High-energy Spin Research Articles

Monolayer MoS2 and WS2 for Vertical Circular‐ Polarized‐Light‐Emitting Diode: from Fundamental Understanding to Device Architecture

AbstractLight‐emitting diodes (LEDs) have revolutionized lighting and displays due to their numerous advantages over conventional lighting mechanisms. Moreover, the directional nature of luminescent materials has spurred significant advancements in the development of circularly polarized LEDs, which hold transformative potential for applications in biomedical imaging, liquid crystal displays, spintronics, and valleytronics. The performance of circularly polarized LEDs mainly depends on the emitter material, which is this study's focus. In particular, semiconducting‐phase 2D monolayer MoS2 and WS2 are attractive emitter‐material candidates owing to their bandgap versatility, high carrier mobility, high exciton binding energy, polarized‐light‐emission properties, and unique spin–valley coupling. Several works have examined the fundamental light‐emission properties of monolayer MoS2 and WS2 from the perspectives of optoelectronic concepts, material fabrication, and device construction. This paper presents approaches to control, tune, and enhance these properties of monolayer MoS2 and WS2. Possible guidelines for monolayer‐material synthesis (top‐down and bottom‐up approaches) and device engineering of vertically stacked MoS2 and WS2 are presented. Finally, the review considers the material topological characteristics, outlines the challenges and potential of monolayer MoS2 and WS2 for developing high‐performance commercial circularly polarized LED devices, and proposes a technological roadmap for leveraging other monolayer transition metal dichalcogenide systems in optoelectronic devices.

Simultaneously Regulated Highly Polarized and Long-Lived Valley Excitons in WSe2/GaN Heterostructures.

Interlayer excitons, with prolonged lifetimes and tunability, hold potential for advanced optoelectronics. Previous research on the interlayer excitons has been dominated by two-dimensional heterostructures. Here, we construct WSe2/GaN composite heterostructures, in which the doping concentration of GaN and the twist angle of bilayer WSe2 are employed as two ingredients for the manipulation of exciton behaviors and polarizations. The exciton energies in monolayer WSe2/GaN can be regulated continuously by the doping levels of the GaN substrate, and a remarkable increase in the valley polarizations is achieved. Especially in a heterostructure with 4°-twisted bilayer WSe2, a maximum polarization of 38.9% with a long lifetime is achieved for the interlayer exciton. Theoretical calculations reveal that the large polarization and long lifetime are attributed to the high exciton binding energy and large spin flipping energy during depolarization in bilayer WSe2/GaN. This work introduces a distinctive member of the interlayer exciton with a high degree of polarization and a long lifetime.

Evolution of the Magnetic Excitations in Electron-Doped La_{2-x}Ce_{x}CuO_{4}.

We investigated the high energy spin excitations in electron-doped La_{2-x}Ce_{x}CuO_{4}, a cuprate superconductor, by resonant inelastic x-ray scattering (RIXS) measurements. Efforts were paid to disentangle the paramagnon signal from non-spin-flip spectral weight mixing in the RIXS spectrum at Q_{∥}=(0.6π,0) and (0.9π,0) along the (1 0) direction. Our results show that, for doping level x from 0.07 to 0.185, the variation of the paramagnon excitation energy is marginal. We discuss the implication of our results in connection with the evolution of the electron correlation strength in this system.

Tunable long-range spin transport in a van der Waals Fe3GeTe2/WSe2/Fe3GeTe2 spin valve.

