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25 result(s) for "Reis, D.A"
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Femtosecond electronic response of atoms to ultra-intense X-rays
An era of exploring the interactions of high-intensity, hard X-rays with matter has begun with the start-up of a hard-X-ray free-electron laser, the Linac Coherent Light Source (LCLS). Understanding how electrons in matter respond to ultra-intense X-ray radiation is essential for all applications. Here we reveal the nature of the electronic response in a free atom to unprecedented high-intensity, short-wavelength, high-fluence radiation (respectively 10 18  W cm −2 , 1.5–0.6 nm, ∼10 5  X-ray photons per Å 2 ). At this fluence, the neon target inevitably changes during the course of a single femtosecond-duration X-ray pulse—by sequentially ejecting electrons—to produce fully-stripped neon through absorption of six photons. Rapid photoejection of inner-shell electrons produces ‘hollow’ atoms and an intensity-induced X-ray transparency. Such transparency, due to the presence of inner-shell vacancies, can be induced in all atomic, molecular and condensed matter systems at high intensity. Quantitative comparison with theory allows us to extract LCLS fluence and pulse duration. Our successful modelling of X-ray/atom interactions using a straightforward rate equation approach augurs favourably for extension to complex systems. First strike from the LCLS The world's first X-ray free-electron laser — the Linac Coherent Light Source (LCLS) at SLAC National Accelerator Laboratory in Menlo Park, California — came online last year. It opened a new era for studies at the atomic level, including the prospect of single-shot imaging of complex nano-objects such as biological molecules. The results of one of the first user experiments carried out at the LCLS are presented in this issue. The new facility produces ultrashort (femtosecond) pulses of high-intensity X-rays at a wavelength of less than 1.5 nm. The experiment examined the electronic response of free neon atoms to such radiation. During a single X-ray pulse, the atoms sequentially ejected all their ten electrons to produce fully stripped neon — 'hollow' atoms that are X-ray transparent. The authors explain the observations and underlying mechanisms of electron stripping using a straightforward model, which bodes well for further studies of interactions of the X-rays with more complex systems. With the start-up of the first X-ray free-electron laser, a new era has begun in dynamical studies of atoms. Here the facility is used to study the fundamental nature of the electronic response in free neon atoms. During a single X-ray pulse, they sequentially eject all their ten electrons to produce fully stripped neon. The authors explain this electron-stripping in a straightforward model, auguring favourably for further studies of interactions of X-rays with more complex systems.
Atomic-Scale Visualization of Inertial Dynamics
The motion of atoms on interatomic potential energy surfaces is fundamental to the dynamics of liquids and solids. An accelerator-based source of femtosecond x-ray pulses allowed us to follow directly atomic displacements on an optically modified energy landscape, leading eventually to the transition from crystalline solid to disordered liquid. We show that, to first order in time, the dynamics are inertial, and we place constraints on the shape and curvature of the transition-state potential energy surface. Our measurements point toward analogies between this nonequilibrium phase transition and the short-time dynamics intrinsic to equilibrium liquids.
X-ray and optical wave mixing
Light-matter interactions are ubiquitous, and underpin a wide range of basic research fields and applied technologies. Although optical interactions have been intensively studied, their microscopic details are often poorly understood and have so far not been directly measurable. X-ray and optical wave mixing was proposed nearly half a century ago as an atomic-scale probe of optical interactions but has not yet been observed owing to a lack of sufficiently intense X-ray sources. Here we use an X-ray laser to demonstrate X-ray and optical sum-frequency generation. The underlying nonlinearity is a reciprocal-space probe of the optically induced charges and associated microscopic fields that arise in an illuminated material. To within the experimental errors, the measured efficiency is consistent with first- principles calculations of microscopic optical polarization in diamond. The ability to probe optical interactions on the atomic scale offers new opportunities in both basic and applied areas of science.
Ultrafast Bond Softening in Bismuth: Mapping a Solid's Interatomic Potential with X-rays
Intense femtosecond laser excitation can produce transient states of matter that would otherwise be inaccessible to laboratory investigation. At high excitation densities, the interatomic forces that bind solids and determine many of their properties can be substantially altered. Here, we present the detailed mapping of the carrier density-dependent interatomic potential of bismuth approaching a solid-solid phase transition. Our experiments combine stroboscopic techniques that use a high-brightness linear electron accelerator-based x-ray source with pulse-by-pulse timing reconstruction for femtosecond resolution, allowing quantitative characterization of the interatomic potential energy surface of the highly excited solid.
Phase fluctuations and the absence of topological defects in a photo-excited charge-ordered nickelate
The dynamics of an order parameter's amplitude and phase determines the collective behaviour of novel states emerging in complex materials. Time- and momentum-resolved pump-probe spectroscopy, by virtue of measuring material properties at atomic and electronic time scales out of equilibrium, can decouple entangled degrees of freedom by visualizing their corresponding dynamics in the time domain. Here we combine time-resolved femotosecond optical and resonant X-ray diffraction measurements on charge ordered La 1.75 Sr 0.25 NiO 4 to reveal unforeseen photoinduced phase fluctuations of the charge order parameter. Such fluctuations preserve long-range order without creating topological defects, distinct from thermal phase fluctuations near the critical temperature in equilibrium. Importantly, relaxation of the phase fluctuations is found to be an order of magnitude slower than that of the order parameter's amplitude fluctuations, and thus limits charge order recovery. This new aspect of phase fluctuations provides a more holistic view of the phase's importance in ordering phenomena of quantum matter. Time- and momentum-resolved spectroscopy gives dynamical information on complex materials, enabling disentanglement of their coupled degrees of freedom. Using time-resolved X-ray diffraction at a free electron laser, Lee et al . investigate the charge order parameter in a striped nickelate.
