Reversible non-volatile electronic switching in a near-room-temperature van der Waals ferromagnet.

Non-volatile phase-change memory devices utilize local heating to toggle between crystalline and amorphous states with distinct electrical properties. Expanding on this kind of switching to two topologically distinct phases requires controlled non-volatile switching between two crystalline phases with distinct symmetries. Here, we report the observation of reversible and non-volatile switching between two stable and closely related crystal structures, with remarkably distinct electronic structures, in the near-room-temperature van der Waals ferromagnet Fe5-δGeTe2. We show that the switching is enabled by the ordering and disordering of Fe site vacancies that results in distinct crystalline symmetries of the two phases, which can be controlled by a thermal annealing and quenching method. The two phases are distinguished by the presence of topological nodal lines due to the preserved global inversion symmetry in the site-disordered phase, flat bands resulting from quantum destructive interference on a bipartite lattice, and broken inversion symmetry in the site-ordered phase.

A Novel Voltage Controlled Decoupling Method for Transmit Coils in MRI.

Array coils are ubiquitous in MRI and are becoming more widely used in MR spectroscopy. Conventional PIN diode decoupling circuits require significant currents to forward bias the diodes. The approach proposed here does not require significant current and thus reduces concerns for contaminating the B0 homogeneity with the detune current. Additionally, the proposed approach will facilitate the construction of array coils for MRI due to its simplicity.Clinical Relevance- Decoupling is critical for constructing RF coil arrays and enables rapid MR imaging.

Anomalous excitonic phase diagram in band-gap-tuned Ta2Ni(Se,S)5.

During a band-gap-tuned semimetal-to-semiconductor transition, Coulomb attraction between electrons and holes can cause spontaneously formed excitons near the zero-band-gap point, or the Lifshitz transition point. This has become an important route to realize bulk excitonic insulators - an insulating ground state distinct from single-particle band insulators. How this route manifests from weak to strong coupling is not clear. In this work, using angle-resolved photoemission spectroscopy (ARPES) and high-resolution synchrotron x-ray diffraction (XRD), we investigate the broken symmetry state across the semimetal-to-semiconductor transition in a leading bulk excitonic insulator candidate system Ta2Ni(Se,S)5. A broken symmetry phase is found to be continuously suppressed from the semimetal side to the semiconductor side, contradicting the anticipated maximal excitonic instability around the Lifshitz transition. Bolstered by first-principles and model calculations, we find strong interband electron-phonon coupling to play a crucial role in the enhanced symmetry breaking on the semimetal side of the phase diagram. Our results not only provide insight into the longstanding debate of the nature of intertwined orders in Ta2NiSe5, but also establish a basis for exploring band-gap-tuned structural and electronic instabilities in strongly coupled systems.

Real-space imaging of periodic nanotextures in thin films via phasing of diffraction data.

New properties and exotic quantum phenomena can form due to periodic nanotextures, including Moire patterns, ferroic domains, and topologically protected magnetization and polarization textures. Despite the availability of powerful tools to characterize the atomic crystal structure, the visualization of nanoscale strain-modulated structural motifs remains challenging. Here, we develop nondestructive real-space imaging of periodic lattice distortions in thin epitaxial films and report an emergent periodic nanotexture in a Mott insulator. Specifically, we combine iterative phase retrieval with unsupervised machine learning to invert the diffuse scattering pattern from conventional X-ray reciprocal-space maps into real-space images of crystalline displacements. Our imaging in PbTiO3/SrTiO3 superlattices exhibiting checkerboard strain modulation substantiates published phase-field model calculations. Furthermore, the imaging of biaxially strained Mott insulator Ca2RuO4 reveals a strain-induced nanotexture comprised of nanometer-thin metallic-structure wires separated by nanometer-thin Mott-insulating-structure walls, as confirmed by cryogenic scanning transmission electron microscopy (cryo-STEM). The nanotexture in Ca2RuO4 film is induced by the metal-to-insulator transition and has not been reported in bulk crystals. We expect the phasing of diffuse X-ray scattering from thin crystalline films in combination with cryo-STEM to open a powerful avenue for discovering, visualizing, and quantifying the periodic strain-modulated structures in quantum materials.

Harnessing interpretable and unsupervised machine learning to address big data from modern X-ray diffraction.

