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Fluctuations and stochastic transitions are ubiquitous in nanometre-scale systems, especially in the presence of disorder. However, their direct observation has so far been impeded by a seemingly fundamental, signal-limited compromise between spatial and temporal resolution. Here we develop coherent correlation imaging (CCI) to overcome this dilemma. Our method begins by classifying recorded camera frames in Fourier space. Contrast and spatial resolution emerge by averaging selectively over same-state frames. Temporal resolution down to the acquisition time of a single frame arises independently from an exceptionally low misclassification rate, which we achieve by combining a correlation-based similarity metric1,2 with a modified, iterative hierarchical clustering algorithm3,4. We apply CCI to study previously inaccessible magnetic fluctuations in a highly degenerate magnetic stripe domain state with nanometre-scale resolution. We uncover an intricate network of transitions between more than 30 discrete states. Our spatiotemporal data enable us to reconstruct the pinning energy landscape and to thereby explain the dynamics observed on a microscopic level. CCI massively expands the potential of emerging high-coherence X-ray sources and paves the way for addressing large fundamental questions such as the contribution of pinning5–8 and topology9–12 in phase transitions and the role of spin and charge order fluctuations in high-temperature superconductivity13,14.

The detection and manipulation of antiferromagnetic domains and topological antiferromagnetic textures are of central interest to solid-state physics. A fundamental step is identifying tools to probe the mesoscopic texture of an antiferromagnetic order parameter. In this work, we demonstrate that Bragg coherent diffractive imaging can be extended to study the mesoscopic texture of an antiferromagnetic order parameter using resonant magnetic x-ray scattering. We study the onset of the antiferromagnet transition in PrNiO 3 , focusing on a temperature regime in which the antiferromagnetic domains are dilute in the beam spot and the coherent diffraction pattern modulating the antiferromagnetic peak is greatly simplified. We demonstrate that it is possible to extract the arrangements and sizes of these domains from single diffraction patterns and show that the approach could be extended to a time-structured light source to study the motion of dilute domains or the motion of topological defects in an antiferromagnetic spin texture.

Magnetic domains play a fundamental role in physics of magnetism and its technological applications. Dynamics of antiferromagnetic domains is poorly understood, although antiferromagnets are expected to be extensively used in future electronic devices wherein it determines the stability and operational speed. Dynamics of antiferromagnets also features prominently in the studies of topological quantum matter. Real-space imaging of fluctuating antiferromagnetic domains is therefore highly desired but has never been demonstrated. We use coherent x-ray diffraction to obtain videos of fluctuating micrometer-scale antiferromagnetic domains in Ni 2 MnTeO 6 on time scales from 10 −1 to 10 3 s. In the collinear phase, thermally activated domain wall motion is observed in the vicinity of the Néel temperature. Unexpectedly, the fluctuations persist through the full range of the higher-temperature helical phase. These observations illustrate the high potential significance of the dynamic domain imaging in phase transition studies and in magnetic device research.

While electron-phonon coupling (EPC) is crucial for Cooper pairing in conventional superconductors, its role in high-$T_c$ superconducting cuprates is debated. Using resonant inelastic x-ray scattering at the oxygen $K$-edge, we studied the EPC in Bi$_2$Sr$_2$CaCu$_2$O$_{8+\delta}$ (Bi2212) and Nd$_{1+x}$Ba$_{2-x}$Cu$_3$O$_{7-\delta}$ (NBCO) at different doping levels ranging from heavily underdoped ($p =0.07$) to overdoped ($p=0.21$). We analyze the data with a localized Lang-Firsov model that allows for the coherent excitations of two phonon modes. While electronic band dispersion effects are non-negligible, we are able to perform a study of the relative values of EPC matrix elements in these cuprate families. In the case of NBCO, the choice of the excitation energy allows us to disentangle modes related to the CuO$_3$ chains and the CuO$_2$ planes. Combining the results from the two families, we find the EPC strength decreases with doping at $\mathbf{q_\parallel}=(-0.25, 0)$ r.l.u., but has a non-monotonic trend as a function of doping at smaller momenta. This behavior is attributed to the screening effect of charge carriers. We also find that the phonon intensity is enhanced in the vicinity of the charge-density-wave (CDW) excitations while the extracted EPC strength appears to be less sensitive to their proximity. By performing a comparative study of two cuprate families, we are able to identify general trends in the EPC for the cuprates and provide experimental input to theories invoking a synergistic role for this interaction in $d$-wave pairing., Comment: 10 pages, 5 figures