Mineral Deposition on the Rough Walls of a Fracture
Modeling carbonate growth in fractures and pores is important for understanding carbon sequestration in the environment or when supersaturated solutions are injected into rocks. Here, we study the simple but nontrivial problem of calcite growth on fractures with rough walls of the same mineral using kinetic Monte Carlo simulations of attachment and detachment of molecules and scaling approaches. First, we consider wedge-shaped fracture walls whose upper terraces are in the same low-energy planes and show that the valleys are slowly filled by the propagation of parallel monolayer steps in the wedge sides. The growth ceases when the walls reach these low-energy configurations so that a gap between the walls may not be filled. Second, we consider fracture walls with equally separated monolayer steps (vicinal surfaces with roughness below 1 nm) and show that growth by step propagation will eventually clog the fracture gap. In both cases, scaling approaches predict the times to attain the final configurations as a function of the initial geometry and the step-propagation velocity, which is set by the saturation index. The same reasoning applied to a random wall geometry shows that step propagation leads to lateral filling of surface valleys until the wall reaches the low-energy crystalline plane that has the smallest initial density of molecules. Thus, the final configurations of the fracture walls are much more sensitive to the crystallography than to the roughness or the local curvature. The framework developed here may be used to determine those configurations, the times to reach them, and the mass of deposited mineral. Effects of transport limitations are discussed when the fracture gap is significantly narrowed.
Temperature Effects in the Initial Stages of Heteroepitaxial Film Growth
Kinetic Monte Carlo simulations of a model of thin film heteroepitaxy are performed to investigate the effects of the deposition temperature in the initial growth stages. Broad ranges of the rates of surface processes are used to model materials with several activation energies and several temperature changes, in conditions of larger diffusivity on the substrate in comparison with other film layers. When films with the same coverage are compared, the roughness increases with the deposition temperature in the regimes of island growth, coalescence, and initial formation of the continuous films. Concomitantly, the position of the minimum of the autocorrelation function is displaced to larger sizes. These apparently universal trends are consequences of the formation of wider and taller islands, and are observed with or without Ehrlich-Schwöebel barriers for adatom diffusion at step edges. The roughness increase with temperature qualitatively matches the observations of recent works on the deposition of inorganic and organic materials. In thicker films, simulations with some parameter sets show the decrease of roughness with temperature. In these cases, a re-entrance of roughness may be observed in the initial formation of the continuous films.
Effects of porosity in a model of corrosion and passive layer growth
We introduce a stochastic lattice model to investigate the effects of pore formation in a passive layer grown with products of metal corrosion. It considers that an anionic species diffuses across that layer and reacts at the corrosion front (metal-oxide interface), producing a random distribution of compact regions and large pores, respectively represented by O (oxide) and P (pore) sites. O sites are assumed to have very small pores, so that the fraction Φ of P sites is an estimate of the porosity, and the ratio between anion diffusion coefficients in those regions is Dr<1. Simulation results without the large pores (Φ=0) are similar to those of a formerly studied model of corrosion and passivation and are explained by a scaling approach. If Φ>0 and Dr≪1, significant changes are observed in passive layer growth and corrosion front roughness. For small Φ, a slowdown of the growth rate is observed, which is interpreted as a consequence of the confinement of anions in isolated pores for long times. However, the presence of large pores near the corrosion front increases the frequency of reactions at those regions, which leads to an increase in the roughness of that front. This model may be a first step to represent defects in a passive layer which favor pitting corrosion.
Coherent control of pulsed X-ray beams
Synchrotrons produce continuous trains of closely spaced X-ray pulses. Application of such sources to the study of atomic-scale motion requires efficient modulation of these beams on timescales ranging from nanoseconds to femtoseconds. However, ultrafast X-ray modulators are not generally available. Here we report efficient subnanosecond coherent switching of synchrotron beams by using acoustic pulses in a crystal to modulate the anomalous low-loss transmission of X-ray pulses. The acoustic excitation transfers energy between two X-ray beams in a time shorter than the synchrotron pulse width of about 100 ps. Gigahertz modulation of the diffracted X-rays is also observed. We report different geometric arrangements, such as a switch based on the collision of two counter-propagating acoustic pulses: this doubles the X-ray modulation frequency, and also provides a means of observing a localized transient strain inside an opaque material. We expect that these techniques could be scaled to produce subpicosecond pulses, through laser-generated coherent optical phonon modulation of X-ray diffraction in crystals. Such ultrafast capabilities have been demonstrated thus far only in laser-generated X-ray sources, or through the use of X-ray streak cameras 1 , 2 , 3 , 4 , 5 , 6 .
Energetics and biomechanics as determining factors of swimming performance: Updating the state of the art
The biophysical determinants related to swimming performance are one of the most attractive topics within swimming science. The aim of this paper was to do an update of the “state of art” about the interplay between performance, energetic and biomechanics in competitive swimming. Throughout the manuscript some recent highlights are described: (i) the relationship between swimmer's segmental kinematics (segmental velocities, stroke length, stroke frequency, stroke index and coordination index) and his center of mass kinematics (swimming velocity and speed fluctuation); (ii) the relationships between energetic (energy expenditure and energy cost) and swimmer's kinematics; and (iii) the prediction of swimming performance derived from above mentioned parameters.