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X-ray photoelectron spectroscopy (XPS) measures the binding energy of core-level electrons, which are well-localised to specific atomic sites in a molecular system, providing valuable information on the local chemical environment. The technique relies on measuring the photoelectron spectrum upon x-ray photoionisation, and the resolution is often limited by the bandwidth of the ionising x-ray pulse. This is particularly problematic for time-resolved XPS, where the desired time resolution enforces a fundamental lower limit on the bandwidth of the x-ray source. In this work, we report a novel correlation analysis which exploits the correlation between the x-ray and photoelectron spectra to improve the resolution of XPS measurements. We show that with this correlation-based spectral-domain ghost imaging method we can achieve sub-bandwidth resolution in XPS measurements. This analysis method enables XPS for sources with large bandwidth or spectral jitter, previously considered unfeasible for XPS measurements. [ABSTRACT FROM AUTHOR]

Short-wavelength free-electron lasers are now well established as essential and unrivalled sources of ultrabright coherent X-ray radiation. One of the key characteristics of these intense X-ray pulses is their expected few-femtosecond duration. No measurement has succeeded so far in directly determining the temporal structure or even the duration of these ultrashort pulses in the few-femtosecond range. Here, by deploying the so-called streaking spectroscopy technique at the Linac Coherent Light Source, we demonstrate a non-invasive scheme for temporal characterization of X-ray pulses with sub-femtosecond resolution. This method is independent of photon energy, decoupled from machine parameters, and provides an upper bound on the X-ray pulse duration. We measured the duration of the shortest X-ray pulses currently available to be on average no longer than 4.4 fs. Analysing the pulse substructure indicates a small percentage of the free-electron laser pulses consisting of individual high-intensity spikes to be on the order of hundreds of attoseconds. [ABSTRACT FROM AUTHOR]

Kinetic Boltzmann equations are used to describe electron emission spectra obtained after irradiation of noble-gas clusters with intense vacuum ultraviolet (VUV) radiation from a free-electron-laser (FEL). The experimental photoelectron spectra give a complementary and more detailed view of nonlinear processes within atoms and clusters in an intense laser field compared to mass spectroscopy data. Results from our model obtained in this study confirm the experimental and theoretical findings on the differing ionization scenarios at longer (100 nm) and shorter (32 nm) VUV radiation wavelengths. At the wavelength of 100 nm the thermoelectronic electron emission dominates the emission spectra. This indicates the plasma formation and the inverse bremsstrahlung (IB) heating of electrons inside the plasma. This effect is clearly visible for xenon (with the fitted temperature of 6-7 eV), and less visible for argon (with the fitted temperature of 2-3 eV). The two-photon-ionization rate for argon that initiates the cluster ionization, is much lower than the singlephotoionization rate for xenon. Also, more of the photoelectrons created within an argon cluster are able to leave it, as they are more energetic than those released from a xenon cluster. Therefore, the IB heating of plasma electrons in argon is less efficient than in xenon, as the density of the electrons remaining within the cluster is lower. At a wavelength of 32 nm the dominant ionization mechanism identified from the electron spectra of argon clusters is the direct multistep ionization. The signature of the thermalization of electrons is also observed. However, as the heating of electrons due to the inverse bremsstrahlung process is weak at these radiation wavelengths and pulse fluences, the increase of the electron temperature with the pulse intensity is mainly due to the increasing photoionization rate within the irradiated sample. [ABSTRACT FROM AUTHOR]

Abstract: We performed time-of-flight (TOF) spectroscopy on a jet of rare gas clusters using light pulses at λ FEL =32nm produced by the FLASH VUV freeelectron-laser (Hamburg, Germany) with a maximum peak power density of about 3×1013 W/cm2 at the sample. Energy deposition on the clusters was found to be strongly dependent on lambda and much more efficient in the VUV than in the IR and visible spectral range. We observed multiple ionization of rare gas atoms coming from clusters; the latter fragment completely upon absorption of a single pulse. We have also measured high quality photoelectron spectra. Small angle soft X-ray scattering (SAXS) from a single light pulse (λ FEL =32nm), was recorded with high signal to noise ratio for very large (N atoms 3×106) Argon clusters. [Copyright &y& Elsevier]

We present time-resolved femtosecond photoelectron momentum images and angular distributions of dissociating, laser-aligned 1,4-dibromobenzene (C6H4Br2) molecules measured in a near-infrared pump, soft-x-ray probe experiment performed at an x-ray free-electron laser. The observed alignment dependence of the bromine 2p photoelectron angular distributions is compared to density functional theory calculations and interpreted in terms of photoelectron diffraction. While no clear time-dependent effects are observed in the angular distribution of the Br(2p) photoelectrons, other, low-energy electrons show a pronounced dependence on the time delay between the near-infrared laser and the x-ray pulse. [ABSTRACT FROM AUTHOR]