The hard X-ray free-electron laser at the Pohang Accelerator Laboratory (PAL-XFEL) in the Republic of Korea achieved saturation of a 0.144 nm free-electron laser beam on 27 November 2016, making it the third hard X-ray free-electron laser in the world, following the demonstrations of the Linac Coherent Light Source (LCLS) and the SPring-8 Angstrom Compact Free Electron Laser (SACLA). The use of electron-beam-based alignment incorporating undulator radiation spectrum analysis has allowed reliable operation of PAL-XFEL with unprecedented temporal stability and dispersion-free orbits. In particular, a timing jitter of just 20 fs for the free-electron laser photon beam is consistently achieved due to the use of a state-of-the-art design of the electron linear accelerator and electron-beam-based alignment. The low timing jitter of the electron beam makes it possible to observe Bi(111) phonon dynamics without the need for timing-jitter correction, indicating that PAL-XFEL will be an extremely useful tool for hard X-ray time-resolved experiments. The Pohang Accelerator Laboratory X-ray Free Electron Laser (PAL-XFEL) in South Korea has now entered operation with a timing jitter of just 20 fs.

Hard X-ray free-electron laser with femtosecond-scale timing jitter

Crucial to many light-driven processes in transition metal complexes is the absorption and dissipation of energy by 3d electrons. But a detailed understanding of such non-equilibrium excited-state dynamics and their interplay with structural changes is challenging: a multitude of excited states and possible transitions result in phenomena too complex to unravel when faced with the indirect sensitivity of optical spectroscopy to spin dynamics and the flux limitations of ultrafast X-ray sources. Such a situation exists for archetypal polypyridyl iron complexes, such as [Fe(2,2'-bipyridine)3](2+), where the excited-state charge and spin dynamics involved in the transition from a low- to a high-spin state (spin crossover) have long been a source of interest and controversy. Here we demonstrate that femtosecond resolution X-ray fluorescence spectroscopy, with its sensitivity to spin state, can elucidate the spin crossover dynamics of [Fe(2,2'-bipyridine)3](2+) on photoinduced metal-to-ligand charge transfer excitation. We are able to track the charge and spin dynamics, and establish the critical role of intermediate spin states in the crossover mechanism. We anticipate that these capabilities will make our method a valuable tool for mapping in unprecedented detail the fundamental electronic excited-state dynamics that underpin many useful light-triggered molecular phenomena involving 3d transition metal complexes.

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Tracking excited-state charge and spin dynamics in iron coordination complexes

Ultrafast electron probes are powerful tools, complementary to x-ray free-electron lasers, used to study structural dynamics in material, chemical, and biological sciences. High brightness, relativistic electron beams with femtosecond pulse duration can resolve details of the dynamic processes on atomic time and length scales. SLAC National Accelerator Laboratory recently launched the Ultrafast Electron Diffraction (UED) and microscopy Initiative aiming at developing the next generation ultrafast electron scattering instruments. As the first stage of the Initiative, a mega-electron-volt (MeV) UED system has been constructed and commissioned to serve ultrafast science experiments and instrumentation development. The system operates at 120-Hz repetition rate with outstanding performance. In this paper, we report on the SLAC MeV UED system and its performance, including the reciprocal space resolution, temporal resolution, and machine stability.

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Mega-electron-volt ultrafast electron diffraction at SLAC National Accelerator Laboratory

The SwissFEL X-ray Free Electron Laser (XFEL) facility started construction at the Paul Scherrer Institute (Villigen, Switzerland) in 2013 and will be ready to accept its first users in 2018 on the Aramis hard X-ray branch. In the following sections we will summarize the various aspects of the project, including the design of the soft and hard X-ray branches of the accelerator, the results of SwissFEL performance simulations, details of the photon beamlines and experimental stations, and our first commissioning results.