The seamless integration of two-dimensional (2D) ferromagnetic materials with similar or dissimilar materials can widen the scope of low-power spintronics. In this regard, a vertical van der Waals (vdW) heterostructure of 2D ferromagnets with semiconducting transition metal dichalcogenides (TMDCs) forms magnetic junctions with exceptional stability and electrical control. Interestingly, 2D metallic Fe3GeTe2 (FGT) reveals above room temperature Curie temperatures and has large magneto anisotropy due to spin-orbit coupling. In addition, it also possesses topological states and a large Berry curvature. Herein, we designed the FGT/WSe2/FGT vdW heterostructure with a uniform and sharp interface so that FGT could maintain its inherent electronic properties. Also, the uniform thickness of the barrier provides a smooth flow of spins through the junctions as tunneling exponentially decays with an increasing barrier thickness. However, strong energy-dependent spin polarization is crucial for achieving optimum spin valve properties, such as large tunneling magnetoresistance (TMR) along with the manipulation of the magnitude and sign reversal. We have observed a shifting of high-energy localized minority spin states toward low-energy regions, which causes spin polarization fluctuation between -42.5% and 41% over a wide range of bias voltage. This leads to a negative TMR% of ∼-100% at 0.1 V Å-1 and also a large positive TMR% at 0.2 V Å-1 and -0.4 V Å-1. Besides, the system exhibits a highly tunable large anomalous Hall conductivity (AHC) of 626 S cm-1. Interestingly, such unprecedented electronic behaviour with large and switchable spin polarization, anomalous Hall conductivity and TMR can be incorporated into MTJ devices, which provide electrical control and long-range spin transport. Additionally, the system emerges as a standout candidate in low-power spintronic devices (e.g., MRAM and magnetic sensors) owing to its distinctive energy-dependent electronic structure with a wide range of external bias.

An overview of the spin dynamics of antiferromagnetic Mn5Si3

The metallic compound Mn5Si3 hosts a series of antiferromagnetic phases that can be controlled by external stimuli, such as temperature and magnetic field. In this work, we investigate the spin-excitation spectrum of bulk Mn5Si3 by combining inelastic neutron scattering measurements and density functional theory calculations. We study the evolution of the dynamical response under external parameters and demonstrate that the spin dynamics of each phase is robust against any combination of temperature and magnetic field. In particular, the high-energy spin dynamics is very characteristic of the different phases consisting of either spin waves or broad fluctuation patterns.

Probing Gluons with the Future Spin Physics Detector

In this paper, we review the physics studies to be performed with the Spin Physics Detector (SPD) at the Nuclotron-based Ion Collider fAcility (NICA) which is a multi-purpose experiment designed to study nucleon spin structure in the three dimensions. With capabilities to collide polarized protons and deuterons with center-of-mass energy up to 27 GeV and luminosity up to 1032cm−2s−1 for protons (an order of magnitude less for deuterons), the experiment is considered to allow measurements of cross-sections and spin asymmetries of hadronic processes sensitive to the unpolarized and various polarized (helicity, Sivers, Boer-Mulders) gluon distributions inside the nucleons. Results from the SPD will be complimentary to the present high-energy spin experiments at the RHIC (Relativistic Heavy Ion Collider) facility or future experiments such as the Electron-Ion Collider (EIC) at BNL (Brookhaven National Laboratory) and the AFTER experiment at the LHC (Large Hadron Collider) in understanding the spin structure of the basic building blocks of visible matter. Monte Carlo simulation-based results presented here demonstrate the impact of the SPD asymmetry measurements on gluon helicity parton distribution function (PDF) and gluon Sivers functions. With polarized deuteron collisions, the SPD is expected to be the unique laboratory for probing tensor-polarized gluon distributions. Additionally, there are possibilities of colliding other light nuclei, such as carbon, at reduced collision energy and luminosity during the first stage of the experiment.

High-energy spin excitations in the quantum spin liquid candidate Zn-substituted barlowite probed by resonant inelastic x-ray scattering

A quantum spin liquid is a novel ground state that can support long-range entanglement between magnetic moments, resulting in exotic spin excitations involving fractionalized $S=\frac{1}{2}$ spinons. Here, we measure the excitations in single crystals of the spin liquid candidate Zn-barlowite using resonant inelastic x-ray scattering. By analyzing the incident polarization and temperature dependences, we deduce a clear magnetic scattering contribution forming a broad continuum that surprisingly extends up to $\ensuremath{\sim}200$ meV ($\ensuremath{\sim}14J$, where $J$ is the magnetic exchange). The excitation spectrum indicates that significant contributions may arise from multiple pairs of spinons and/or antispinons at high energies. Furthermore, the observation of similar scattering in the hexagonal barlowite parent material above its ordering temperature suggests the presence of similar high-energy excitations, irrespective of the low-energy physics.