Recently, rutile ${\mathrm{RuO}}_{2}$ has raised interest for its itinerant antiferromagnetism, crystal Hall effect, and strain-induced superconductivity. Understanding and manipulating these properties demands resolving the electronic structure and the relative roles of the rutile crystal field and $4d$ spin-orbit coupling (SOC). Here, we use O-K and Ru ${M}_{3}$ x-ray absorption and Ru ${M}_{3}$ resonant inelastic x-ray scattering to disentangle the contributions of crystal field, SOC, and electronic correlations in ${\mathrm{RuO}}_{2}$. The locally orthorhombic site symmetry of the Ru ions introduces significant crystal field contributions beyond the approximate octahedral coordination yielding a crystal field energy scale of $\mathrm{\ensuremath{\Delta}}({t}_{2g})\ensuremath{\approx}1\phantom{\rule{0.16em}{0ex}}\mathrm{eV}$ breaking the degeneracy of the ${t}_{2g}$ orbitals. This splitting exceeds the Ru SOC ($\ensuremath{\approx}160$ meV) suggesting a more subtle role of SOC, primarily through the modification of itinerant (rather than local) $4d$ electronic states, ultimately highlighting the importance of the local symmetry in ${\mathrm{RuO}}_{2}$. Remarkably, our analysis can be extended to other members of the rutile family, thus advancing the comprehension of the interplay among crystal field symmetry, electron correlations, and SOC in transition metal compounds with the rutile structure.

Despite mounting evidence that materials imperfections are a major obstacle to practical applications of superconducting qubits, connections between microscopic material properties and qubit coherence are poorly understood. Here, we combine measurements of transmon qubit relaxation times (T1) with spectroscopy and microscopy of the polycrystalline niobium films used in qubit fabrication. By comparing films deposited using three different techniques, we reveal correlations between T1 and intrinsic film properties such as grain size, enhanced oxygen diffusion along grain boundaries, and the concentration of suboxides near the surface. Qubit and resonator measurements show signatures of two-level system defects, which we propose to be hosted in the grain boundaries and surface oxides. We also show that the residual resistance ratio of the polycrystalline niobium films can be used as a figure of merit for qubit lifetime. This comprehensive approach to understanding qubit decoherence charts a pathway for materials-driven improvements of superconducting qubit performance. Understanding the connection between qubit coherence and microscopic materials properties is vital for improving device performance. Here, the relaxation times of superconducting transmon qubits are found to be directly correlated with Nb film properties such as grain size and surface oxide composition.

Like other experimental techniques, X-ray Photon Correlation Spectroscopy is subject to various kinds of noise. Random and correlated fluctuations and heterogeneities can be present in a two-time correlation function and obscure the information about the intrinsic dynamics of a sample. Simultaneously addressing the disparate origins of noise in the experimental data is challenging. We propose a computational approach for improving the signal-to-noise ratio in two-time correlation functions that is based on Convolutional Neural Network Encoder-Decoder (CNN-ED) models. Such models extract features from an image via convolutional layers, project them to a low dimensional space and then reconstruct a clean image from this reduced representation via transposed convolutional layers. Not only are ED models a general tool for random noise removal, but their application to low signal-to-noise data can enhance the data quantitative usage since they are able to learn the functional form of the signal. We demonstrate that the CNN-ED models trained on real-world experimental data help to effectively extract equilibrium dynamics parameters from two-time correlation functions, containing statistical noise and dynamic heterogeneities. Strategies for optimizing the models performance and their applicability limits are discussed., Comment: 5 pages, 10 figures

Although CDW correlations are a ubiquitous feature of the superconducting cuprates, their disparate properties suggest a crucial role for pinning the CDW to the lattice. Here, we report coherent resonant X-ray speckle correlation analysis, which directly determines the reproducibility of CDW domain patterns in La1.875Ba0.125CuO4 (LBCO 1/8) with thermal cycling. While CDW order is only observed below 54 K, where a structural phase transition creates inequivalent Cu-O bonds, we discover remarkably reproducible CDW domain memory upon repeated cycling to far higher temperatures. That memory is only lost on cycling to 240(3) K, which recovers the four-fold symmetry of the CuO2 planes. We infer that the structural features that develop below 240 K determine the CDW pinning landscape below 54 K. This opens a view into the complex coupling between charge and lattice degrees of freedom in superconducting cuprates., The understanding of charge density wave (CDW) correlations in cuprate superconductors remains hampered due to the lack of scattering phase information. Here, Chen et al. discover a reproducible CDW domain memory effect upon repeated cycling to temperatures well above the CDW ordering temperature.

