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We design and realize an arrival time diagnostic for ultrashort X-ray pulses achieving unprecedented high sensitivity in the soft X-ray regime via cross-correlation with a ≈1550 nm optical laser. An interferometric detection scheme is combined with a multi-layer sample design to greatly improve the sensitivity of the measurement. We achieve up to 275% of relative signal change when exposed to 1.6 mJ/cm 2 of soft X-rays at 530 eV, more than a hundred-fold improvement in sensitivity as compared to previously reported techniques. The resolution of the arrival time measurement is estimated to around 2.8 fs (rms). The demonstrated X-ray arrival time monitor paves the way for sub-10 fs-level timing jitter at high repetition rate X-ray facilities.

New high-repetition-rate x-ray free electron lasers (XFELs) require for their operation highly reliable ultrafast laser systems with high pulse energy, high repetition rate, and high average power. In this Letter, we present high-average-power scaling of near-infrared optical parametric chirped pulse amplification (OPCPA) in potassium titanyl arsenate (KTA) with tunable center wavelengths from 1.5 to 2.0 μm. Using a three-stage amplification scheme and a kW-level InnoSlab Yb:YAG pump amplifier for the final non-collinear KTA stage, we demonstrate an amplified output power of 106.2 W at a center wavelength of 1.75 μm and 100 kHz. Idler absorption introduces a potential upper limit on the average power scaling of center wavelengths <1.70  μm. Future scaling of average power to hundreds of Watts is possible at center wavelengths ≥1.70  μm.

We present a 100 kHz, sub-20 fs optical parametric chirped-pulse amplifier (OPCPA) system delivering 88.6 W average power at a center wavelength of 800 nm. The seed pulses are derived from the pump laser via white-light continuum generation and are amplified in three non-collinear OPCPA stages. The final two high-power stages are pumped with a 661 W Yb:YAG InnoSlab amplifier. A simple and robust design is used for the OPCPA system to avoid thermal effects and enhance long-term stability, resulting in excellent beam quality and high conversion efficiency. To the best of our knowledge, this is the highest average power OPCPA system reported to date.

Two-dimensional materials are subject to intrinsic and dynamic rippling that modulates their optoelectronic and electromechanical properties. Here, we directly visualize the dynamics of these processes within monolayer transition metal dichalcogenide MoS2 using femtosecond electron scattering techniques as a real-time probe with atomic-scale resolution. We show that optical excitation induces large-amplitude in-plane displacements and ultrafast wrinkling of the monolayer on nanometer length-scales, developing on picosecond time-scales. These deformations are associated with several percent peak strains that are fully reversible over tens of millions of cycles. Direct measurements of electron-phonon coupling times and the subsequent interfacial thermal heat flow between the monolayer and substrate are also obtained. These measurements, coupled with first-principles modeling, provide a new understanding of the dynamic structural processes that underlie the functionality of two-dimensional materials and open up new opportunities for ultrafast strain engineering using all-optical methods.

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.

Ultrafast optical lasers play an essential role in exploiting the unique capabilities of recently commissioned X-ray free-electron laser facilities such as the Linac Coherent Light Source (LCLS). Pump-probe experimental techniques reveal ultrafast dynamics in atomic and molecular processes and reveal new insights in chemistry, biology, material science and high-energy-density physics. This manuscript describes the laser systems and experimental methods that enable cutting-edge optical laser/X-ray pump-probe experiments to be performed at LCLS.

Using balanced detection in both the radio frequency (RF) and the optical domain, we remotely synchronize the repetition rate of a Ti:sapphire oscillator to an Er-doped fiber oscillator through a 360 m length-stabilized dispersion compensated fiber link. The drift between these two optical oscillators is 3.3 fs root mean square (rms) over 24 hours. The 68 MHz Er-doped fiber oscillator is locked to a 476 MHz local RF reference clock, and serves as a master clock to distribute 10 fs-level timing signals through stabilized fiber links. This steady remote two-color optical-to-optical synchronization is an important step toward an integrated femtosecond fiber timing distribution system for free-electron lasers (FELs); it does not require x-ray pulses, and it makes sub-10-fs optical/x-ray pump-probe experiments feasible.

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.

The dioxygen we breathe is formed by light-induced oxidation of water in photosystem II. O2 formation takes place at a catalytic manganese cluster within milliseconds after the photosystem II reaction centre is excited by three single-turnover flashes. Here we present combined X-ray emission spectra and diffraction data of 2-flash (2F) and 3-flash (3F) photosystem II samples, and of a transient 3F' state (250 μs after the third flash), collected under functional conditions using an X-ray free electron laser. The spectra show that the initial O-O bond formation, coupled to Mn reduction, does not yet occur within 250 μs after the third flash. Diffraction data of all states studied exhibit an anomalous scattering signal from Mn but show no significant structural changes at the present resolution of 4.5 Å. This study represents the initial frames in a molecular movie of the structural changes during the catalytic reaction in photosystem II.

X-ray free-electron laser (XFEL) sources enable the use of crystallography to solve three-dimensional macromolecular structures under native conditions and without radiation damage. Results to date, however, have been limited by the challenge of deriving accurate Bragg intensities from a heterogeneous population of microcrystals, while at the same time modeling the X-ray spectrum and detector geometry. Here we present a computational approach designed to extract meaningful high-resolution signals from fewer diffraction measurements.

