The time–energy information of ultrashort X-ray free-electron laser pulses generated by the Linac Coherent Light Source is measured with attosecond resolution via angular streaking of neon 1s photoelectrons. The X-ray pulses promote electrons from the neon core level into an ionization continuum, where they are dressed with the electric field of a circularly polarized infrared laser. This induces characteristic modulations of the resulting photoelectron energy and angular distribution. From these modulations we recover the single-shot attosecond intensity structure and chirp of arbitrary X-ray pulses based on self-amplified spontaneous emission, which have eluded direct measurement so far. We characterize individual attosecond pulses, including their instantaneous frequency, and identify double pulses with well-defined delays and spectral properties, thus paving the way for X-ray pump/X-ray probe attosecond free-electron laser science.

Attosecond time–energy structure of X-ray free-electron laser pulses

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

Light-driven sodium pumps actively transport small cations across cellular membranes1. These pumps are used by microorganisms to convert light into membrane potential and have become useful optogenetic tools with applications in neuroscience. Although the resting state structures of the prototypical sodium pump Krokinobacter eikastus rhodopsin 2 (KR2) have been solved2,3, it is unclear how structural alterations over time allow sodium to be translocated against a concentration gradient. Here, using the Swiss X-ray Free Electron Laser4, we have collected serial crystallographic data at ten pump-probe delays from femtoseconds to milliseconds. High-resolution structural snapshots throughout the KR2 photocycle show how retinal isomerization is completed on the femtosecond timescale and changes the local structure of the binding pocket in the early nanoseconds. Subsequent rearrangements and deprotonation of the retinal Schiff base open an electrostatic gate in microseconds. Structural and spectroscopic data, in combination with quantum chemical calculations, indicate that a sodium ion binds transiently close to the retinal within one millisecond. In the last structural intermediate, at 20 milliseconds after activation, we identified a potential second sodium-binding site close to the extracellular exit. These results provide direct molecular insight into the dynamics of active cation transport across biological membranes.

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Femtosecond-to-millisecond structural changes in a light-driven sodium pump.

10 years of pioneering X-ray science at the Free-Electron Laser FLASH at DESY

Over more than a century, X-rays have transformed our understanding of the fundamental structure of matter and have been an indispensable tool for chemistry, physics, biology, materials science and related fields. Recent advances in ultrafast X-ray sources operating in the femtosecond to attosecond regimes have opened an important new frontier in X-ray science. These advances now enable: (i) sensitive probing of structural dynamics in matter on the fundamental timescales of atomic motion, (ii) element-specific probing of electronic structure and charge dynamics on fundamental timescales of electronic motion, and (iii) powerful new approaches for unravelling the coupling between electronic and atomic structural dynamics that underpin the properties and function of matter. Most notable is the recent realization of X-ray free-electron lasers (XFELs) with numerous new XFEL facilities in operation or under development worldwide. Advances in XFELs are complemented by advances in synchrotron-based and table-top laser-plasma X-ray sources now operating in the femtosecond regime, and laser-based high-order harmonic XUV sources operating in the attosecond regime. This article is part of the theme issue 'Measurement of ultrafast electronic and structural dynamics with X-rays'.

https://royalsocietypublishing.org/doi/pdf/10.1098/rsta.2018.0384

Recent advances in ultrafast X-ray sources

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.

Patrick Pollet

Papers

SwissFEL: The Swiss X-ray Free Electron Laser