Magnetic frustration can produce exotic spin configurations and dynamics. Here, the authors explore the seemingly simple competition between ferromagnetic nearest- and antiferromagnetic next-nearest neighbor interactions along Ising spin chains, as realized in the magnetoelectric compound Lu${}_{2}$CoMnO${}_{6}$. Commonly, this situation is described by the axial next-nearest-neighbor Ising model. For the first time, the authors measure and calculate its correlated magnetic dynamics, resulting from a characteristic fractal set of first-order phase boundaries. Experiments and Monte Carlo simulations reveal a dynamics slowdown while approaching the phase transition regime.

Revealing the predominant driving force behind symmetry breaking in correlated materials is sometimes a formidable task due to the intertwined nature of different degrees of freedom. This is the case for La2-xSrxNiO4+{\delta} in which coupled incommensurate charge and spin stripes form at low temperatures. Here, we use resonant X-ray photon correlation spectroscopy to study the temporal stability and domain memory of the charge and spin stripes in La2-xSrxNiO4+{\delta}. Although spin stripes are more spatially correlated, charge stripes maintain a better temporal stability against temperature change. More intriguingly, charge order shows robust domain memory with thermal cycling up to 250 K, far above the ordering temperature. These results demonstrate the pinning of charge stripes to the lattice and that charge condensation is the predominant factor in the formation of stripe orders in nickelates., Comment: 7 pages; accepted in Physical Review Letters

Charge density wave (CDW) correlations are prevalent in all copper-oxide superconductors. While CDWs in conventional metals are driven by coupling between lattice vibrations and electrons, the role of the electron-phonon coupling (EPC) in cuprate CDWs is strongly debated. Using Cu ${L}_{3}$ edge resonant inelastic x-ray scattering, we study the CDW and Cu-O bond-stretching phonons in the stripe-ordered cuprate ${\mathrm{La}}_{1.8\ensuremath{-}x}{\mathrm{Eu}}_{0.2}{\mathrm{Sr}}_{x}{\mathrm{CuO}}_{4+\ensuremath{\delta}}$. We investigate the interplay between charge order and EPC as a function of doping and temperature and find that the EPC is enhanced in a narrow momentum region around the CDW ordering vector. By detuning the incident photon energy from the absorption resonance, we extract an EPC matrix element at the CDW ordering vector of $M\ensuremath{\simeq}0.36\text{ }\text{ }\mathrm{eV}$, which decreases to $M\ensuremath{\simeq}0.30\text{ }\text{ }\mathrm{eV}$ at high temperature in the absence of the CDW. Our results suggest a feedback mechanism in which the CDW enhances the EPC which, in turn, further stabilizes the CDW.

The discovery of charge-density-wave-related effects in the resonant inelastic x-ray scattering spectra of cuprates holds the tantalizing promise of clarifying the interactions that stabilize the electronic order. Here, we report a comprehensive resonant inelastic x-ray scattering study of La_{2-x}Sr_{x}CuO_{4} finding that charge-density wave effects persist up to a remarkably high doping level of x=0.21 before disappearing at x=0.25. The inelastic excitation spectra remain essentially unchanged with doping despite crossing a topological transition in the Fermi surface. This indicates that the spectra contain little or no direct coupling to electronic excitations near the Fermi surface, rather they are dominated by the resonant cross section for phonons and charge-density-wave-induced phonon softening. We interpret our results in terms of a charge-density wave that is generated by strong correlations and a phonon response that is driven by the charge-density-wave-induced modification of the lattice.