The information content of crystalline materials becomes astronomical when collective electronic behavior and their fluctuations are taken into account. In the past decade, improvements in source brightness and detector technology at modern X-ray facilities have allowed a dramatically increased fraction of this information to be captured. Now, the primary challenge is to understand and discover scientific principles from big datasets when a comprehensive analysis is beyond human reach. We report the development of an unsupervised machine learning approach, X-ray diffraction (XRD) temperature clustering (X-TEC), that can automatically extract charge density wave order parameters and detect intraunit cell ordering and its fluctuations from a series of high-volume X-ray diffraction measurements taken at multiple temperatures. We benchmark X-TEC with diffraction data on a quasi-skutterudite family of materials, (CaxSr[Formula: see text])3Rh4Sn13, where a quantum critical point is observed as a function of Ca concentration. We apply X-TEC to XRD data on the pyrochlore metal, Cd2Re2O7, to investigate its two much-debated structural phase transitions and uncover the Goldstone mode accompanying them. We demonstrate how unprecedented atomic-scale knowledge can be gained when human researchers connect the X-TEC results to physical principles. Specifically, we extract from the X-TEC-revealed selection rules that the Cd and Re displacements are approximately equal in amplitude but out of phase. This discovery reveals a previously unknown involvement of [Formula: see text] Re, supporting the idea of an electronic origin to the structural order. Our approach can radically transform XRD experiments by allowing in operando data analysis and enabling researchers to refine experiments by discovering interesting regions of phase space on the fly.

Unconventional Hysteretic Transition in a Charge Density Wave.

Hysteresis underlies a large number of phase transitions in solids, giving rise to exotic metastable states that are otherwise inaccessible. Here, we report an unconventional hysteretic transition in a quasi-2D material, EuTe_{4}. By combining transport, photoemission, diffraction, and x-ray absorption measurements, we observe that the hysteresis loop has a temperature width of more than 400 K, setting a record among crystalline solids. The transition has an origin distinct from known mechanisms, lying entirely within the incommensurate charge density wave (CDW) phase of EuTe_{4} with no change in the CDW modulation periodicity. We interpret the hysteresis as an unusual switching of the relative CDW phases in different layers, a phenomenon unique to quasi-2D compounds that is not present in either purely 2D or strongly coupled 3D systems. Our findings challenge the established theories on metastable states in density wave systems, pushing the boundary of understanding hysteretic transitions in a broken-symmetry state.

Unconventional chiral charge order in kagome superconductor KV3Sb5.

Intertwining quantum order and non-trivial topology is at the frontier of condensed matter physics1-4. A charge-density-wave-like order with orbital currents has been proposed for achieving the quantum anomalous Hall effect5,6 in topological materials and for the hidden phase in cuprate high-temperature superconductors7,8. However, the experimental realization of such an order is challenging. Here we use high-resolution scanning tunnelling microscopy to discover an unconventional chiral charge order in a kagome material, KV3Sb5, with both a topological band structure and a superconducting ground state. Through both topography and spectroscopic imaging, we observe a robust 2 × 2 superlattice. Spectroscopically, an energy gap opens at the Fermi level, across which the 2 × 2 charge modulation exhibits an intensity reversal in real space, signalling charge ordering. At the impurity-pinning-free region, the strength of intrinsic charge modulations further exhibits chiral anisotropy with unusual magnetic field response. Theoretical analysis of our experiments suggests a tantalizing unconventional chiral charge density wave in the frustrated kagome lattice, which can not only lead to a large anomalous Hall effect with orbital magnetism, but also be a precursor of unconventional superconductivity.

Side-bounce beamlines using single-reflection diamond monochromators at Cornell High Energy Synchrotron Source.

The design and implementation of new beamlines featuring side-bounce (single-reflection) diamond monochromators at Cornell High Energy Synchrotron Source (CHESS) are described. Undulator radiation is monochromated using an interchangeable set of diamond crystal plates reflecting radiation in the horizontal (synchrotron) plane, where each crystal plate is set to one of the low-index Bragg reflections (111, 220, 311 and 400) in either Bragg or Laue reflection geometries. At the nominal Bragg angle of 18° these reflections deliver monochromated X-rays with photon energies of 9.7, 15.9, 18.65 and 22.5 keV, respectively. An X-ray mirror downstream of the diamond monochromator is used for rejection of higher radiation harmonics and for initial focusing of the monochromated beam. The characteristics of the X-ray beam entering the experimental station were measured experimentally and compared with the results of simulations. A reasonable agreement is demonstrated. It is shown that the use of selected high-dislocation-density `mosaic' diamond single-crystal plates produced using the chemical vapor deposition method yields a few-fold enhancement in the flux density of the monochromated beam in comparison with that delivered by perfect crystals under the same conditions. At present, the Functional Materials Beamline at CHESS, which is used for time-resolved in situ characterization of soft materials during processing, has been outfitted with the described setup.

