Discerning charge patterns in a cuprate: Copper oxides are well known to be able to achieve the order required for superconductivity. They can also achieve another order—one that produces patterns in their charge density. Experiments using nuclear magnetic resonanceand resonant x-ray scattering have both detected this so-called charge density wave (CDW) in yttrium-based cuprates. However, the nature of the CDW appeared to be different in the two types of measurement. Gerber et al. used pulsed magnetic fields of up to 28 T, combined with scattering, to bridge the gap (see the Perspective by Julien). As the magnetic field increased, a two-dimensional CDW gave way to a three-dimensional one. Science , this issue p. 949 ; see also p. 914

The X-ray Pump–Probe instrument achieves femtosecond time-resolution with hard X-ray methods using a free-electron laser source. It covers a photon energy range of 4–24 keV. A femtosecond optical laser system is available across a broad spectrum of wavelengths for generating transient states of matter. The instrument is designed to emphasize versatility and the scientific goals encompass ultrafast physical, chemical and biological processes involved in the transformation of matter and transfer of energy at the atomic scale.

We report hard x-ray single-shot spectral measurements of the Linac Coherent Light Source. The spectrometer is based on a $10\hspace{0.17em}\mu$ m thick cylindrically bent Si single crystal operating in the symmetric Bragg geometry to provide dispersion and high transmission simultaneously. It covers a spectral range >1% using the Si(111) reflection. Using the Si(333) reflection, it reaches a resolving power of better than 42 000 and transmits >83% of the incident flux at 8.3 keV. The high resolution enabled the observation of individual spectral spikes characteristic of a self-amplified spontaneous emission x-ray free electron laser source. Potential applications of the device are discussed.

The existence of charge-density-wave (CDW) correlations in cuprate superconductors has now been established. However, the nature of the CDW ground state has remained uncertain because disorder and the presence of superconductivity typically limit the CDW correlation lengths to only a dozen unit cells or less. Here we explore the field-induced 3D CDW correlations in extremely pure detwinned crystals of YBa₂Cu₃O₂ (YBCO) ortho-II and ortho-VIII at magnetic fields in excess of the resistive upper critical field ($H_{\mathrm{c}2}$) where superconductivity is heavily suppressed. We observe that the 3D CDW is unidirectional and possesses a long in-plane correlation length as well as significant correlations between neighboring CuO₂ planes. It is significant that we observe only a single sharply defined transition at a critical field proportional to $H_{\mathrm{c}2}$, given that the field range used in this investigation overlaps with other high-field experiments including quantum oscillation measurements. The correlation volume is at least two to three orders of magnitude larger than that of the zero-field CDW. This is by far the largest CDW correlation volume observed in any cuprate crystal and so is presumably representative of the high-field ground state of an “ideal” disorder-free cuprate. Significance Compelling evidence of various forms of nonsuperconducting electronic order in the cuprate high-temperature superconductors has fundamentally altered our understanding of the essential physics of these materials. However, it has been difficult to establish the nature of the quantum (zero-temperature) phases that compete and/or coexist with superconductivity. By studying high-quality crystals of YBCO using an X-ray laser and pulsed magnetic fields, we have established that the field induced charge-density-wave (CDW) order that arises when superconductivity is suppressed at low temperatures is incommensurate, unidirectional, and 3D-ordered. While disorder ultimately precludes true CDW long-range order, there does appear to be a sharply defined crossover field, which we associate with a transition to a nematic state with long-range orientational order.

Split-pulse x-ray photon correlation spectroscopy has been proposed as one of the unique capabilities made possible with x-ray free electron lasers. It enables characterization of atomic-scale structural dynamics that dictates the macroscopic properties of various disordered material systems. Central to the experimental concept are x-ray optics that are capable of splitting an individual coherent femtosecond x-ray pulse into two distinct pulses, introduce an adjustable time delay between them, and then recombine the two pulses at the sample position such that they generate two coherent scattering patterns in rapid succession. Recent developments in such optics showed that, while true “amplitude-splitting” optics at hard x-ray wavelengths remains a technical challenge, wavefront and wavelength splitting are both feasible, able to deliver two micron-sized focused beams to the sample with sufficient relative stability. Here we show, however, that the conventional approach to speckle visibility spectroscopy using these beam-splitting techniques can be problematic, even leading to a decoupling of speckle visibility and material dynamics. In response, we discuss the details of the experimental approaches and data analysis protocols for addressing issues caused by subtle beam dissimilarities for both wavefront- and wavelength-splitting setups. We also show that in some scattering geometries, the $Q$-space mismatch can be resolved by using two beams of slightly different incidence angles and slightly different wavelengths at the same time. Instead of measuring the visibility of weak speckle patterns, the time correlation in sample structure is encoded in the “side band” of the spatial autocorrelation of the summed speckle patterns and can be retrieved straightforwardly from the experimental data. We demonstrate this with a numerical simulation.