Spin excitations of magnetic thin films are the founding element for novel transport concepts in spintronics, magnonics, and magnetic devices in general. While spin dynamics have been extensively studied in bulk materials, their behaviour in mesoscopic films is less known due to experimental limitations. Here, we employ Resonant Inelastic X-Ray Scattering to investigate the spin excitation spectrum in mesoscopic Fe films, from bulk-like down to 3 unit cells thick. In bulk-like samples, we find isotropic, dispersive ferromagnons consistent with the dispersion observed by neutron scattering in bulk single crystals. As the thickness is reduced, these ferromagnons survive and evolve anisotropically: renormalising to lower energies along the out-of-plane direction while retaining their dispersion in the in-plane direction. This thickness dependence is captured by simple Heisenberg model calculations accounting for the confinement in the out-of-plane direction through the loss of Fe bonds. Our findings highlight the effects of mesoscopic scaling on spin dynamics and identify thickness as a knob for fine-tuning and controlling magnetic properties in films., Comment: 17 pages, 4, figure, submitted

Ru M3-edge resonant inelastic x-ray scattering (RIXS) measurements of with 27 meV resolution reveals a spin–orbit exciton without noticeable splitting. We extract values for the spin–orbit coupling constant ( meV) and trigonal distortion field energy ( meV) which support the nature of . We demonstrate the feasibility of M-edge RIXS for 4d systems, which allows ultra high-resolution RIXS of 4d systems until instrumentation for L-edge RIXS improves.

Charge density waves (CDWs) in the cuprate high-temperature superconductors have evoked much interest, yet their typical short-range nature has raised questions regarding the role of disorder. Here we report a resonant X-ray diffraction study of ZrTe\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${}_{3}$$\end{document}3, a model CDW system, with focus on the influence of disorder. Near the CDW transition temperature, we observe two independent signals that arise concomitantly, only to become clearly separated in momentum while developing very different correlation lengths in the well-ordered state that is reached at a distinctly lower temperature. Anomalously slow dynamics of mesoscopic charge domains are further found near the transition temperature, in spite of the expected strong thermal fluctuations. Our observations signify the presence of distinct experimental fingerprints of pristine and disorder-perturbed CDWs. We discuss the latter also in the context of Friedel oscillations, which we argue might promote CDW formation via a self-amplifying process., The role of disorder in the formation of charge density waves (CDWs) remains elusive in typical CDW materials. Here, the authors report coexisting diffraction signals and anomalous slow dynamics of charge domains near the CDW transition temperature in ZrTe\documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${}_{3}$$\end{document}3, suggesting as fingerprints of pristine and disorder-perturbed CDWs.

We describe the current and future plans for using artificial intelligence and machine learning (AI/ML) methods at the National Synchrotron Light Source II (NSLS-II), a scientific user facility at the Brookhaven National Laboratory. We discuss the opportunity for using the AI/ML tools and techniques developed in the data and computational science areas to greatly improve the scientific output of large scale experimental user facilities. We describe our current and future plans in areas including from detecting and recovering from faults, optimizing the source and instrument configurations, streamlining the pipeline from measurement to insight, through data acquisition, processing, analysis. The overall strategy and direction of the NSLS-II facility in relation to AI/ML is presented.

Electron Multiplying Charge Coupled Devices, EMCCD are used as x-ray detectors. The NSLS-II Soft Inelastic x-ray Scattering (SIX) beam line has two EMCCDs for x-ray detection in the spectrometer arm. The spectrometer with high resolving power disperses x-rays vertically. The x-ray vertical position on the sensor plane is related to its energy. This allows for very accurate x-ray energy measurements through x-ray coordinates. X-rays interact with silicon and create a number of electron–hole pairs proportional to the x-ray energy. Electrons drift and diffuse toward pixel gates and are collected there. The diffused electrons form a charge cloud distributed over several neighboring pixels. This charge sharing enables coordinate measurements with accuracy better than the pixel pitch. The charge distribution shape has to be taken into account to achieve ultimate accuracy in coordinate measurements. In this paper, we present a method of the charge distribution shape analysis and demonstrate its applications. The drift and diffusion of electrons from the point of generation to pixel gates results in the bell-shaped electron cloud usually approximated by Gaussian shape. The number of electrons collected under a pixel is proportional to the shape function integral. These electron packets get transferred to the sense node of the output amplifier. The transfer process could introduce distortions to the original charge distribution. For example, during transfers, electrons in the packet could be exposed to traps if they are present in the sensor. The trapping and later the release processes distort the apparent shape of the charge distribution. Therefore, deviations of the charge distribution shape from the originally symmetrical form can indicate the presence of trap centers in the sensor and can be used for sensor diagnostics.

