Proc Natl Acad Sci U S A
January 2025
A central paradigm of nonequilibrium physics concerns the dynamics of heterogeneity and disorder, impacting processes ranging from the behavior of glasses to the emergent functionality of active matter. Understanding these complex mesoscopic systems requires probing the microscopic trajectories associated with irreversible processes, the role of fluctuations and entropy growth, and the timescales on which nonequilibrium responses are ultimately maintained. Approaches that illuminate these processes in model systems may enable a more general understanding of other heterogeneous nonequilibrium phenomena, and potentially define ultimate speed and energy cost limits for information processing technologies.
View Article and Find Full Text PDFIn unconventional superconductors, coupled charge and lattice degrees of freedom can manifest in ordered phases of matter that are intertwined. In the cuprate family, fluctuating short-range charge correlations can coalesce into a longer-range charge density wave (CDW) order which is thought to intertwine with superconductivity, yet the nature of the interaction is still poorly understood. Here, by measuring subtle lattice fluctuations in underdoped YBaCuO on quasi-static timescales (thousands of seconds) through X-ray photon correlation spectroscopy, we report sensitivity to both superconductivity and CDW.
View Article and Find Full Text PDFUnderstanding the interplay between charge, nematic, and structural ordering tendencies in cuprate superconductors is critical to unraveling their complex phase diagram. Using pump-probe time-resolved resonant X-ray scattering on the (0 0 1) Bragg peak at the Cu [Formula: see text] and O [Formula: see text] resonances, we investigate nonequilibrium dynamics of [Formula: see text] nematic order and its association with both charge density wave (CDW) order and lattice dynamics in La[Formula: see text]Eu[Formula: see text]Sr[Formula: see text]CuO[Formula: see text]. The orbital selectivity of the resonant X-ray scattering cross-section allows nematicity dynamics associated with the planar O 2[Formula: see text] and Cu 3[Formula: see text] states to be distinguished from the response of anisotropic lattice distortions.
View Article and Find Full Text PDFThe mechanism(s) through which child contact can lead to more positive mental health and romantic relationship outcomes among incarcerated fathers are not sufficiently studied. The present study tests whether the associations between frequency of child contact and later psychological distress and conflict in romantic relationships are mediated by perceived social support. Self-reported longitudinal data from a sample of incarcerated men who participated in a fatherhood education program ( = 2,096) were analyzed using structural equation modeling.
View Article and Find Full Text PDFUnderstanding the nature and origin of collective excitations in materials is of fundamental importance for unraveling the underlying physics of a many-body system. Excitation spectra are usually obtained by measuring the dynamical structure factor, S(Q, ω), using inelastic neutron or x-ray scattering techniques and are analyzed by comparing the experimental results against calculated predictions. We introduce a data-driven analysis tool which leverages 'neural implicit representations' that are specifically tailored for handling spectrographic measurements and are able to efficiently obtain unknown parameters from experimental data via automatic differentiation.
View Article and Find Full Text PDFIntroduction: Economic distress and the relationship stability of remarried couples has been subject to some exploration, but less emphasis has been placed on how economic distress among remarried couples impacts other relationship domains, particularly sexual intimacy.
Methods: Through the lens of multidimensional family development theory (MFDT), this study utilizes longitudinal data over a three-year period to examine the links between economic distress, couple engagement, relationship satisfaction, and perceptions of sexual intimacy among remarried couples ( = 1,161 couples; 97% White).
Results: Through a dyadic structural equation model, results showed that wives' report of economic distress was directly related to their self-rejection of a partner's sexual advances.
Little research has examined the potential spillover of parenting difficulties in the coparental stepfamily subsystem. Using family systems theory as a guide, we longitudinally examined: (a) whether early parenting difficulties within stepfamilies persist 1 year later and (b) whether the parenting difficulties experienced by one partner impact the parenting difficulties of the other partner within remarriages. Copies of marriage licenses were used to identify remarried individuals.
View Article and Find Full Text PDFX-ray Free Electron Lasers provide femtosecond x-ray pulses with narrow bandwidth and unprecedented peak brightness. Special modes of operation have been developed to deliver double pulses for x-ray pump, x-ray probe experiments. However, the longest delay between the two pulses achieved with existing single bucket methods is less than 1 picosecond, thus preventing the exploration of longer time-scale dynamics.
View Article and Find Full Text PDFWe demonstrate for the case of photoexcited [Ru(2,2'-bipyridine)] how femtosecond resonant inelastic X-ray scattering (RIXS) at the ligand K-edge allows one to uniquely probe changes in the valence electronic structure following a metal-to-ligand charge-transfer (MLCT) excitation. Metal-ligand hybridization is probed by nitrogen-1s resonances providing information on both the electron-accepting ligand in the MLCT state and the hole density of the metal center. By comparing to spectrum calculations based on density functional theory, we are able to distinguish the electronic structure of the electron-accepting ligand and the other ligands and determine a temporal upper limit of (250 ± 40) fs for electron localization following the charge-transfer excitation.
View Article and Find Full Text PDFWe design and realize an arrival time diagnostic for ultrashort X-ray pulses achieving unprecedented high sensitivity in the soft X-ray regime via cross-correlation with a ≈1550 nm optical laser. An interferometric detection scheme is combined with a multi-layer sample design to greatly improve the sensitivity of the measurement. We achieve up to 275% of relative signal change when exposed to 1.
View Article and Find Full Text PDFThe normalization of scattered intensity by incident flux is a crucial step in analyzing data from stochastic x-ray free electron laser sources and is complicated by non-linearities traditionally attributed to detector saturation. Here we show that such non-linearities can also arise when the sample spectra are non-uniform within the monochromator bandwidth. A method for modeling and removing this non-linearity using multivariate regression with shot-by-shot x-ray photon energy as an independent variable is presented.
