Jean-Charles Castagna

X-ray–optical cross-correlator for gas-phase experiments at the Linac Coherent Light Source free-electron laser

X-ray–optical pump–probe experiments at the Linac Coherent Light Source (LCLS) have so far been limited to a time resolution of 280 fs fwhm due to timing jitter between the accelerator-based free-electron laser (FEL) and optical lasers. We have implemented a single-shot cross-correlator for femtosecond x-ray and infrared pulses. A reference experiment relying only on the pulse arrival time information from the cross-correlator shows a time resolution better than 50 fs fwhm (22 fs rms) and also yields a direct measurement of the maximal x-ray pulse length. The improved time resolution enables ultrafast pump–probe experiments with x-ray pulses from LCLS and other FEL sources.

Spectral encoding of x-ray/optical relative delay.

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.

The Atomic, Molecular and Optical Science instrument at the Linac Coherent Light Source

A description of the Atomic, Molecular and Optical Sciences (AMO) instrument at the Linac Coherent Light Source is presented. Recent scientific highlights illustrate the imaging, time-resolved spectroscopy and high-power density capabilities of the AMO instrument.

Femtosecond X-ray-induced fragmentation of fullerenes

A new class of femtosecond, intense, short – wavelength lasers – the free-electron laser – has opened up new opportunities to investigate the structure and dynamics in many scientific areas. These new lasers, whose performance keeps increasing, enable the understanding of physical and chemical changes at an atomic spatial scale and on the time scale of atomic motion which is essential for a broad range of scientific fields. We describe here the interaction of fullerenes in the multiphoton regime with the Linac Coherent Light Source (LCLS) X-ray free-electron laser at SLAC National Laboratory. In particular, we report on new data regarding the ionization of Ho3N@C80 molecules and compare the results with our prior C60 investigation of radiation damage induced by the LCLS pulses. We also discuss briefly the potential impact of newly available instrumentation to physical and chemical sciences when they are coupled with FELs as well as theoretical calculations and modeling.

Experimental strategies for optical pump - soft x-ray probe experiments at the LCLS

Free electron laser (FEL) based x-ray sources show great promise for use in ultrafast molecular studies due to the short pulse durations and site/element sensitivity in this spectral range. However, the self amplified spontaneous emission (SASE) process mostly used in FELs is intrinsically noisy resulting in highly fluctuating beam parameters. Additionally timing synchronization of optical and FEL sources adds delay jitter in pump-probe experiments. We show how we mitigate the effects of source noise for the case of ultrafast molecular spectroscopy of the nucleobase thymine. Using binning and resorting techniques allows us to increase time and spectral resolution. In addition, choosing observables independent of noisy beam parameters enhances the signal fidelity.

Split and Delay System for Soft X-ray Pump/Soft X-ray Probe Experiments at the LCLS Free Electron Laser

We will report on the development of a mirror based x-ray split and delay system for soft x-rays at the Linac Coherent Light Source free electron laser. The instrument will be based on an edge-polished mirror design, using grazing incidence mirrors to cover an energy range up 2000 eV. Two mirrors located immediately after the AMO Kirkpatrick-Baez mirrors will split the FEL wavefront; one of these mirrors will be translated and rotated to produce a variable delay up to 100 femtoseconds.

The LAMP instrument at the Linac Coherent Light Source free-electron laser

The Laser Applications in Materials Processing (LAMP) instrument is a new end-station for soft X-ray imaging, high-field physics, and ultrafast X-ray science experiments that is available to users at the Linac Coherent Light Source (LCLS) free-electron laser. While the instrument resides in the Atomic, Molecular and Optical science hutch, its components can be used at any LCLS beamline. The end-station has a modular design that provides high flexibility in order to meet user-defined experimental requirements and specifications. The ultra-high-vacuum environment supports different sample delivery systems, including pulsed and continuous atomic, molecular, and cluster jets; liquid and aerosols jets; and effusive metal vapor beams. It also houses movable, large-format, high-speed pnCCD X-ray detectors for detecting scattered and fluorescent photons. Multiple charged-particle spectrometer options are compatible with the LAMP chamber, including a double-sided spectrometer for simultaneous and even coincident measurements of electrons, ions, and photons produced by the interaction of the high-intensity X-ray beam with the various samples. Here we describe the design and capabilities of the spectrometers along with some general aspects of the LAMP chamber and show some results from the initial instrument commissioning.

X-ray split and delay device for ultrafast x-ray science at the AMO instrument at LCLS

Ultrafast molecular dynamics can be studied using x-rays from both synchrotrons sources and x-ray free electron lasers. Synchrotron studies are limited by the 10-100 ps duration pulses to processes where the Auger lifetime can be used to probe dynamics initiated by excitation of an inner-shell electron to an antibonding orbital. The short pulses produced by x-ray free electron lasers offer the opportunity to study molecular dynamics directly with pump-probe techniques. A two-mirror x-ray split and delay device has been developed for x- ray pump - x-ray probe experiments at the soft x-ray AMO instrument at the LCLS. The device operates over a photon energy range of 250-1800 eV with a variable delay of up to 200 femtoseconds with 0.1 fs resolution.

Next Generation Endstation for Concurrent Measurements of Charged Products and Photons in LCLS FEL Experiments

We are designing and building the next generation multi-purpose instrumentation especially adapted to accommodate unique large-area, single-photon counting pnCCD detectors together with advanced many-particle ion and electron imaging spectrometers (reaction microscope, REMI; velocity map imaging, VMI; magnetic bottle) for simultaneous detection of scattered and fluorescent photons and charged particles in experiments at the LCLS FEL.