Coherent Light Source Free Electron Research Articles

Nonuniform Flow Dynamics Probed by Nanosecond X-Ray Speckle Visibility Spectroscopy.

We report observations of nanosecond nonuniform colloidal dynamics in a free flowing liquid jet using ultrafast x-ray speckle visibility spectroscopy. Utilizing a nanosecond double-bunch mode, the Linac Coherent Light Source free electron laser produced pairs of femtosecond coherent hard x-ray pulses. By exploring anisotropy in the visibility of summed speckle patterns which relates to the correlation functions, we evaluate not only the average particle flow rate in a colloidal nanoparticle jet, but also the nonuniform flow field within. The methodology presented here establishes the foundation for the study of nano- and atomic-scale inhomogeneous fluctuations in complex matter using x-ray free electron laser sources.

Two mirror X-ray pulse split and delay instrument for femtosecond time resolved investigations at the LCLS free electron laser facility.

We built a two-mirror based X-ray split and delay (XRSD) device for soft X-rays at the Linac Coherent Light Source free electron laser facility. The instrument is based on an edge-polished mirror design covering an energy range of 250 eV-1800 eV and producing a delay between the two split pulses variable up to 400 femtoseconds with a sub-100 attosecond resolution. We present experimental and simulation results regarding molecular dissociation dynamics in CH3I and CO probed by the XRSD device. We observed ion kinetic energy and branching ratio dependence on the delay times which were reliably produced by the XRSD instrument.

Molecular dynamics induced by short and intense x-ray pulses from the LCLS

The past six years have led to a wealth of experimental and theoretical data revealing the nature of the interaction between gas-phase molecules and short and intense x-ray pulses, from the Linac coherent light source free electron laser (FEL). We present here a few highlights that describe some of the first photoabsorption measurements of gas-phase molecules. In particular, we report on a three decades long prediction of single-site double core holes (ss-DCH) and two-site double core holes (ts-DCH) in diatomic and triatomic molecules. We also describe recent measurements that validate a simple theory regarding femtosecond intense x-ray induced fragmentation dynamics of C60 as well as photoabsorption measurements of encapsulated fullerenes, Ho3N@C80. The latter investigation opens the way for even more complex molecular studies with FELs. In all of the described highlights, working in close collaboration with theorists enabled the interpretation of, or predicted our measurements, and in some cases our experiments guided the modeling. We conclude this article by describing the potential of new instrumentation for chemical and biological sciences especially in light of new or improved FELs.

Damage threshold of platinum coating used for optics for self-seeding of soft X-ray free electron laser.

We investigated the experimental damage threshold of platinum coating on a silicon substrate illuminated by soft x-ray radiation at grazing incidence angle of 2 degrees. The coating was the same as the blazed grating used for the soft X-ray self-seeding optics of the Linac Coherent Light Source free electron laser. The irradiation condition was chosen such that the absorbed dose was similar to the maximum dose expected for the grating. The expected dose was simulated by solving the Helmholtz equation in non-homogenous media. The experiment was performed at 900 eV photon energy for both single pulse and multi-shot conditions. We have not observed single shot damage. This corresponds to a single shot damage threshold being higher than 3 J/cm(2). The multiple shot damage threshold measured for 10 shots and about 600 shots was determined to be 0.95 J/cm(2) and 0.75 J/cm(2) respectively. The damage threshold occurred at an instantaneous dose which is higher that the melt dose of platinum.

Multiphoton ionization and fragmentation of molecules with the LCLS X-ray FEL

The photoionization of diatomic and polyatomic molecules with intense femtosecond X-ray pulses from the Linac Coherent Light Source free electron laser have been investigated using photoion spectrometry. The dominant mechanism measured is multiple core-ionization-Auger decay cycles leading to molecular fragmentation followed by the production of highly charged atomic ions. This work sheds light on fundamental aspects of matter–intense X-ray interaction and impacts research relevant to matter under extreme conditions and molecular radiation damage, pertinent to single bio-molecule imaging.

Double core-hole formation in small molecules at the LCLS free electron laser

We have investigated nonlinear processes in small molecules by x-ray photoelectron spectroscopy using the Linac Coherent Light Source free electron laser, and by simulations. The main focus of the experiments was the formation of the two-site double core-hole (tsDCH) states in the molecules CO2, N2O and N2. These experiments are described in detail and the results are compared with simulations of the photoelectron spectra. The double core-hole states, and in particular the tsDCH states, have been predicted to be highly sensitive to the chemical environment. The theory behind this chemical sensitivity is validated by the experiments. Furthermore, our simulations of the relative integrated intensities of the peaks associated with the nonlinear processes show that this type of simulation, in combination with experimental data, provides a useful tool for estimating the duration of ultra-short x-ray pulses.

Using covariance mapping to investigate the dynamics of multi-photon ionization processes of Ne atoms exposed to X-FEL pulses

We report on a detailed investigation into the electron emission processes of Ne atoms exposed to intense femtosecond x-ray pulses, provided by the Linac Coherent Light Source Free Electron Laser (FEL) at Stanford. The covariance mapping technique is applied to analyse the data, and the capability of this approach to disentangle both linear and nonlinear correlation features which may be hidden on coincidence maps of the same data set is demonstrated. Different correction techniques which enable improvements on the quality of the spectral features extracted from the covariance maps are explored. Finally, a method for deriving characteristics of the x-ray FEL pulses based on covariance mapping in combination with model simulations is presented.