Kinetics of molecular oxygen / Au (001) surface interaction has been studied at high temperature and near atmospheric pressures of O2 gas with in situ x-ray scattering measurements. We find that the hexagonal reconstruction (hex) of Au (001) surface lifts to (1x1) in the presence of O2 gas, indicating that the (1x1) is more favored when some oxygen atoms present on the surface. The measured lifting rate constant vs. temperature is found to be highest at intermediate temperature exhibiting a 'volcano'-type behavior. At low temperature, the hex-to-(1x1) activation barrier (Eact = 1.3(3) eV) limits the lifting. At high temperature, oxygen adsorption energy (Eads = 1.6(2) eV) limits the lifting. The (1x1)-to-hex activation barrier (Ehex = 0.41(14) eV) is also obtained from hex recovery kinetics. The pressure-temperature (PT) surface phase diagram obtained in this study shows three regions: hex at low P and T, (1x1) at high P and T, and coexistence of the hex and (1x1) at the intermediate P and T., Comment: 27 pages, 10 figures, submitted J. Phys. Chem. C

The oxidation and reduction of Ru(0001) surfaces at the confined space between two-dimensional nanoporous silica frameworks and Ru(0001) have been investigated using synchrotron-based ambient pressure X-ray photoelectron spectroscopy (AP-XPS). The porous nature of the frameworks and the weak interaction between the silica and the ruthenium substrate allow oxygen and hydrogen molecules to go through the nanopores and react with the metal at the interface between the silica framework and the metal surface. In this work, three types of two-dimensional silica frameworks have been used to study their influence in the oxidation and reduction of the ruthenium surface at elevated pressures and temperatures. These frameworks are bilayer silica (0.5 nm thick), bilayer aluminosilicate (0.5 nm thick), and zeolite MFI nanosheets (3 nm thick). It is found that the silica frameworks stay essentially intact under these conditions, but they strongly affect the oxidation of ruthenium, with the 0.5 nm thick aluminosilicate ...

We present X-ray crystal truncation rods measurements of Pt(111) surface under electrochemical conditions. Analyses of crystal truncation rods reveal that surface oxide formation buckles the top surface layer of platinum to two different heights at the potential (0.95 V vs RHE) below the so-called place-exchange potential. While the anti-Bragg intensity, sensitive to the top surface layer, drops in response to the anodic charge transfers, its responses to the cathodic charge transfers are significantly delayed. Implications to the surface oxidation and reduction behaviors are discussed.

Manipulating magnetic domains is essential for many technological applications. Recent breakthroughs in Antiferromagnetic Spintronics brought up novel concepts for electronic device development. Imaging antiferromagnetic domains is of key importance to this field. Unfortunately, some of the basic domain types, such as antiphase domains, cannot be imaged by conventional techniques. Herein, we present a new domain projection imaging technique based on the localization of domain boundaries by resonant magnetic diffraction of coherent X rays. Contrast arises from reduction of the scattered intensity at the domain boundaries due to destructive interference effects. We demonstrate this approach by imaging antiphase domains in a collinear antiferromagnet Fe2Mo3O8, and observe evidence of domain wall interaction with a structural defect. This technique does not involve any numerical algorithms. It is fast, sensitive, produces large-scale images in a single-exposure measurement, and is applicable to a variety of magnetic domain types., Imaging the antiferromagnetic (AFM) domains facilitates the understanding and design of AFM spintronics but is still challenging. Here the authors show an imaging approach for antiphase domains in AFM Fe2Mo3O8 by resonantly scattered coherent soft X-rays, which is also applicable to collinear antiferromagnets.

The metal-insulator phase transition in magnetite, known as the Verwey transition, is characterized by a charge-orbital ordering and a lattice transformation from a cubic to monoclinic structure. We use $x$-ray photon correlation spectroscopy to investigate the dynamics of this charge-orbitally ordered insulating phase undergoing the insulator-to-metal transition. By tuning to the Fe ${L}_{3}$ edge at the $(00\frac{1}{2})$ superlattice peak, we probe the evolution of the Fe ${t}_{2g}$ orbitally ordered domains present in the low temperature insulating phase and forbidden in the high temperature metallic phase. We observe two distinct regimes below the Verwey transition. In the first regime, magnetite follows an Arrhenius behavior and the characteristic timescale for orbital fluctuations decreases as the temperature increases. In the second regime, magnetite phase separates into metallic and insulating domains, and the kinetics of the phase transition is dictated by metallic-insulating interfacial boundary conditions.

