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Chollet, M.

Publications and source records attributed to Chollet, M..

At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Multiple Supersonic Phase Fronts Launched at a Complex-Oxide Heterointerface

Selective optical excitation of a substrate lattice can drive phase changes across heterointerfaces. This phenomenon is a nonequilibrium analogue of static strain control in heterostructures and may lead to new applications in optically controlled phase change devices. Here, we make use of time-resolved nonresonant and resonant x-ray diffraction to clarify the underlying physics and to separate different microscopic degrees of freedom in space and time. We also measure the dynamics of the lattice and that of the charge disproportionation in NdNiO 3 , when an insulator-metal transition is driven by coherent lattice distortions in the LaAlO 3 substrate. We find that charge redistribution propagates at supersonic speeds from the interface into the NdNiO 3 film, followed by a sonic lattice wave. Our results establish a hierarchy of events for ultrafast control at complex-oxide heterointerfaces, when combined with measurements of magnetic disordering and of the metal-insulator transition.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO 3

The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here in this paper we apply subpicosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO 3 ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray-scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large-amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and incoherent across unit cells. This effect is associated with a dynamic rotation of the ferroelectric polarization switching on and then off on picosecond time scales. These transient polarization modulations are followed by long-lived vibrational heating effects driven by resonant excitation of the ferroelectric soft mode, as reflected in changes in the c-axis tetragonality. The ultrafast structural characterization described here enables a direct comparison with first-principles-based molecular-dynamics simulations, with good agreement obtained.

36 MATERIALS SCIENCE↗
DOE OSTI2016

ePix100 camera: Use and applications at LCLS

The ePix100 x-ray camera is a new system designed and built at SLAC for experiments at the Linac Coherent Light Source (LCLS). The camera is the first member of a family of detectors built around a single hardware and software platform, supporting a variety of front-end chips. With a readout speed of 120 Hz, matching the LCLS repetition rate, a noise lower than 80 e-rms and pixels of 50 µm × 50 µm, this camera offers a viable alternative to fast readout, direct conversion, scientific CCDs in imaging mode. The detector, designed for applications such as X-ray Photon Correlation Spectroscopy (XPCS) and wavelength dispersive X-ray Emission Spectroscopy (XES) in the energy range from 2 to 10 keV and above, comprises up to 0.5 Mpixels in a very compact form factor. In this paper, we report the performance of the camera during its first use at LCLS.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2016

The origin of incipient ferroelectricity in lead telluride

The interactions between electrons and lattice vibrations are fundamental to materials behaviour. In the case of group IV–VI, V and related materials, these interactions are strong, and the materials exist near electronic and structural phase transitions. The prototypical example is PbTe whose incipient ferroelectric behaviour has been recently associated with large phonon anharmonicity and thermoelectricity. Here we show that it is primarily electron-phonon coupling involving electron states near the band edges that leads to the ferroelectric instability in PbTe. Using a combination of nonequilibrium lattice dynamics measurements and first principles calculations, we find that photoexcitation reduces the Peierls-like electronic instability and reinforces the paraelectric state. This weakens the long-range forces along the cubic direction tied to resonant bonding and low lattice thermal conductivity. Lastly, our results demonstrate how free-electron-laser-based ultrafast X-ray scattering can be utilized to shed light on the microscopic mechanisms that determine materials properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Synchrotron XRD analysis of irradiated UO{sub 2} fuel at various burn-up

The micro-XRD technique based on synchrotron radiation is a powerful tool to analyze subtle changes in the crystal lattice structure of irradiated nuclear fuels. The micrometric beam size probes a relatively small volume in the samples. This, in turn, can allow studying the evolution of the material with burn-up even at the level of the grain sizes of the fuel. We report here the results obtained by micro-XRD performed at the microXAS beamline of the Swiss Light Source (SLS) on the two end-members of a series of burn-ups, i.e. a fresh non-irradiated UO2 (reference sample) and a 9 cycle sample, plus the first results on 5- and 7 cycle fuels. The use of the micro-beam allows us to follow the extent of grain polygonization as a function of burn-up and in a lower degree of temperature. The microXAS beamline being the only one where series of spent fuel are investigated, the current results presented in this study are of unique value. In earlier work at lower burn-ups and for doped fuel it has been shown that there is a strong difference in polygonization between center and periphery. While for the 9-cycle a complete restructuring could be shown here, the results for the 5- and 7-cycle samples are not fully conclusive. We obtain interesting results for these samples where both center and the periphery regions exhibit a mix of XRD reflexes, indicating various stages of sub-grain formation. Further detail analyses are needed on the basis of the numerous 2D XRD pictures captured to gain a clearer picture.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2016