Spontaneous gyrotropic electronic order in a transition-metal dichalcogenide.

Chirality is ubiquitous in nature, and populations of opposite chiralities are surprisingly asymmetric at fundamental levels1,2. Examples range from parity violation in the subatomic weak force to homochirality in biomolecules. The ability to achieve chirality-selective synthesis (chiral induction) is of great importance in stereochemistry, molecular biology and pharmacology2. In condensed matter physics, a crystalline electronic system is geometrically chiral when it lacks mirror planes, space-inversion centres or rotoinversion axes1. Typically, geometrical chirality is predefined by the chiral lattice structure of a material, which is fixed on formation of the crystal. By contrast, in materials with gyrotropic order3-6, electrons spontaneously organize themselves to exhibit macroscopic chirality in an originally achiral lattice. Although such order-which has been proposed as the quantum analogue of cholesteric liquid crystals-has attracted considerable interest3-15, no clear observation or manipulation of gyrotropic order has been achieved so far. Here we report the realization of optical chiral induction and the observation of a gyrotropically ordered phase in the transition-metal dichalcogenide semimetal 1T-TiSe2. We show that shining mid-infrared circularly polarized light on 1T-TiSe2 while cooling it below the critical temperature leads to the preferential formation of one chiral domain. The chirality of this state is confirmed by the measurement of an out-of-plane circular photogalvanic current, the direction of which depends on the optical induction. Although the role of domain walls requires further investigation with local probes, the methodology demonstrated here can be applied to realize and control chiral electronic phases in other quantum materials4,16.

Reciprocal space imaging of ionic correlations in intercalation compounds.

The intercalation of alkali ions into layered materials has played an essential role in battery technology since the development of the first lithium-ion electrodes. Coulomb repulsion between the intercalants leads to ordering of the intercalant sublattice, which hinders ionic diffusion and impacts battery performance. While conventional diffraction can identify the long-range order that can occur at discrete intercalant concentrations during the charging cycle, it cannot determine short-range order at other concentrations that also disrupt ionic mobility. In this Article, we show that the use of real-space transforms of single-crystal diffuse scattering, measured with high-energy synchrotron X-rays, allows a model-independent measurement of the temperature dependence of the length scale of ionic correlations along each of the crystallographic axes in sodium-intercalated V2O5. The techniques described here provide a new way of probing the evolution of structural ordering in crystalline materials.

Setting Carriers Free: Healing Faulty Interfaces Promotes Delocalization and Transport in Nanocrystal Solids.

Superlattices of epitaxially connected nanocrystals (NCs) are model systems to study electronic and optical properties of NC arrays. Using elemental analysis and structural analysis by in situ X-ray fluorescence and grazing-incidence small-angle scattering, respectively, we show that epitaxial superlattices of PbSe NCs keep their structural integrity up to temperatures of 300 °C; an ideal starting point to assess the effect of gentle thermal annealing on the superlattice properties. We find that annealing such superlattices between 75 and 150 °C induces a marked red shift of the NC band-edge transition. In fact, the post-annealing band-edge reflects theoretical predictions on the impact of charge carrier delocalization in these epitaxial superlattices. In addition, we observe a pronounced enhancement of the charge carrier mobility and a reduction of the hopping activation energy after mild annealing. While the superstructure remains intact at these temperatures, structural defect studies through X-ray diffraction indicate that annealing markedly decreases the density of point defects and edge dislocations. This indicates that the connections between NCs in as-synthesized superlattices still form a major source of grain boundaries and defects, which prevent carrier delocalization over multiple NCs and hamper NC-to-NC transport. Overcoming the limitations imposed by interfacial defects is therefore an essential next step in the development of high-quality optoelectronic devices based on NC solids.