The applied potential dependent rate of atomic step motion of the Ag(001) surface in weak NaF electrolyte has been measured using a new extension of the technique of X-ray Photon Correlation Spectroscopy (XPCS). For applied potentials between hydrogen evolution and oxidation, the surface configuration completely changes on timescales of 10(2)-10(4) seconds depending upon the applied potential. These dynamics, directly measured over large areas of the sample surface simultaneously, are related to the surface energy relative to over or under potential. Concurrent specular X-ray scattering measurements reveal how the ordering of the water layers at the interface correlates with the dynamics.

A central characteristic of living beings is the ability to learn from and respond to their environment leading to habit formation and decision making. This behavior, known as habituation, is universal among all forms of life with a central nervous system, and is also observed in single-cell organisms that do not possess a brain. Here, we report the discovery of habituation-based plasticity utilizing a perovskite quantum system by dynamical modulation of electron localization. Microscopic mechanisms and pathways that enable this organismic collective charge-lattice interaction are elucidated by first-principles theory, synchrotron investigations, ab initio molecular dynamics simulations, and in situ environmental breathing studies. We implement a learning algorithm inspired by the conductance relaxation behavior of perovskites that naturally incorporates habituation, and demonstrate learning to forget: A key feature of animal and human brains. Incorporating this elementary skill in learning boosts the capability of neural computing in a sequential, dynamic environment., United States. Army Research Office (Grant W911NF-16-1-0289), United States. Air Force Office of Scientific Research (Grant FA9550-16-1-0159), United States. Army Research Office (Grant W911NF-16-1-0042)

Charge-density-wave (CDW) correlations feature prominently in the phase diagram of the cuprates, motivating competing theories of whether fluctuating CDW correlations aid superconductivity or whether static CDW order coexists with superconductivity in inhomogeneous or spatially modulated states. Here we report Cu L-edge resonant x-ray photon correlation spectroscopy measurements of CDW correlations in superconducting La2−xBaxCuO4, x = 0.11. Static CDW order is shown to exist in the superconducting state at low temperatures and to persist up to at least 85% of the CDW transition temperature. We discuss the implications of our observations for how nominally competing order parameters can coexist in the cuprates.

The occurrence of charge-density-wave (CDW) order in underdoped cuprates is now well established, although the precise nature of the CDW and its relationship with superconductivity is not. Theoretical proposals include contrasting ideas such as that pairing may be driven by CDW fluctuations or that static CDWs may intertwine with a spatially modulated superconducting wave function. We test the dynamics of CDW order in ${\mathrm{La}}_{1.825}{\mathrm{Ba}}_{0.125}{\mathrm{CuO}}_{4}$ by using x-ray photon correlation spectroscopy at the CDW wave vector, detected resonantly at the Cu ${L}_{3}$ edge. We find that the CDW domains are strikingly static, with no evidence of significant fluctuations up to $2\text{ }\textthreequarters{}\text{ }\text{ }\mathrm{h}$. We discuss the implications of these results for some of the competing theories.

Ferroelectric transitions of a hexagonal multiferroic, $\mathrm{ErMn}{\mathrm{O}}_{3}$, are studied by x-ray scattering techniques. An isosymmetry transition, similar to that previously observed for $\mathrm{YMn}{\mathrm{O}}_{3}$, approximately 300 K below the well-known ferroic transition temperature, is investigated. The partially glassy behavior of the isosymmetry transition is identified by the appearance of quasielastic scattering lines in high-energy-resolution scans. The glassy behavior is further supported by the increased interlayer decorrelation of $(\sqrt{3}\ifmmode\times\else\texttimes\fi{}\sqrt{3})R{30}^{\ensuremath{\circ}}$ ordering below the isosymmetry transition. The transition behavior is considered for possible hidden sluggish modes and two-step phase transitions theoretically predicted for the stacked triangular antiferromagnets. The in-plane azimuthal (orientational) ordering behaviors were also compared to the theoretical predictions. Coherent x-ray speckle measurements show unambiguously that the domain sizes decrease anomalously near both the isosymmetry and ferroic transitions. However, domain boundary fluctuations increase monotonically with an Arrhenius form with an activation energy of 0.54(5) eV through both transitions.