View Article and Find Full Text PDFA method for measuring resonant inelastic X-ray scattering based on the conversion of X-ray photons into photoelectrons is presented. The setup is compact, relies on commercially available detectors, and offers significant flexibility. This method is demonstrated at the Linac Coherent Light Source with ∼0.
View Article and Find Full Text PDFX-ray absorption spectroscopy at the L-edge of 3d transition metals provides unique information on the local metal charge and spin states by directly probing 3d-derived molecular orbitals through 2p-3d transitions. However, this soft x-ray technique has been rarely used at synchrotron facilities for mechanistic studies of metalloenzymes due to the difficulties of x-ray-induced sample damage and strong background signals from light elements that can dominate the low metal signal. Here, we combine femtosecond soft x-ray pulses from a free-electron laser with a novel x-ray fluorescence-yield spectrometer to overcome these difficulties.
View Article and Find Full Text PDFJ Gerontol Soc Work
August 2018
This study measured the need for formal alternative modes of transportation among older adults by applying traditional factors of the Behavioral Model. Survey participants who regularly drove were compared to those who could no longer drive. Race/ethnicity and self-reported health were significant predictors of perceived need for transportation services for both groups.
View Article and Find Full Text PDFX-ray free electron lasers (XFELs) enable unprecedented new ways to study the electronic structure and dynamics of transition metal systems. L-edge absorption spectroscopy is a powerful technique for such studies and the feasibility of this method at XFELs for solutions and solids has been demonstrated. However, the required x-ray bandwidth is an order of magnitude narrower than that of self-amplified spontaneous emission (SASE), and additional monochromatization is needed.
View Article and Find Full Text PDFUnderstanding interfacial charge-transfer processes on the atomic level is crucial to support the rational design of energy-challenge relevant systems such as solar cells, batteries, and photocatalysts. A femtosecond time-resolved core-level photoelectron spectroscopy study is performed that probes the electronic structure of the interface between ruthenium-based N3 dye molecules and ZnO nanocrystals within the first picosecond after photoexcitation and from the unique perspective of the Ru reporter atom at the center of the dye. A transient chemical shift of the Ru 3d inner-shell photolines by (2.
View Article and Find Full Text PDFThis paper describes the development of new instrumentation at the Linac Coherent Light Source for conducting THz excitation experiments in an ultra high vacuum environment probed by soft X-ray diffraction. This consists of a cantilevered, fully motorized mirror system which can provide 600 kV cm(-1) electric field strengths across the sample and an X-ray detector that can span the full Ewald sphere with in-vacuum motion. The scientific applications motivated by this development, the details of the instrument, and spectra demonstrating the field strengths achieved using this newly developed system are discussed.
View Article and Find Full Text PDFA gas monitor detector was implemented and characterized at the Soft X-ray Research (SXR) instrument to measure the average, absolute and pulse-resolved photon flux of the LCLS beam in the energy range between 280 and 2000 eV. The detector is placed after the monochromator and addresses the need to provide reliable absolute pulse energy as well as pulse-resolved measurements for the various experiments at this instrument. This detector provides a reliable non-invasive measurement for determining flux levels on the samples in the downstream experimental chamber and for optimizing signal levels of secondary detectors and for the essential need of data normalization.
View Article and Find Full Text PDFThe Soft X-ray Research instrument provides intense ultrashort X-ray pulses in the energy range 280-2000 eV. A diverse set of experimental stations may be installed to investigate a broad range of scientific topics such as ultrafast chemistry, highly correlated materials, magnetism, surface science, and matter under extreme conditions. A brief description of the main instrument components will be given, followed by some selected scientific highlights.
View Article and Find Full Text PDFUsing data from a statewide needs assessment survey, this study examines and compares the self-reported future concerns of two age groups in Mississippi: Early wave Baby Boomers (age 55 to 64; n = 383) and the young-old (age 65 to 75; n = 349). Items under analysis focus on issues related to future concerns surrounding financial resources, health, and employment. Results from multivariate analyses of variance (MANOVA) indicate that Early wave Baby Boomers have higher levels of future concern than the young-old group in all three areas.
View Article and Find Full Text PDFL-edge spectroscopy of 3d transition metals provides important electronic structure information and has been used in many fields. However, the use of this method for studying dilute aqueous systems, such as metalloenzymes, has not been prevalent because of severe radiation damage and the lack of suitable detection systems. Here we present spectra from a dilute Mn aqueous solution using a high-transmission zone-plate spectrometer at the Linac Coherent Light Source (LCLS).
View Article and Find Full Text PDFWe present a flexible and compact experimental setup that combines an in vacuum liquid jet with an x-ray emission spectrometer to enable static and femtosecond time-resolved resonant inelastic soft x-ray scattering (RIXS) measurements from liquids at free electron laser (FEL) light sources. We demonstrate the feasibility of this type of experiments with the measurements performed at the Linac Coherent Light Source FEL facility. At the FEL we observed changes in the RIXS spectra at high peak fluences which currently sets a limit to maximum attainable count rate at FELs.
View Article and Find Full Text PDFWe present the first single-shot images of ferromagnetic, nanoscale spin order taken with femtosecond x-ray pulses. X-ray-induced electron and spin dynamics can be outrun with pulses shorter than 80 fs in the investigated fluence regime, and no permanent aftereffects in the samples are observed below a fluence of 25 mJ/cm(2). Employing resonant spatially muliplexed x-ray holography results in a low imaging threshold of 5 mJ/cm(2).
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