Author Correction: Reciprocal space imaging of ionic correlations in intercalation compounds.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Disorder raises the critical temperature of a cuprate superconductor.

With the discovery of charge-density waves (CDWs) in most members of the cuprate high-temperature superconductors, the interplay between superconductivity and CDWs has become a key point in the debate on the origin of high-temperature superconductivity. Some experiments in cuprates point toward a CDW state competing with superconductivity, but others raise the possibility of a CDW-superconductivity intertwined order or more elusive pair-density waves (PDWs). Here, we have used proton irradiation to induce disorder in crystals of [Formula: see text] and observed a striking 50% increase of [Formula: see text], accompanied by a suppression of the CDWs. This is in sharp contrast with the behavior expected of a d-wave superconductor, for which both magnetic and nonmagnetic defects should suppress [Formula: see text] Our results thus make an unambiguous case for the strong detrimental effect of the CDW on bulk superconductivity in [Formula: see text] Using tunnel diode oscillator (TDO) measurements, we find indications for potential dynamic layer decoupling in a PDW phase. Our results establish irradiation-induced disorder as a particularly relevant tuning parameter for the many families of superconductors with coexisting density waves, which we demonstrate on superconductors such as the dichalcogenides and [Formula: see text].

Preferential quenching of 5d antiferromagnetic order in Sr3(Ir1-x Mn x )2O7.

The breakdown of [Formula: see text] antiferromagnetism in the limit of strong disorder is studied in Sr3(Ir1-x Mn x )2O7. Upon Mn-substitution, antiferromagnetic ordering of the Ir cations becomes increasingly two-dimensional, resulting in the complete suppression of long-range Ir magnetic order above [Formula: see text]. Long-range antiferromagnetism however persists on the Mn sites to higher Mn concentrations (x > 0.25) and is necessarily mediated via a random network of majority Ir sites. Our data suggest a shift in the Mn valence from Mn4+ to Mn3+ at intermediate doping levels, which in turn generates nonmagnetic Ir5+ sites and suppresses long-range order within the Ir network. The collapse of long-range [Formula: see text] antiferromagnetism and the survival of percolating antiferromagnetic order on Mn-sites demonstrates a complex 3d-5d exchange process that surprisingly enables minority Mn spins to order far below the conventional percolation threshold for a bilayer square lattice.

Divergence of the quadrupole-strain susceptibility of the electronic nematic system YbRu2Ge2.

Ferroquadrupole order associated with local [Formula: see text] atomic orbitals of rare-earth ions is a realization of electronic nematic order. However, there are relatively few examples of intermetallic materials which exhibit continuous ferroquadrupole phase transitions, motivating the search for additional materials that fall into this category. Furthermore, it is not clear a priori whether experimental approaches based on transport measurements which have been successfully used to probe the nematic susceptibility in materials such as the Fe-based superconductors will be as effective in the case of [Formula: see text] intermetallic materials, for which the important electronic degrees of freedom are local rather than itinerant and are consequently less strongly coupled to the charge-carrying quasiparticles near the Fermi energy. In the present work, we demonstrate that the intermetallic compound [Formula: see text] exhibits a tetragonal-to-orthorhombic phase transition consistent with ferroquadrupole order of the Yb ions and go on to show that elastoresistivity measurements can indeed provide a clear window on the diverging nematic susceptibility in this system. This material provides an arena in which to study the causes and consequences of electronic nematicity.

Dual Nature of Magnetism in a Uranium Heavy-Fermion System.

The duality between the localized and itinerant nature of magnetism in 5f-electron systems has been a long-standing puzzle. Here, we report inelastic neutron scattering measurements, which reveal both local and itinerant aspects of magnetism in a single-crystalline system of UPt_{2}Si_{2}. In the antiferromagnetic state, we observe a broad continuum of diffuse magnetic scattering with a resonancelike gap of ≈7 meV and the surprising absence of coherent spin waves, suggestive of itinerant magnetism. While the gap closes above the Néel temperature, strong dynamic spin correlations persist to a high temperature. Nevertheless, the size and temperature dependence of the total magnetic spectral weight can be well described by a local moment with J=4. Furthermore, polarized neutron measurements reveal that the magnetic fluctuations are mostly transverse, with little or none of the longitudinal component expected for itinerant moments. These results suggest that a dual description of local and itinerant magnetism is required to understand UPt_{2}Si_{2} and, by extension, other 5f systems, in general.