Itinerant and localized magnetization dynamics in antiferromagnetic Ho

Using femtosecond time-resolved resonant magnetic x-ray diffraction at the Ho L 3 absorption edge, we investigate the demagnetization dynamics in antiferromagnetically ordered metallic Ho after femtosecond optical excitation. Here, tuning the x-ray energy to the electric dipole (E1, 2p → 5d) or quadrupole (E2, 2p → 4f) transition allows us to selectively and independently study the spin dynamics of the itinerant 5d and localized 4f electronic subsystems via the suppression of the magnetic (2 1 3–τ) satellite peak. We find demagnetization time scales very similar to ferromagnetic 4f systems, suggesting that the loss of magnetic order occurs via a similar spin-flip process in both cases. The simultaneous demagnetization of both subsystems demonstrates strong intra-atomic 4f–5d exchange coupling. In addition, an ultrafast lattice contraction due to the release of magneto-striction leads to a transient shift of the magnetic satellite peak.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Ultrafast dynamics of localized magnetic moments in the unconventional Mott insulator Sr 2 IrO 4

Here, we report a time-resolved study of the ultrafast dynamics of the magnetic moments formed by the ${{J}_{\text{eff}}}=1/2$ states in Sr 2 IrO 4 by directly probing the localized iridium 5d magnetic state through resonant x-ray diffraction. Using optical pump–hard x-ray probe measurements, two relaxation time scales were determined: a fast fluence-independent relaxation is found to take place on a time scale of 1.5 ps, followed by a slower relaxation on a time scale of 500 ps–1.5 ns.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2015

Nonlinear delayed symmetry breaking in a solid excited by hard x-ray free electron laser pulses

We have studied the ultrafast changes of electronic states in bulk ZnO upon intense hard x-ray excitation from a free electron laser. By monitoring the transient anisotropy induced in an optical probe beam, we observe a delayed breaking of the initial c-plane symmetry of the crystal that lasts for several picoseconds. Interaction with the intense x-ray pulses modifies the electronic state filling in a manner inconsistent with a simple increase in electronic temperature. These results may indicate a way to use intense ultrashort x-ray pulses to investigate high-energy carrier dynamics and to control certain properties of solid-state materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Demonstration of simultaneous experiments using thin crystal multiplexing at the Linac Coherent Light Source

Multiplexing of the Linac Coherent Light Source beam was demonstrated for hard X-rays by spectral division using a near-perfect diamond thin-crystal monochromator operating in the Bragg geometry. The wavefront and coherence properties of both the reflected and transmitted beams were well preserved, thus allowing simultaneous measurements at two separate instruments. In this report, the structure determination of a prototypical protein was performed using serial femtosecond crystallography simultaneously with a femtosecond time-resolved XANES studies of photoexcited spin transition dynamics in an iron spin-crossover system. The results of both experiments using the multiplexed beams are similar to those obtained separately, using a dedicated beam, with no significant differences in quality.

43 PARTICLE ACCELERATORS↗
DOE OSTI2014

Demonstration of Single-Crystal Self-Seeded Two-Color X-Ray Free-Electron Lasers

A scheme for generating two simultaneous hard-x-ray free-electron laser pulses with a controllable difference in photon energy is described and then demonstrated using the self-seeding setup at the Linac Coherent Light Source (LCLS). The scheme takes advantage of the existing LCLS equipment, which allows two independent rotations of the self-seeding diamond crystal. The two degrees of freedom are used to select two nearby crystal reflections, causing two wavelengths to be present in the forward transmitted seeding x-ray pulse. The free-electron laser system must support amplification at both desired wavelengths.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2014

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

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.

43 PARTICLE ACCELERATORS↗
DOE OSTI2014

All-diamond optical assemblies for a beam-multiplexing X-ray monochromator at the Linac Coherent Light Source

A double-crystal diamond (111) monochromator recently implemented at the Linac Coherent Light Source (LCLS) enables splitting of the primary X-ray beam into a pink (transmitted) and a monochromatic (reflected) branch. The first monochromator crystal, with a thickness of ~100 µm, provides sufficient X-ray transmittance to enable simultaneous operation of two beamlines. This article reports the design, fabrication and X-ray characterization of the first and second (300 µm-thick) crystals utilized in the monochromator and the optical assemblies holding these crystals. Each crystal plate has a region of about 5 × 2 mm with low defect concentration, sufficient for use in X-ray optics at the LCLS. The optical assemblies holding the crystals were designed to provide mounting on a rigid substrate and to minimize mounting-induced crystal strain. The induced strain was evaluated using double-crystal X-ray topography and was found to be small over the 5 × 2 mm working regions of the crystals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