Coupling of terahertz light with nanometre-wavelength magnon modes via spin–orbit torque

Spin-based technologies can operate at terahertz frequencies but require manipulation techniques that work at ultrafast timescales to become practical. For instance, devices based on spin waves, also known as magnons, require efficient generation of high-energy exchange spin waves at nanometre wavelengths. To achieve this, a substantial coupling is needed between the magnon modes and an electro-magnetic stimulus such as a coherent terahertz field pulse. However, it has been difficult to excite non-uniform spin waves efficiently using terahertz light because of the large momentum mismatch between the submillimetre-wave radiation and the nanometre-sized spin waves. Here we improve the light–matter interaction by engineering thin films to exploit relativistic spin–orbit torques that are confined to the interfaces of heavy metal/ferromagnet heterostructures. We are able to excite spin-wave modes with frequencies of up to 0.6 THz and wavelengths as short as 6 nm using broadband terahertz radiation. Numerical simulations demonstrate that the coupling of terahertz light to exchange-dominated magnons originates solely from interfacial spin–orbit torques. Our results are of general applicability to other magnetic multilayered structures, and offer the prospect of nanoscale control of high-frequency signals.

An Atom-Pair Design Strategy for Optimizing the Synergistic Electron Effects of Catalytic Sites in NO Selective Reduction.

Effective adsorption and speedy surface reactions are vital requirements for efficient active sites in catalysis, but it remains challenging to maximize these two functions simultaneously. We present a solution to this issue by designing a series of atom-pair catalytic sites with tunable electronic interactions. As a case study, NO selective reduction occurring on V1 -W1 /TiO2 is chosen. Experimental and theoretical results reveal that the synergistic electron effect present between the paired atoms enriches high-energy spin charge around the Fermi level, simultaneously rendering reactant (NH3 or O2 ) adsorption more effective and subsequent surface reactions speedier as compared with single V or W atom alone, and hence higher reaction rates. This strategy enables us to rationally design a high-performance V1 -Mo1 /TiO2 catalyst with optimized vanadium(IV)-molybdenum(V) electronic interactions, which has exceptional activity significantly higher than the commercial or reported catalysts.

Crossover of high-energy spin fluctuations from collective triplons to localized magnetic excitations in Sr14−xCaxCu24O41 ladders

We studied the magnetic excitations in the quasi-one-dimensional (q-1D) ladder subsystem of Sr14−xCaxCu24O41 (SCCO) using Cu L3-edge resonant inelastic X-ray scattering (RIXS). By comparing momentum-resolved RIXS spectra with high (x = 12.2) and without (x = 0) Ca content, we track the evolution of the magnetic excitations from collective two-triplon (2 T) excitations (x = 0) to weakly-dispersive gapped modes at an energy of 280 meV (x = 12.2). Density matrix renormalization group (DMRG) calculations of the RIXS response in the doped ladders suggest that the flat magnetic dispersion and damped excitation profile observed at x = 12.2 originates from enhanced hole localization. This interpretation is supported by polarization-dependent RIXS measurements, where we disentangle the spin-conserving ΔS = 0 scattering from the predominant ΔS = 1 spin-flip signal in the RIXS spectra. The results show that the low-energy weight in the ΔS = 0 channel is depleted when Sr is replaced by Ca, consistent with a reduced carrier mobility. Our results demonstrate that off-ladder impurities can affect both the low-energy magnetic excitations and superconducting correlations in the CuO4 plaquettes. Finally, our study characterizes the magnetic and charge fluctuations in the phase from which superconductivity emerges in SCCO at elevated pressures.