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.

X-Ray FEL Induced Double Core-Hole and High Charge State Production

We report novel results on multiple photoionization of the N2 molecule by femtosecond x-ray pulses from the Linac Coherent Light Source free electron laser. Ion spectroscopy reveals the ionization and dissociation dynamics, including a molecular mechanism of frustrated absorption that suppresses the formation of high charge states at short pulse durations. Auger and photo-electron analysis of double core hole production (through absorption of two photons on the time scale shorter than the Auger decay) agrees well with theory for the case of both K-shell holes on the same N atom, and gives an experimental upper bound for the relative contribution in case of one core hole on each N atom.

Nanoplasma Dynamics of Single Large Xenon Clusters Irradiated with Superintense X-Ray Pulses from the Linac Coherent Light Source Free-Electron Laser

The plasma dynamics of single mesoscopic Xe particles irradiated with intense femtosecond x-ray pulses exceeding 10(16) W/cm2 from the Linac Coherent Light Source free-electron laser are investigated. Simultaneous recording of diffraction patterns and ion spectra allows eliminating the influence of the laser focal volume intensity and particle size distribution. The data show that for clusters illuminated with intense x-ray pulses, highly charged ionization fragments in a narrow distribution are created and that the nanoplasma recombination is efficiently suppressed.

Auger Electron Angular Distribution of Double Core-Hole States in the Molecular Reference Frame

The Linac Coherent Light Source free electron laser is a source of high brightness x rays, 2×10(11) photons in a ∼5 fs pulse, that can be focused to produce double core vacancies through rapid sequential ionization. This enables double core vacancy Auger electron spectroscopy, an entirely new way to study femtosecond chemical dynamics with Auger electrons that probe the local valence structure of molecules near a specific atomic core. Using 1.1 keV photons for sequential x-ray ionization of impulsively aligned molecular nitrogen, we observed a rich single-site double core vacancy Auger electron spectrum near 413 eV, in good agreement with ab initio calculations, and we measured the corresponding Auger electron angle dependence in the molecular frame.

Double Core-Hole Production inN2: Beating the Auger Clock

We investigate the creation of double K-shell holes in N2 molecules via sequential absorption of two photons on a time scale shorter than the core-hole lifetime by using intense x-ray pulses from the Linac Coherent Light Source free electron laser. The production and decay of these states is characterized by photoelectron spectroscopy and Auger electron spectroscopy. In molecules, two types of double core holes are expected, the first with two core holes on the same N atom, and the second with one core hole on each N atom. We report the first direct observations of the former type of core hole in a molecule, in good agreement with theory, and provide an experimental upper bound for the relative contribution of the latter type.

Colossal Magnetoresistive Manganite Based Fast Bolometric X-ray Sensors for Total Energy Measurements of Free Electron Lasers

Bolometric detectors based on epitaxial thin films of rare earth perovskite manganites have been proposed as total energy monitors for X-ray pulses at the Linac Coherent Light Source free electron laser. We demonstrate such a detector scheme based on epitaxial thin films of the perovskite manganese oxide material Nd{sub 0.67}Sr{sub x0.33}MnO{sub 3}, grown by pulsed laser deposition on buffered silicon substrates. The substrate and sensor materials are chosen to meet the conflicting requirements of radiation hardness, sensitivity, speed and linearity over a dynamic range of three orders of magnitude. The key challenge in the material development is the integration of the sensor material with Si. Si is required to withstand the free electron laser pulse impact and to achieve a readout speed three orders of magnitude faster than conventional cryoradiometers for compatibility with the Linac Coherent Light Source pulse rate. We discuss sensor material development and the photoresponse of prototype devices. This Linac Coherent Light Source total energy monitor represents the first practical application of manganite materials as bolometric sensors.

Development of CMR Manganite Sensors for Energy Measurement of the Linear Coherent Light Source Free Electron Laser Xray Pulses

ABSTRACTWe are developing Colossal Magnetoresistive (CMR) manganite thin film bolometric sensors to be employed as total energy detectors for beam diagnostics of the Linear Coherent Light Source (LCLS) Free Electron Laser (FEL) (at the Stanford Linear Accelerator). LCLS is an ultra bright, ultra short coherent x-ray source whose peak brightness will exceed that of third generation x-ray sources by about ten orders of magnitude and average brightness by three orders of magnitudes. It is expected to produce 1012 x-rays per 200 fs pulse with a repeat frequency of 120 Hz through self-amplified stimulated emission. In characterizing the beam, it will be necessary to measure the total energy of the FEL pulse. The Advanced Detector Group at Lawrence Livermore Laboratory has developed a scheme for FEL total energy measurements based on bolometric detection and are collaborating with Towson University to implement such a detector using CMR manganite thin films. Here we discuss the basic scheme, results of simulations of the thermal response and the materials development efforts towards fabricating the thin film detectors.