Capturing dynamical correlations using implicit neural representations.

Understanding 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. In this work, we employ linear spin wave theory simulations to train a machine learning platform, enabling precise exchange parameter extraction from inelastic neutron scattering data on the square-lattice spin-1 antiferromagnet La2NiO4, showcasing a viable pathway towards automatic refinement of advanced models for ordered magnetic systems.

Understanding unconventional magnetic order in a candidate axion insulator by resonant elastic x-ray scattering.

Magnetic topological insulators and semimetals are a class of crystalline solids whose properties are strongly influenced by the coupling between non-trivial electronic topology and magnetic spin configurations. Such materials can host exotic electromagnetic responses. Among these are topological insulators with certain types of antiferromagnetic order which are predicted to realize axion electrodynamics. Here we investigate the highly unusual helimagnetic phases recently reported in EuIn2As2, which has been identified as a candidate for an axion insulator. Using resonant elastic x-ray scattering we show that the two types of magnetic order observed in EuIn2As2 are spatially uniform phases with commensurate chiral magnetic structures, ruling out a possible phase-separation scenario, and we propose that entropy associated with low energy spin fluctuations plays a significant role in driving the phase transition between them. Our results establish that the magnetic order in EuIn2As2 satisfies the symmetry requirements for an axion insulator.

Narrowband, Angle-Tunable, Helicity-Dependent Terahertz Emission from Nanowires of the Topological Dirac Semimetal Cd3As2.

All-optical control of terahertz pulses is essential for the development of optoelectronic devices for next-generation quantum technologies. Despite substantial research in THz generation methods, polarization control remains difficult. Here, we demonstrate that by exploiting band structure topology, both helicity-dependent and helicity-independent THz emission can be generated from nanowires of the topological Dirac semimetal Cd3As2. We show that narrowband THz pulses can be generated at oblique incidence by driving the system with optical (1.55 eV) pulses with circular polarization. Varying the incident angle also provides control of the peak emission frequency, with peak frequencies spanning 0.21-1.40 THz as the angle is tuned from 15 to 45°. We therefore present Cd3As2 nanowires as a promising novel material platform for controllable terahertz emission.

Room-Temperature Type-II Multiferroic Phase Induced by Pressure in Cupric Oxide.

According to previous theoretical work, the binary oxide CuO can become a room-temperature multiferroic via tuning of the superexchange interactions by application of pressure. Thus far, however, there has been no experimental evidence for the predicted room-temperature multiferroicity. Here, we show by neutron diffraction that the multiferroic phase in CuO reaches 295 K with the application of 18.5 GPa pressure. We also develop a spin Hamiltonian based on density functional theory and employing superexchange theory for the magnetic interactions, which can reproduce the experimental results. The present Letter provides a stimulus to develop room-temperature multiferroic materials by alternative methods based on existing low temperature compounds, such as epitaxial strain, for tunable multifunctional devices and memory applications.

Multi-mode excitation drives disorder during the ultrafast melting of a C4-symmetry-broken phase.

Spontaneous C4-symmetry breaking phases are ubiquitous in layered quantum materials, and often compete with other phases such as superconductivity. Preferential suppression of the symmetry broken phases by light has been used to explain non-equilibrium light induced superconductivity, metallicity, and the creation of metastable states. Key to understanding how these phases emerge is understanding how C4 symmetry is restored. A leading approach is based on time-dependent Ginzburg-Landau theory, which explains the coherence response seen in many systems. However, we show that, for the case of the single layered manganite La0.5Sr1.5MnO4, the theory fails. Instead, we find an ultrafast inhomogeneous disordering transition in which the mean-field order parameter no longer reflects the atomic-scale state of the system. Our results suggest that disorder may be common to light-induced phase transitions, and methods beyond the mean-field are necessary for understanding and manipulating photoinduced phases.

Classical Spin Liquid or Extended Critical Range in h-YMnO_{3}?

Neutron spectroscopy on the classical triangular-lattice frustrated antiferromagnet h-YMnO_{3} reveals diffuse, gapless magnetic excitations present both far below and above the ordering temperature. The correlation length of the excitations increases as the temperature approaches zero, bearing a strong resemblance to critical scattering. We model the dynamics in the ordered and correlated disordered phase as critical spin correlations in a two-dimensional magnetic state. We propose that our findings may provide a general framework to understand features often attributed to classical spin liquids.

Real Space Imaging of Spin Stripe Domain Fluctuations in a Complex Oxide.