Disentangling the role of bond lengths and orbital symmetries in controlling Tc of optimally doped YBa2Cu3O7

Optimally doped YBCO (YBa$_{2}$Cu$_{3}$O$_{7}$) has a high critical temperature, at 92 K. It is largely believed that Cooper pairs form in YBCO and other cuprates because of spin fluctuations, the issue and the detailed mechanism is far from settled. In the present work, we employ a state-of-the-art \emph{ab initio} ability to compute both the low and high energy spin fluctuations in optimally doped YBCO. We benchmark our results against recent inelastic neutron scattering and resonant inelastic X-ray scattering measurements. Further, we use strain as an external parameter to modulate the spin fluctuations and superconductivity. We disentangle the roles of Barium-apical Oxygen hybridization, the interlayer coupling and orbital symmetries by applying an idealized strain, and also a strain with a fully relaxed structure. We show that shortening the distance between Cu layers is conducive for enhanced Fermi surface nesting, that increases spin fluctuations and drives up $T_{c}$. However, when the structure is fully relaxed electrons flow to the d$_{z^2}$ orbital as a consequence of a shortened Ba-O bond which is detrimental for superconductivity

Tunable spin injection and detection across a van der Waals interface.

Van der Waals heterostructures with two-dimensional magnets offer a magnetic junction with an atomically sharp and clean interface. This attribute ensures that the magnetic layers maintain their intrinsic spin-polarized electronic states and spin-flipping scattering processes at a minimum level, a trait that can expand spintronic device functionalities. Here, using a van der Waals assembly of ferromagnetic Fe3GeTe2 with non-magnetic hexagonal boron nitride and WSe2 layers, we demonstrate electrically tunable, highly transparent spin injection and detection across the van der Waals interfaces. By varying an electrical bias, the net spin polarization of the injected carriers can be modulated and reversed in polarity, which leads to sign changes of the tunnelling magnetoresistance. We attribute the spin polarization reversals to sizable contributions from high-energy localized spin states in the metallic ferromagnet, so far inaccessible in conventional magnetic junctions. Such tunability of the spin-valve operations opens a promising route for the electronic control of next-generation low-dimensional spintronic device applications.

Spin-excitation anisotropy in the nematic state of detwinned FeSe

The origin of the electronic nematicity in FeSe is one of the most important unresolved puzzles in the study of iron-based superconductors. In both spin- and orbital-nematic models, the intrinsic magnetic excitations at Q1 = (1, 0) and Q2 = (0, 1) of twin-free FeSe are expected to provide decisive criteria for clarifying this issue. Although a spin-fluctuation anisotropy below 10 meV between Q1 and Q2 has been observed by inelastic neutron scattering at low temperature, it remains unclear whether such an anisotropy also persists at higher energies and associates with the nematic transition Ts. Here we use resonant inelastic X-ray scattering to probe the high-energy magnetic excitations of detwinned FeSe. A prominent anisotropy between the magnetic excitations along the H and K directions is found to persist to E ≈ 200 meV, which decreases gradually with increasing temperature and finally vanishes at a temperature around Ts. The measured high-energy spin excitations are dispersive and underdamped, which can be understood from a local-moment perspective.Taking together the large energy scale far beyond the dxz/dyz orbital splitting, we suggest that the nematicity in FeSe is probably spin-driven.