We present the results of a series of coherent x-ray scattering temperature-dependent experiments from Pt(001) in high vacuum. The resulting speckled diffraction patterns are analyzed with x-ray photon correlation spectroscopy. We find that the hexagonally reconstructed Pt(001) surface exhibits orientational dynamics below 1640 K and a critical behavior as $T$ increases to ${T}_{\mathrm{R}}$ $=$ 1834 K, near the roughening transition, as proposed by Abernathy et al. [Phys. Rev. Lett. 69, 941 (1992)]. The inverse autocorrelation time constant ${\ensuremath{\tau}}^{\ensuremath{-}1}$ of the surface diverges as $T$ approaches ${T}_{\mathrm{R}}$. The average integrated intensity remains constant below ${T}_{\mathrm{R}}$ but drops suddenly over a narrow temperature range, indicating abrupt lifting of the hexagonal reconstruction with the roughening transition. This behavior is compared to that of Au(001), for which ${\ensuremath{\tau}}^{\ensuremath{-}1}$ approaches a finite value as the reconstruction lifts gradually over a wide temperature range.

We have performed coherent x-ray scattering experiments on the hexagonally reconstructed Pt (001) surface to study the temperature-dependent surface dynamics. By correlating speckle patterns collected at the (001) anti-Bragg position we are able to measure surface dynamics when the averaged incoherent x-ray scattering appears static. In the temperature range above the rotational epitaxy transition and below the roughening transition (1750 K - 1830 K), we have observed well-defined oscillatory autocorrelations of speckles that persist for tens of minutes, in addition to the expected thermal decorrelation. The observed oscillations indicate surface dynamics due to "step-flow" motion. This is shown with a simple model in which the phase of the scattered x-rays from the steps within the illumination area is retained in the coherent x-ray scattering. This demonstrates a possibility that x-ray speckles can be used to monitor the real-space real-time evolution of surfaces in addition to the traditional decorrelation measurements., Comment: 12 pages, 3 figures

It has long been conceived that in equilibrium electrode surfaces in contact with electrolytes remain highly dynamic, exhibiting steady processes such as detachment and adsorption of surface atoms. Importantly, some of those microstate fluctuations play an essential role on formation of surface structure and composition, and ultimately affect the functionality of electrodes. Surface-sensitive techniques, like STM and surface x-ray scattering (SXS), have become invaluable to unraveling electrode surface structures under changing electrochemical environments. Measurements on surface dynamics, however, remain challenging for electrochemical systems [[1]]. In this talk, we will report on the study of Au (111) surface dynamics by coherent surface x-ray scattering (CSXS). A brief introduction will be given for implementation of CSXS and ISXS for electrochemical studies. Time-resolved capability of CSXS will be highlighted. To elucidate factors that could influence surface dynamics, Au (111) electrode surfaces are systemically tailored by varying electrochemical conditions. Phase transition in Au (111) electrode surface had been well characterized by SXS, with structural changes that were shown to be both dependent on potentials and solution chemistry [[2]]. A sharp drop in x-ray scattering intensity around 0.12 V, shown in Fig. 1 (black curve), marks phase transition from (p x√3) to (1x1), which then can be reconstructed back to form a (p x√3) structure in a reverse potential scan. A similar potential dependence is found with increasing chloride concentration as shown in Fig. 1 (red curve). Careful comparison of the hysteresis loops, presented in Fig. 1, additionally reveals that chloride concentration influences the kinetics of phase transition in Au (111) surfaces. In additional to structural details, we have also attained some preliminary results on the dynamics of Au (111) surfaces from CSXS experiments. In the present work, surface dynamics are quantified in terms of correlation time, a parameter that describes the temporal separation between two configurations that are no longer resemble each other due to microstate fluctuations. Correlation time in relation to surface structure will be shown and discussed as a function of applied potential and chloride concentration. A comprehensive analysis on surface dynamics will be performed to help establish its relations with surface structure and solution chemistry. [1] M. Pierce, V. Komanicky, A. Barbour, D. C. Hennessy, C. Zhu, A. Sandy, H. You, Phys. Rev. B 86, 085410 (2012). [2] J. Wang, B.M. Ocko, A. J. Davenport, H. S. Isaacs, Phys. Rev. B 46 10321 (1992). Figure 1

