Anisotropic structural dynamics of monolayer crystals revealed by femtosecond surface x-ray scattering

X-ray scattering is one of the primary tools to determine crystallographic configuration with atomic accuracy. However, the measurement of ultrafast structural dynamics in monolayer crystals remains a long-standing challenge due to a significant reduction of diffraction volume and complexity of data analysis, prohibiting the application of ultrafast x-ray scattering to study nonequilibrium structural properties at the two-dimensional limit. Here, we demonstrate femtosecond surface x-ray diffraction in combination with crystallographic model-refinement calculations to quantify the ultrafast structural dynamics of monolayer WSe$_2$ crystals supported on a substrate. We found the absorbed optical photon energy is preferably coupled to the in-plane lattice vibrations within 2 picoseconds while the out-of-plane lattice vibration amplitude remains unchanged during the first 10 picoseconds. The model-assisted fitting suggests an asymmetric intralayer spacing change upon excitation. The observed nonequilibrium anisotropic structural dynamics in two-dimensional materials agrees with first-principles nonadiabatic modeling in both real and momentum space, marking the distinct structural dynamics of monolayer crystals from their bulk counterparts. The demonstrated methods unlock the benefit of surface sensitive x-ray scattering to quantitatively measure ultrafast structural dynamics in atomically thin materials and across interfaces

Primary structural dynamics in graphite

The structural dynamics of graphite and graphene are unique, because of the selective coupling between electron and lattice motions and hence the limit on electric and electro-optic properties. Here, we report on the femtosecond probing of graphite films (1–3 nm) using ultrafast electron crystallography in the transmission mode. Two time scales are observed for the dynamics: a 700 fs initial decrease in diffraction intensity due to lattice phonons in optically dark regions of the Brillouin zone, followed by a 12 ps decrease due to phonon thermalization near the Г and K regions. These results indicate the non-equilibrium distortion of the unit cells at early time and the subsequent role of long-wavelength atomic motions in the thermalization process. Theory and experiment are now in agreement regarding the nature of nuclear motions, but the results suggest that potential change plays a role in the lateral dynamics of the lattice

Predicting protein dynamics from structural ensembles

The biological properties of proteins are uniquely determined by their structure and dynamics. A protein in solution populates a structural ensemble of metastable configurations around the global fold. From overall rotation to local fluctuations, the dynamics of proteins can cover several orders of magnitude in time scales. We propose a simulation-free coarse-grained approach which utilizes knowledge of the important metastable folded states of the protein to predict the protein dynamics. This approach is based upon the Langevin Equation for Protein Dynamics (LE4PD), a Langevin formalism in the coordinates of the protein backbone. The linear modes of this Langevin formalism organize the fluctuations of the protein, so that more extended dynamical cooperativity relates to increasing energy barriers to mode diffusion. The accuracy of the LE4PD is verified by analyzing the predicted dynamics across a set of seven different proteins for which both relaxation data and NMR solution structures are available. Using experimental NMR conformers as the input structural ensembles, LE4PD predicts quantitatively accurate results, with correlation coefficient \r{ho} = .93 to NMR backbone relaxation measurements for the seven proteins. The NMR solution structure derived ensemble and predicted dynamical relaxation is compared with molecular dy- namics simulation-derived structural ensembles and LE4PD predictions, and are consistent in the timescale of the simulations. The use of the experimental NMR conformers frees the approach from computationally demanding simulations

Lectures on Structural Stability in Dynamics

These lectures present results and problems on the characterization of structurally stable dynamics. We will shed light those which do not seem to depend on the regularity class (holomorphic or differentiable). Furthermore, we will present some links between the problems of structural stability in dynamical systems and in singularity theory.Comment: 30pages and 9 figure

Structural dynamics verification facility study

The need for a structural dynamics verification facility to support structures programs was studied. Most of the industry operated facilities are used for highly focused research, component development, and problem solving, and are not used for the generic understanding of the coupled dynamic response of major engine subsystems. Capabilities for the proposed facility include: the ability to both excite and measure coupled structural dynamic response of elastic blades on elastic shafting, the mechanical simulation of various dynamical loadings representative of those seen in operating engines, and the measurement of engine dynamic deflections and interface forces caused by alternative engine mounting configurations and compliances

SPS structural dynamics and control workshop: Findings and recommendations

The structural dynamics and control of the Solar Power Satellite (SPS), a concept which holds promise for meeting a portion of the energy needs of the United States beyond the year 2000 are examined. The assumptions, methodologies and conclusions of existing SPS studies in the areas of structural dynamics and control (with structural design and materials also being considered) are assessed

Fractional Integration and Structural Breaks in U.S. Macro Dynamics

This paper identifies structural breaks in the post-World War II joint dynamics of U.S. inflation, unemployment and the short-term interest rate. We derive a structural break-date procedure which allows for long-memory behavior in all three series and perform the analysis for alternative data frequencies. Both long-memory and short-run coefficients are relevant for characterizing the changing patterns of U.S. macroeconomic dynamics. We provide an economic interpretation of those changes by examining the link between macroeconomic events and structural breaks.Fractional integration, structural breaks, multivariate analysis, inflation dynamics

Structural Dynamics of Free Proteins in Diffraction

Among the macromolecular patterns of biological significance, right-handed α-helices are perhaps the most abundant structural motifs. Here, guided by experimental findings, we discuss both ultrafast initial steps and longer-time-scale structural dynamics of helix-coil transitions induced by a range of temperature jumps in large, isolated macromolecular ensembles of an α-helical protein segment thymosin β_9 (Tβ_9), and elucidate the comprehensive picture of (un)folding. In continuation of an earlier theoretical work from this laboratory that utilized a simplistic structure-scrambling algorithm combined with a variety of self-avoidance thresholds to approximately model helix-coil transitions in Tβ_9, in the present contribution we focus on the actual dynamics of unfolding as obtained from massively distributed ensemble-convergent MD simulations which provide an unprecedented scope of information on the nature of transient macromolecular structures, and with atomic-scale spatiotemporal resolution. In addition to the use of radial distribution functions of ultrafast electron diffraction (UED) simulations in gaining an insight into the elementary steps of conformational interconversions, we also investigate the structural dynamics of the protein via the native (α-helical) hydrogen bonding contact metric which is an intuitive coarse graining approach. Importantly, the decay of α-helical motifs and the (globular) conformational annealing in Tβ_9 occur consecutively or competitively, depending on the magnitude of temperature jump