The original observation of the Einstein-de Haas effect was a landmark experiment in the early history of modern physics that illustrates the relationship between magnetism and angular momentum. Today the effect is still discussed in elementary physics courses to demonstrate that the angular momentum associated with the aligned electron spins in a ferromagnet can be converted to mechanical angular momentum by reversing the direction of magnetisation using an external magnetic field. In recent times, a related problem in magnetism concerns the time-scale over which this angular momentum transfer can occur. It is known experimentally for several metallic ferromagnets that intense photoexcitation leads to a drop in the magnetisation on a time scale shorter than 100 fs, a phenomenon called ultrafast demagnetisation. The microscopic mechanism for this process has been hotly debated, with one key question still unanswered: where does the angular momentum go on these sub-picosecond time scales? Here we show using femtosecond time-resolved x-ray diffraction that a large fraction of the angular momentum lost from the spin system on the laserinduced demagnetisation of ferromagnetic iron is transferred to the lattice on sub-picosecond timescales, manifesting as a transverse strain wave that propagates from the surface into the bulk. By fitting a simple model of the x-ray data to simulations and optical data, we roughly estimate that the angular momentum occurs on a time scale of 200 fs and corresponds to 80% of the angular momentum lost from the spin system. Our results show that interaction with the lattice plays an essential role in the process of ultrafast demagnetisation in this system.

The Ultrafast Einstein-De Haas Effect

Catching CO oxidation Details of the transition state that forms as carbon monoxide (CO) adsorbed on a ruthenium surface is oxidized to CO2 have been revealed by ultrafast excitation and probe methods. Öström et al. initiated the reaction between CO and adsorbed oxygen atoms with laser pulses that rapidly heated the surface and then probed the changes in electronic structure with oxygen x-ray absorption spectroscopy. They observed transition-state configurations that are consistent with density functional theory and a quantum oscillator model. Science, this issue p. 978 Ultrafast x-ray spectroscopy reveals electronic changes that occur during the oxidation of carbon monoxide on a ruthenium surface. Femtosecond x-ray laser pulses are used to probe the carbon monoxide (CO) oxidation reaction on ruthenium (Ru) initiated by an optical laser pulse. On a time scale of a few hundred femtoseconds, the optical laser pulse excites motions of CO and oxygen (O) on the surface, allowing the reactants to collide, and, with a transient close to a picosecond (ps), new electronic states appear in the O K-edge x-ray absorption spectrum. Density functional theory calculations indicate that these result from changes in the adsorption site and bond formation between CO and O with a distribution of OC–O bond lengths close to the transition state (TS). After 1 ps, 10% of the CO populate the TS region, which is consistent with predictions based on a quantum oscillator model.

/pdf/probing-the-transition-state-region-in-catalytic-co-522ich01rc.pdf

"Probing the Transition State Region in Catalytic CO Oxidation on Ru" data files

Linear accelerator-based free-electron lasers (FELs) are the leading source of fully coherent X-rays with ultra-high peak powers and ultra-short pulse lengths. Current X-ray FEL facilities have proved their worth as useful tools for diverse scientific applications. In this paper, we present an overview of the features and future prospects of X-ray FELs, including the working principles and properties of X-ray FELs, the operational status of different FEL facilities worldwide, the applications supported by such facilities, and the current developments and outlook for X-ray FEL-based research.

Features and futures of X-ray free-electron lasers.