Understanding the formation and dynamics of charge and spin-ordered states in low-dimensional transition metal oxide materials is crucial to understanding unconventional high-temperature superconductivity. La_{2-x}Sr_{x}NiO_{4+δ} (LSNO) has attracted much attention due to its interesting spin dynamics. Recent x-ray photon correlation spectroscopy studies have revealed slow dynamics of the spin order (SO) stripes in LSNO. Here, we applied resonant soft x-ray ptychography to map the spatial distribution of the SO stripe domain inhomogeneity in real space. The reconstructed images show the SO domains are spatially anisotropic, in agreement with previous diffraction studies. For the SO stripe domains, it is found that the correlation lengths along different directions are strongly coupled in space. Surprisingly, fluctuations were observed in the real space amplitude signal, rather than the phase or position. We attribute the observed slow dynamics of the stripe domains in LSNO to thermal fluctuations of the SO domain boundaries.

Persistent coherence of quantum superpositions in an optimally doped cuprate revealed by 2D spectroscopy.

Quantum materials displaying intriguing magnetic and electronic properties could be key to the development of future technologies. However, it is poorly understood how the macroscopic behavior emerges in complex materials with strong electronic correlations. While measurements of the dynamics of excited electronic populations have been able to give some insight, they have largely neglected the intricate dynamics of quantum coherence. Here, we apply multidimensional coherent spectroscopy to a prototypical cuprate and report unprecedented coherent dynamics persisting for ~500 fs, originating directly from the quantum superposition of optically excited states separated by 20 to 60 meV. These results reveal that the states in this energy range are correlated with the optically excited states at ~1.5 eV and point to nontrivial interactions between quantum many-body states on the different energy scales. In revealing these dynamics and correlations, we demonstrate that multidimensional coherent spectroscopy can interrogate complex quantum materials in unprecedented ways.

Photocatalytic water splitting by N-TiO2 on MgO (111) with exceptional quantum efficiencies at elevated temperatures.

Photocatalytic water splitting is attracting enormous interest for the storage of solar energy but no practical method has yet been identified. In the past decades, various systems have been developed but most of them suffer from low activities, a narrow range of absorption and poor quantum efficiencies (Q.E.) due to fast recombination of charge carriers. Here we report a dramatic suppression of electron-hole pair recombination on the surface of N-doped TiO2 based nanocatalysts under enhanced concentrations of H+ and OH-, and local electric field polarization of a MgO (111) support during photolysis of water at elevated temperatures. Thus, a broad optical absorption is seen, producing O2 and H2 in a 1:2 molar ratio with a H2 evolution rate of over 11,000 µmol g-1 h-1 without any sacrificial reagents at 270 °C. An exceptional range of Q.E. from 81.8% at 437 nm to 3.2% at 1000 nm is also reported.

Electromagnon excitation in cupric oxide measured by Fabry-Pérot enhanced terahertz Mueller matrix ellipsometry.

Here we present the use of Fabry-Pérot enhanced terahertz (THz) Mueller matrix ellipsometry to measure an electromagnon excitation in monoclinic cupric oxide (CuO). As a magnetically induced ferroelectric multiferroic, CuO exhibits coupling between electric and magnetic order. This gives rise to special quasiparticle excitations at THz frequencies called electromagnons. In order to measure the electromagnons in CuO, we exploit single-crystal CuO as a THz Fabry-Pérot cavity to resonantly enhance the excitation's signature. This enhancement technique enables the complex index of refraction to be extracted. We observe a peak in the absorption coefficient near 0.705 THz and 215 K, which corresponds to the electromagnon excitation. This absorption peak is observed along only one major polarizability axis in the monoclinic a-c plane. We show the excitation can be represented using the Lorentz oscillator model, and discuss how these Lorentz parameters evolve with temperature. Our findings are in excellent agreement with previous characterizations by THz time-domain spectroscopy (THz-TDS), which demonstrates the validity of this enhancement technique.

Transverse and longitudinal spin-fluctuations in INVAR Fe0.65Ni0.35.

The presence of spin-fluctuations deep within the ordered state of ferromagnetic [Formula: see text] alloy [Formula: see text] has long been suspected but seldom directly observed. Inhomogeneities of one type or another have been cited as important in stabilizing [Formula: see text] behaviour-either longitudinal spin-fluctuations associated with the [Formula: see text]-state (local environment) model or transverse magnetisation arising from non-collinear spin structures. In this study we employ small-angle neutron scattering with neutron polarization analysis to distinguish between the two possibilities. Surprisingly we in fact find evidence of dominant but uncorrelated longitudinal spin-fluctuations coexisting with transverse magnetisation which exists in short-range clusters of size ~[Formula: see text]. This finding supports recent first principles calculations of [Formula: see text] in which both longitudinal spin-fluctuations and magnetic short-range order are identified as important ingredients in reproducing the equilibrium [Formula: see text] lattice.

Layer-by-layer epitaxial thin films of the pyrochlore Tb2Ti2O7.