SwissFEL: The Swiss X-ray Free Electron Laser

European XFEL is a free-electron laser (FEL) user facility providing soft and hard X-ray FEL radiation to initially six scientific instruments. Starting user operation in fall 2017 European XFEL will provide new research opportunities to users from science domains as diverse as physics, chemistry, geo- and planetary sciences, materials sciences or biology. The unique feature of European XFEL is the provision of high average brilliance in the soft and hard X-ray regime, combined with the pulse properties of FEL radiation of extreme peak intensities, femtosecond pulse duration and high degree of coherence. The high average brilliance is achieved through acceleration of up to 27,000 electron bunches per second by the super-conducting electron accelerator. Enabling the usage of this high average brilliance in user experiments is one of the major instrumentation drivers for European XFEL. The radiation generated by three FEL sources is distributed via long beam transport systems to the experiment hall where the scientific instruments are located side-by-side. The X-ray beam transport systems have been optimized to maintain the unique features of the FEL radiation which will be monitored using build-in photon diagnostics. The six scientific instruments are optimized for specific applications using soft or hard X-ray techniques and include integrated lasers, dedicated sample environment, large area high frame rate detector(s) and computing systems capable of processing large quantities of data.

Photon Beam Transport and Scientific Instruments at the European XFEL

Recently, few-femtosecond pulses have become available at hard X-ray free-electron lasers Coupled with the available sub-10 fs optical pulses, investigations into few-femtosecond dynamics are not far off However, achieving sufficient synchronization between optical lasers and X-ray pulses continues to be challenging We report a 'measure-and-sort' approach, which achieves sub-10 fs root-mean-squared (rms) error measurement at hard X-ray FELs, far beyond the 100-200 fs rms jitter limitations This timing diagnostic, now routinely available at the Linac Coherent Light Source (LCLS), is based on ultrafast free-carrier generation in optically transparent materials Correlation between two independent measurements enables unambiguous demonstration of ~6 fs rms error in reporting the optical/X-ray delay, with single shot error suggesting the possibility of reaching few-femtosecond resolution

Achieving few-femtosecond time-sorting at hard X-ray free-electron lasers

The advent of few femtosecond x-ray light sources brings promise of x-ray/optical pump-probe experiments that can measure chemical and structural changes in the 10–100 fs time regime. Widely distributed timing systems used at x-ray Free-Electron Laser facilities are typically limited to above 50 fs fwhm jitter in active x-ray/optical synchronization. The approach of single-shot timing measurements is used to sort results in the event processing stage. This has seen wide use to accommodate the insufficient precision of active stabilization schemes. In this article, we review the current technique for “measure-and-sort” at the Linac Coherent Light Source at the SLAC National Accelerator Laboratory. The relative arrival time between an x-ray pulse and an optical pulse is measured near the experimental interaction region as a spectrally encoded cross-correlation signal. The cross-correlation provides a time-stamp for filter-and-sort algorithms used for real-time sorting. Sub-10 fs rms resolution is common in this technique, placing timing precision at the same scale as the duration of the shortest achievable x-ray pulses.

Spectral encoding method for measuring the relative arrival time between x-ray/optical pulses

A recently demonstrated single-shot measurement of the relative delay between x-ray FEL pulses and optical laser pulses has now been improved to ~10 fs rms error and has successfully been demonstrated for both soft and hard x-ray pulses. It is based on x-ray induced step-like reduction in optical transmissivity of a semiconductor membrane (Si 3 N 4 ). The transmissivity is probed by an optical continuum spanning 450 - 650 nm where spectral chirp provides a mapping of the step in spectrum to the arrival time of the x-ray pulse relative to the optical laser system.

Spectral encoding based measurement of x-ray/optical relative delay to ~10 fs rms

http://absimage.aps.org/image/DAMOP12/MWS_DAMOP12-2012-000484.pdf

Doug French

Papers

Achieving few-femtosecond time-sorting at hard X-ray free-electron lasers

Spectral encoding method for measuring the relative arrival time between x-ray/optical pulses

Spectral encoding based measurement of x-ray/optical relative delay to ~10 fs rms

Measuring 10 fs dynamics via resonant x-ray pump/x-ray probe spectroscopy