Unidirectional spin density wave state in metallic (Sr1-xLa x )2IrO4.

Materials that exhibit both strong spin-orbit coupling and electron correlation effects are predicted to host numerous new electronic states. One prominent example is the Jeff = 1/2 Mott state in Sr2IrO4, where introducing carriers is predicted to manifest high temperature superconductivity analogous to the S = 1/2 Mott state of La2CuO4. While bulk superconductivity currently remains elusive, anomalous quasiparticle behaviors paralleling those in the cuprates such as pseudogap formation and the formation of a d-wave gap are observed upon electron-doping Sr2IrO4. Here we establish a magnetic parallel between electron-doped Sr2IrO4 and hole-doped La2CuO4 by unveiling a spin density wave state in electron-doped Sr2IrO4. Our magnetic resonant X-ray scattering data reveal the presence of an incommensurate magnetic state reminiscent of the diagonal spin density wave state observed in the monolayer cuprate (La1-xSr x )2CuO4. This link supports the conjecture that the quenched Mott phases in electron-doped Sr2IrO4 and hole-doped La2CuO4 support common competing electronic phases.

Origin of long lifetime of band-edge charge carriers in organic-inorganic lead iodide perovskites.

Long carrier lifetime is what makes hybrid organic-inorganic perovskites high-performance photovoltaic materials. Several microscopic mechanisms behind the unusually long carrier lifetime have been proposed, such as formation of large polarons, Rashba effect, ferroelectric domains, and photon recycling. Here, we show that the screening of band-edge charge carriers by rotation of organic cation molecules can be a major contribution to the prolonged carrier lifetime. Our results reveal that the band-edge carrier lifetime increases when the system enters from a phase with lower rotational entropy to another phase with higher entropy. These results imply that the recombination of the photoexcited electrons and holes is suppressed by the screening, leading to the formation of polarons and thereby extending the lifetime. Thus, searching for organic-inorganic perovskites with high rotational entropy over a wide range of temperature may be a key to achieve superior solar cell performance.

Charge Density Wave in the New Polymorphs of RE2Ru3Ge5 (RE = Pr, Sm, Dy).

A new polymorph of the RE2Ru3Ge5 (RE = Pr, Sm, Dy) compounds has been grown as single crystals via an indium flux. These compounds crystallize in tetragonal space group P4/mnc with the Sc2Fe3Si5-type structure, having lattice parameters a = 11.020(2) Šand c = 5.853(1) Šfor RE = Pr, a = 10.982(2) Šand c = 5.777(1) Šfor RE = Sm, and a = 10.927(2) Šand c = 5.697(1) Šfor RE = Dy. These materials exhibit a structural transition at low temperature, which is attributed to an apparent charge density wave (CDW). Both the high-temperature average crystal structure and the low-temperature incommensurately modulated crystal structure (for Sm2Ru3Ge5 as a representative) have been solved. The charge density wave order is manifested by periodic distortions of the one-dimensional zigzag Ge chains. From X-ray diffraction, charge transport (electrical resistivity, Hall effect, magnetoresistance), magnetic measurements, and heat capacity, the ordering temperatures (TCDW) observed in the Pr and Sm analogues are ∼200 and ∼175 K, respectively. The charge transport measurement results indicate an electronic state transition happening simultaneously with the CDW transition. X-ray absorption near-edge spectroscopy (XANES) and electronic band structure results are also reported.

Entropy-driven structural transition and kinetic trapping in formamidinium lead iodide perovskite.

A challenge of hybrid perovskite solar cells is device instability, which calls for an understanding of the perovskite structural stability and phase transitions. Using neutron diffraction and first-principles calculations on formamidinium lead iodide (FAPbI3), we show that the entropy contribution to the Gibbs free energy caused by isotropic rotations of the FA+ cation plays a crucial role in the cubic-to-hexagonal structural phase transition. Furthermore, we observe that the cubic-to-hexagonal phase transition exhibits a large thermal hysteresis. Our first-principles calculations confirm the existence of a potential barrier between the cubic and hexagonal structures, which provides an explanation for the observed thermal hysteresis. By exploiting the potential barrier, we demonstrate kinetic trapping of the cubic phase, desirable for solar cells, even at 8.2 K by thermal quenching.