Ptychography is a high-resolution imaging technique, which does not require lenses for image magnification and which provides phase contrast with high sensitivity. Here, we propose to use x-ray ptychography for the imaging of surface structure in crystalline samples. We show that ptychography can be used to image atomic step structures using coherent diffraction patterns recorded along the crystal truncation rod of a crystal surface. In a proof-of-concept experiment on a Pt (111) sample, we present ptychographic reconstructions showing features consistent with surface steps. Due to the penetration power of x-rays, this method could find interesting applications for the study of surface structures under buried interfaces or in harsh environments.

We report a joint experimental and theoretical investigation of the transport gap, optical properties, and electronic structure of two chemically similar, inhomogeneously mixed-valent polyoxovanadate molecule-based magnets. We attribute the substantial gap in $[{\mathrm{NHEt}}_{3}{]}_{4}[{\mathrm{V}}_{8}^{\mathrm{IV}}{\mathrm{V}}_{4}^{\mathrm{V}}{\mathrm{As}}_{8}{\mathrm{O}}_{40}({\mathrm{H}}_{2}\mathrm{O})]∙{\mathrm{H}}_{2}\mathrm{O}$ to weak $p\text{\ensuremath{-}}d$ hybridization and a large on-site Coulomb repulsion $(U=6\phantom{\rule{0.3em}{0ex}}\mathrm{eV})$. The reduced gap in $[{\mathrm{NHEt}}_{3}{]}_{3}[{\mathrm{V}}_{6}^{\mathrm{IV}}{\mathrm{V}}_{6}^{\mathrm{V}}{\mathrm{As}}_{8}{\mathrm{O}}_{40}({\mathrm{HCO}}_{2})]∙2{\mathrm{H}}_{2}\mathrm{O}$ is associated with a smaller value of $U$ $(4\phantom{\rule{0.3em}{0ex}}\mathrm{eV})$, at least from a molecular point of view, although the transport properties also reflect subtle organization of the molecular structure and differences between direct and indirect intermolecular charge transfer. A detailed analysis of the vibrational response supports the important role of local molecular distortions and hydrogen bonding in the intramolecular and intermolecular charge transport of $[{\mathrm{NHEt}}_{3}{]}_{4}[{\mathrm{V}}_{8}^{\mathrm{IV}}{\mathrm{V}}_{4}^{\mathrm{V}}{\mathrm{As}}_{8}{\mathrm{O}}_{40}({\mathrm{H}}_{2}\mathrm{O})]∙{\mathrm{H}}_{2}\mathrm{O}$.

In the above article the name of one of the authors has been mistyped. The correct name of the author is D. Fernandez-Canoto.

not Available.

We observed an epitaxial, air-stable, partially registered (2 × 1) oxide bilayer on Pt (001) nanofacets [V. Komanicky, A. Menzel, K.-C. Chang, and H. You, J. Phys. Chem. 109, 23543 (2005)]. The bilayer is made of two half Pt layers; the top layer has four oxygen bonds and the second layer two. The positions and oxidation states of the Pt atoms are determined by analyzing crystal truncation rods and resonance scattering data. The positions of oxygen atoms are determined by density functional theory (DFT) calculations. Partial registry on the nanofacets and the absence of such registry on the extended Pt (001) surface prepared similarly are explained in DFT calculations by strain relief that can be accommodated only by nanoscale facets.

We developed a method for production of arrays of platinum nanocrystals of controlled size and shape using templates from ordered silica bead monolayers. Silica beads with nominal sizes of 150 and 450 nm were self-assembled into monolayers over strontium titanate single crystal substrates. The monolayers were used as shadow masks for platinum metal deposition on the substrate using the three-step evaporation technique. Produced arrays of epitaxial platinum islands were transformed into nanocrystals by annealing in a quartz tube in nitrogen flow. The shape of particles is determined by the substrate crystallography, while the size of the particles and their spacing are controlled by the size of the silica beads in the monolayer mask. As a proof of concept, arrays of platinum nanocrystals of cubooctahedral shape were prepared on (100) strontium titanate substrates. The nanocrystal arrays were characterized by atomic force microscopy, scanning electron microscopy, and synchrotron X-ray diffraction techniques.