Intense femtosecond x-ray pulses produced at the Linac Coherent Light Source (LCLS) were used for simultaneous x-ray diffraction (XRD) and x-ray emission spectroscopy (XES) of microcrystals of photosystem II (PS II) at room temperature. This method probes the overall protein structure and the electronic structure of the Mn4CaO5 cluster in the oxygen-evolving complex of PS II. XRD data are presented from both the dark state (S1) and the first illuminated state (S2) of PS II. Our simultaneous XRD-XES study shows that the PS II crystals are intact during our measurements at the LCLS, not only with respect to the structure of PS II, but also with regard to the electronic structure of the highly radiation-sensitive Mn4CaO5 cluster, opening new directions for future dynamics studies.

The ultrabright femtosecond X-ray pulses provided by X-ray free-electron lasers open capabilities for studying the structure and dynamics of a wide variety of systems beyond what is possible with synchrotron sources. Recently, this "probe-before-destroy" approach has been demonstrated for atomic structure determination by serial X-ray diffraction of microcrystals. There has been the question whether a similar approach can be extended to probe the local electronic structure by X-ray spectroscopy. To address this, we have carried out femtosecond X-ray emission spectroscopy (XES) at the Linac Coherent Light Source using redox-active Mn complexes. XES probes the charge and spin states as well as the ligand environment, critical for understanding the functional role of redox-active metal sites. Kβ(1,3) XES spectra of Mn(II) and Mn(2)(III,IV) complexes at room temperature were collected using a wavelength dispersive spectrometer and femtosecond X-ray pulses with an individual dose of up to >100 MGy. The spectra were found in agreement with undamaged spectra collected at low dose using synchrotron radiation. Our results demonstrate that the intact electronic structure of redox active transition metal compounds in different oxidation states can be characterized with this shot-by-shot method. This opens the door for studying the chemical dynamics of metal catalytic sites by following reactions under functional conditions. The technique can be combined with X-ray diffraction to simultaneously obtain the geometric structure of the overall protein and the local chemistry of active metal sites and is expected to prove valuable for understanding the mechanism of important metalloproteins, such as photosystem II.

An electrospun liquid microjet has been developed that delivers protein microcrystal suspensions at flow rates of 0.14-3.1 µl min(-1) to perform serial femtosecond crystallography (SFX) studies with X-ray lasers. Thermolysin microcrystals flowed at 0.17 µl min(-1) and diffracted to beyond 4 Å resolution, producing 14,000 indexable diffraction patterns, or four per second, from 140 µg of protein. Nanoflow electrospinning extends SFX to biological samples that necessitate minimal sample consumption.

Most of the dioxygen on earth is generated by the oxidation of water by photosystem II (PS II) using light from the sun. This light-driven, four-photon reaction is catalyzed by the Mn(4)CaO(5) cluster located at the lumenal side of PS II. Various X-ray studies have been carried out at cryogenic temperatures to understand the intermediate steps involved in the water oxidation mechanism. However, the necessity for collecting data at room temperature, especially for studying the transient steps during the O-O bond formation, requires the development of new methodologies. In this paper we report room temperature X-ray diffraction data of PS II microcrystals obtained using ultrashort (< 50 fs) 9 keV X-ray pulses from a hard X-ray free electron laser, namely the Linac Coherent Light Source. The results presented here demonstrate that the "probe before destroy" approach using an X-ray free electron laser works even for the highly-sensitive Mn(4)CaO(5) cluster in PS II at room temperature. We show that these data are comparable to those obtained in synchrotron radiation studies as seen by the similarities in the overall structure of the helices, the protein subunits and the location of the various cofactors. This work is, therefore, an important step toward future studies for resolving the structure of the Mn(4)CaO(5) cluster without any damage at room temperature, and of the reaction intermediates of PS II during O-O bond formation.

We present a new technique for measuring the relative delay between a soft x-ray FEL pulse and an optical laser that indicates a sub 25 fs RMS measurement error. An ultra-short x-ray pulse photo-ionizes a semiconductor (Si(3)N(4)) membrane and changes the optical transmission. An optical continuum pulse with a temporally chirped bandwidth spanning 630 nm-710 nm interacts with the membrane such that the timing of the x-ray pulse can be determined from the onset of the spectral modulation of the transmitted optical pulse. This experiment demonstrates a nearly in situ single-shot measurement of the x-ray pulse arrival time relative to the ultra-short optical pulse., (© 2011 Optical Society of America)

We report on the development of what we consider to be a practical and highly stable stretched-pulse laser based on Yb(3+) -doped silica fiber. The Fabry-Perot cavity uses nonlinear polarization rotation as the mode-locking mechanism, and a semiconductor saturable-absorber mirror to ensure robust self-starting and incorporates a diffraction grating pair to compensate for the normal dispersion of the fiber. Use of a single-mode grating-stabilized telecommunications-qualified pump laser diode ensures reliable, low-noise operation (~0.05% amplitude fluctuations at 10-Hz measurement bandwidth). The laser generates high-quality, 60-pJ pulses of <110-fs duration at a repetition rate of ~54 MHz (3-mW average power).