Layer-by-layer epitaxial growth of the pyrochlore magnet Tb2Ti2O7 on the isostructural substrate Y2Ti2O7 results in high-quality single crystal films of up to 60 nm thickness. Substrate-induced strain is shown to act as a strong and controlled perturbation to the exotic magnetism of Tb2Ti2O7, opening up the general prospect of strain-engineering the diverse magnetic and electrical properties of pyrochlore oxides.

Terahertz field control of in-plane orbital order in La(0.5)Sr(1.5)MnO4.

In-plane anisotropic ground states are ubiquitous in correlated solids such as pnictides, cuprates and manganites. They can arise from doping Mott insulators and compete with phases such as superconductivity; however, their origins are debated. Strong coupling between lattice, charge, orbital and spin degrees of freedom results in simultaneous ordering of multiple parameters, masking the mechanism that drives the transition. Here we demonstrate that the orbital domains in a manganite can be oriented by the polarization of a pulsed THz light field. Through the application of a Hubbard model, we show that domain control can be achieved by enhancing the local Coulomb interactions, which drive domain reorientation. Our results highlight the key role played by the Coulomb interaction in the control and manipulation of orbital order in the manganites and demonstrate a new way to use THz to understand and manipulate anisotropic phases in a potentially broad range of correlated materials.

Witnessing the formation and relaxation of dressed quasi-particles in a strongly correlated electron system.

The non-equilibrium approach to correlated electron systems is often based on the paradigm that different degrees of freedom interact on different timescales. In this context, photo-excitation is treated as an impulsive injection of electronic energy that is transferred to other degrees of freedom only at later times. Here, by studying the ultrafast dynamics of quasi-particles in an archetypal strongly correlated charge-transfer insulator (La2CuO(4+δ)), we show that the interaction between electrons and bosons manifests itself directly in the photo-excitation processes of a correlated material. With the aid of a general theoretical framework (Hubbard-Holstein Hamiltonian), we reveal that sub-gap excitation pilots the formation of itinerant quasi-particles, which are suddenly dressed by an ultrafast reaction of the bosonic field.

Vapour-liquid-solid growth of ternary Bi2Se2Te nanowires.

: High-density growth of single-crystalline Bi2Se2Te nanowires was achieved via the vapour-liquid-solid process. The stoichiometry of samples grown at various substrate temperatures is precisely determined based on energy-dispersive X-ray spectroscopy, X-ray diffraction, and Raman spectroscopy on individual nanowires. We discuss the growth mechanism and present insights into the catalyst-precursor interaction.

Electric field control of the magnetic chiralities in ferroaxial multiferroic RbFe(MoO4)2.

The coupling of magnetic chiralities to the ferroelectric polarization in multiferroic RbFe(MoO4)2 is investigated by neutron spherical polarimetry. Because of the axiality of the crystal structure below T(c)=190 K, helicity and triangular chirality are symmetric-exchange coupled, explaining the onset of the ferroelectricity in this proper-screw magnetic structure--a mechanism that can be generalized to other systems with ferroaxial distortions in the crystal structure. With an applied electric field, we demonstrate control of the chiralities in both structural domains simultaneously.

Strain coupling mechanisms and elastic relaxation associated with spin state transitions in LaCoO3.

Advantage is taken of the wealth of experimental data relating to the evolution with temperature of spin states of Co(3+) in LaCoO3 in order to undertake a detailed investigation of the mechanisms by which changes in electronic structure can influence strain, and elastic and anelastic relaxations in perovskites. The macroscopic strain accompanying changes in the spin state in LaCoO3 is predominantly a volume strain arising simply from the change in effective ionic radius of the Co(3+) ions. This acts to renormalize the octahedral tilting transition temperature in a manner that is easily understood in terms of coupling between the tilt and spin order parameters. Results from resonant ultrasound spectroscopy at high frequencies (0.1-1.5 MHz) reveal stiffening of the shear modulus which scales qualitatively with a spin order parameter defined in terms of changing Co-O bond lengths. From this finding, in combination with results from dynamic mechanical analysis at low frequencies (0.1-50 Hz) and data from the literature, four distinctive anelastic relaxation mechanisms are identified. The relaxation times of these are displayed on an anelasticity map and are tentatively related to spin-spin relaxation, spin-lattice relaxation, migration of twin walls and migration of magnetic polarons. The effective activation energy for the freezing of twin wall motion below ~590 K at low frequencies was found to be 182 ± 21 kJ mol(-1) (1.9 ± 0.2 eV) which is attributed to pinning by pairs of oxygen vacancies, though the local mechanisms appear to have a spread of relaxation times. It seems inevitable that twin walls due to octahedral tilting must have quite different characteristics from the matrix in terms of local spin configurations of Co(3+). A hysteresis in the elastic properties at high temperatures further emphasizes the importance of oxygen content in controlling the properties of LaCoO3.