications that rely on separated free carriers rather than excitons., Comment: 15 pages, 4 Figures. To appear in Nano Letters, 2015