Twist-3 gluon fragmentation contribution to polarized hyperon production in unpolarized proton-proton collision

Understanding the origin and mechanism of the transverse polarization of hyperons produced in unpolarized proton-proton collision, $pp\to \Lambda^\uparrow X$, has been one of the long-standing issues in high-energy spin physics. In the framework of the collinear factorization applicable to large-$p_T$ hadron productions, this phenomenon is a twist-3 observable which is caused by multi-parton correlations either in the initial protons or in the process of fragmentation into the hyperon. We derive the twist-3 gluon fragmentation function (FF) contribution to this process in the leading order (LO) with respect to the QCD coupling constant. Combined with the known results for the contribution from the twist-3 distribution function and the twist-3 quark FF, this completes the LO twist-3 cross section. We also found that the model independent relations among the twist-3 gluon FFs based on the QCD equation of motion and the Lorentz invariance property of the correlation functions guarantee the color gauge invariance and the frame-independence of the cross section.

Unusual spin pseudogap behavior in the spin web lattice Cu3TeO6 probed by Te125 nuclear magnetic resonance

We present a $^{125}\mathrm{Te}$ nuclear magnetic resonance (NMR) study in the three-dimensional spin web lattice ${\mathrm{Cu}}_{3}\mathrm{Te}{\mathrm{O}}_{6}$ which harbors topological magnons. The $^{125}\mathrm{Te}$ NMR spectra and the Knight-shift $\mathcal{K}$ as a function of temperature show a drastic change at ${T}_{\mathrm{S}}\ensuremath{\sim}40\phantom{\rule{0.28em}{0ex}}\mathrm{K}$ much lower than the N\'eel ordering temperature ${T}_{\mathrm{N}}\ensuremath{\sim}61\phantom{\rule{0.28em}{0ex}}\mathrm{K}$, providing evidence for the first-order structural phase transition within the magnetically ordered state. Most remarkably, the temperature dependence of the spin-lattice relaxation rate ${T}_{1}^{\ensuremath{-}1}$ unravels spin-gap-like magnetic excitations, which sharply sets in at ${T}^{*}\ensuremath{\sim}75\phantom{\rule{0.28em}{0ex}}\mathrm{K}$, the temperature well above ${T}_{\mathrm{N}}$. The spin-gap behavior may be understood by weakly dispersive optical magnon branches of high-energy spin excitations originating from the unique corner-sharing Cu hexagon spin-1/2 network with low coordination number.

Coupled spin–orbital fluctuations in a three orbital model for 4d and 5d oxides with electron fillings n = 3, 4, 5—application to NaOsO3, Ca2RuO4 and Sr2IrO4

A unified approach is presented for investigating coupled spin–orbital fluctuations within a realistic three-orbital model for strongly spin–orbit coupled systems with electron fillings n = 3, 4, 5 in the t 2g sector of d yz , d xz , d xy orbitals. A generalized fluctuation propagator is constructed which is consistent with the generalized self-consistent Hartree–Fock approximation where all Coulomb interaction contributions involving orbital diagonal and off-diagonal spin and charge condensates are included. Besides the low-energy magnon, intermediate-energy orbiton and spin–orbiton, and high-energy spin–orbit exciton modes, the generalized spectral function also shows other high-energy excitations such as the Hund’s coupling induced gapped magnon modes. We relate the characteristic features of the coupled spin–orbital excitations to the complex magnetic behavior resulting from the interplay between electronic bands, spin–orbit coupling, Coulomb interactions, and structural distortion effects, as realized in the compounds NaOsO3, Ca2RuO4, and Sr2IrO4.

Post-growth annealing effects on charge and spin excitations in Nd2−xCexCuO4

We report a Cu K- and L$_3$-edge resonant inelastic x-ray scattering study of charge and spin excitations of bulk Nd$_{2-x}$Ce$_x$CuO$_4$, with focus on post-growth annealing effects. For the parent compound Nd$_2$CuO$_4$ ($x = 0$), a clear charge-transfer gap is observed in the as-grown state, whereas the charge excitation spectra indicate that electrons are doped in the annealed state. This is consistent with the observation that annealed thin-film and polycrystalline samples of RE$_2$CuO$_4$ (RE = rare earth) can become metallic and superconducting at sufficiently high electron concentrations without Ce doping. For $x = 0.16$, a Ce concentration for which it is known that oxygen reduction destroys long-range antiferromagnetic order and induces superconductivity, we find that the high-energy spin excitations of non-superconducting as-grown and superconducting annealed crystals are nearly identical. This finding is in stark contrast to the significant changes in the low-energy spin excitations previously observed via neutron scattering.