The metal centres in metalloenzymes and molecular catalysts are responsible for the rearrangement of atoms and electrons during complex chemical reactions, and they enable selective pathways of charge and spin transfer, bond breaking/making and the formation of new molecules. Mapping the electronic structural changes at the metal sites during the reactions gives a unique mechanistic insight that has been difficult to obtain to date. The development of X-ray free-electron lasers (XFELs) enables powerful new probes of electronic structure dynamics to advance our understanding of metalloenzymes. The ultrashort, intense and tunable XFEL pulses enable X-ray spectroscopic studies of metalloenzymes, molecular catalysts and chemical reactions, under functional conditions and in real time. In this Technical Review, we describe the current state of the art of X-ray spectroscopy studies at XFELs and highlight some new techniques currently under development. With more XFEL facilities starting operation and more in the planning or construction phase, new capabilities are expected, including high repetition rate, better XFEL pulse control and advanced instrumentation. For the first time, it will be possible to make real-time molecular movies of metalloenzymes and catalysts in solution, while chemical reactions are taking place. X-ray lasers offer unprecedented capabilities, with their tunable, intense and short X-ray pulses. This Technical Review discusses the current and future use of X-ray lasers for probing molecular catalysts and metalloenzymes and their chemical reactions in real time and under functional conditions.

/pdf/using-x-ray-free-electron-lasers-for-spectroscopy-of-3b0xjw5vac.pdf

Using X-ray free-electron lasers for spectroscopy of molecular catalysts and metalloenzymes

A self-seeded X-ray free-electron laser (XFEL) is a promising approach to realize bright, fully coherent free-electron laser (FEL) sources in the hard X-ray domain that have been a long-standing issue with longitudinal coherence remaining challenging. At the Pohang Accelerator Laboratory XFEL, we have demonstrated a hard X-ray self-seeded XFEL with a peak brightness of 3.2 × 1035 photons s–1 mm–2 mrad–2 0.1% bandwidth (BW)–1 at 9.7 keV. The bandwidth (0.19 eV) is about 1/70 times as wide (close to the Fourier transform limit) and the peak spectral brightness is 40 times higher than in self-amplified spontaneous emission (SASE), with substantial improvements in the stability of self-seeding and noticeably suppressed pedestal effects. We could reach an excellent self-seeding performance at a photon energy of 3.5 keV (lowest) and 14.6 keV (highest) with the same stability as the 9.7 keV self-seeding. The bandwidth of the 14.6 keV seeded FEL was 0.32 eV, and the peak brightness was 1.3 × 1035 photons s–1 mm–2 mrad–2 0.1%BW–1. We show that the use of seeded FEL pulses with higher reproducibility and a cleaner spectrum results in serial femtosecond crystallography data of superior quality compared with data collected using SASE mode. A hard X-ray self-seeded X-ray free-electron laser at the Pohang Accelerator Laboratory provides X-ray pulses with peak brightness of 3.2 × 1035 photons s–1 mm–2 mrad–2 0.1%BW–1 at 9.7 keV and a very small shot-to-shot electron energy jitter of 0.012%.

High-brightness self-seeded X-ray free-electron laser covering the 3.5 keV to 14.6 keV range

We present the first lasing results of SwissFEL, a hard X-ray free-electron laser (FEL) that recently came into operation at the Paul Scherrer Institute in Switzerland. SwissFEL is a very stable, compact and cost-effective X-ray FEL facility driven by a low-energy and ultra-low-emittance electron beam travelling through short-period undulators. It delivers stable hard X-ray FEL radiation at 1-A wavelength with pulse energies of more than 500 μJ, pulse durations of ~30 fs (root mean square) and spectral bandwidth below the per-mil level. Using special configurations, we have produced pulses shorter than 1 fs and, in a different set-up, broadband radiation with an unprecedented bandwidth of ~2%. The extremely small emittance demonstrated at SwissFEL paves the way for even more compact and affordable hard X-ray FELs, potentially boosting the number of facilities worldwide and thereby expanding the population of the scientific community that has access to X-ray FEL radiation. The first lasing results at SwissFEL, an X-ray free-electron laser, are presented, highlighting the facility’s unique capabilities. A general comparison to other major facilities is also provided.

A compact and cost-effective hard X-ray free-electron laser driven by a high-brightness and low-energy electron beam

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A compact and cost-effective hard X-ray free-electron laser driven by a high-brightness and low-energy electron beam