New-phase retention in colloidal core/shell nanocrystals via pressure-modulated phase engineering.

Core/shell nanocrystals (NCs) integrate collaborative functionalization that would trigger advanced properties, such as high energy conversion efficiency, nonblinking emission, and spin–orbit coupling. Such prospects are highly correlated with the crystal structure of individual constituents. However, it is challenging to achieve novel phases in core/shell NCs, generally non-existing in bulk counterparts. Here, we present a fast and clean high-pressure approach to fabricate heterostructured core/shell MnSe/MnS NCs with a new phase that does not occur in their bulk counterparts. We determine the new phase as an orthorhombic MnP structure (B31 phase), with close-packed zigzagged arrangements within unit cells. Encapsulation of the solid MnSe nanorod with an MnS shell allows us to identify two separate phase transitions with recognizable diffraction patterns under high pressure, where the heterointerface effect regulates the wurtzite → rocksalt → B31 phase transitions of the core. First-principles calculations indicate that the B31 phase is thermodynamically stable under high pressure and can survive under ambient conditions owing to the synergistic effect of subtle enthalpy differences and large surface energy in nanomaterials. The ability to retain the new phase may open up the opportunity for future manipulation of electronic and magnetic properties in heterostructured nanostructures.

Dynamical structure factor of a fermionic supersolid on an optical lattice

Interfacing unbiased quantum Monte Carlo simulations with state-of-art analytic continuation techniques, we obtain exact numerical results for dynamical density and spin correlations in the attractive Hubbard model, describing a spin-balanced two-dimensional cold Fermi gas on an optical lattice. We focus on half-filling, where on average one fermion occupies each lattice site, and the system displays an intriguing supersolid phase: a superfluid with a checkerboard density modulation. The coexistence of $U(1)$ broken symmetry and the density modulations makes this regime very challenging and interesting for the calculation of dynamical properties. We compare our unbiased results with state-of-the-art Generalized Random Phase Approximation calculations: both approaches agree on a well-defined low-energy Nambu-Goldstone collective mode in the density correlations, while the higher energy structures appear to differ significantly. We also observe an interesting high-energy spin mode. We argue that our results provide a robust benchmark for Generalized Random Phase Approximation techniques, which are widely considered to be the method of choice for dynamical correlations in Fermi gases. Also, our calculations yield new physical insight in the high-energy behavior of the dynamical structure factor of the attractive Hubbard model, which is a well known prototype lattice model for superconductors and is a fertile field to target the observation of collective modes in strongly correlated systems.

Inelastic light scattering in the spin cluster Mott insulator Cu2OSeO3

Clusters of single spins form the relevant spin entities in the formation of long-range magnetic order in spin cluster Mott insulators. Such type of spin order bears resemblance to molecular crystals, and we therefore may expect a prototypical spin wave spectrum which can be divided into low-energy external and high-energy internal cluster spin wave modes. Here, we study high-energy spin cluster excitations in the spin cluster Mott insulator Cu$_{2}$OSeO$_{3}$ by means of spontaneous Raman scattering. Multiple high-energy optical magnon modes are observed, of which the Raman-activity is shown to originate in the Elliot-Loudon scattering mechanism. Upon crossing the long-range ordering transition temperature the magnetic modes significantly broaden, corresponding to scattering from localized spin excitations within the spin clusters. Different optical phonon modes show a strong temperature dependence, evidencing a strong magnetoelectric coupling between optical phonons and the high-energy spin cluster excitations. Our results support the picture that Cu$_{2}$OSeO$_{3}$ can be regarded as a solid-state molecular crystal of spin nature.