Spin Exchange Interaction Research Articles

Unveiling hidden scaling relations in dissipative relaxation dynamics of strongly correlated quantum impurity systems.

Understanding the time evolution of strongly correlated open quantum systems (OQSs) in response to perturbations (quenches) is of fundamental importance to the precise control of quantum devices. It is, however, rather challenging in multi-impurity quantum systems because such evolution often involves multiple intricate dynamical processes. In this work, we apply the numerically exact hierarchical equations of motion approach to explore the influence of two different types of perturbations, i.e., sudden swapping of the energy levels of impurity systems and activating the inter-impurity spin-exchange interaction, on the dissipation dynamics of the Kondo-correlated two-impurity Anderson model over a wide range of energetic parameters. By evaluating the time-dependent impurity spectral function and other system properties, we analyze the time evolution of the Kondo state in detail and conclude a phenomenologically scaling relation for Kondo dynamics driven by these perturbations. The evolutionary scaling relationship is not only related to the Kondo characteristic energy TK but also significantly affected by the simultaneous non-Kondo dynamic characteristic energy. We expect these results will inspire subsequent theoretical studies on the dynamics of strongly correlated OQSs.

Quantum Spin Exchange Interactions Trigger O p Band Broadening for Enhanced Aqueous Zinc-Ion Battery Performance.

The pressing demand for large-scale energy storage solutions has propelled the development of advanced battery technologies, among which zinc-ion batteries (ZIBs) are prominent due to their resource abundance, high capacity, and safety in aqueous environments. However, the use of manganese oxide cathodes in ZIBs is challenged by their poor electrical conductivity and structural stability, stemming from the intrinsic properties of MnO2 and the destabilizing effects of ion intercalation. To overcome these limitations, our research delves into atomic-level engineering, emphasizing quantum spin exchange interactions (QSEI). These essential for modifying electronic characteristics, can significantly influence material efficiency and functionality. We demonstrate through density functional theory (DFT) calculations that enhanced QSEI in manganese oxides broadens the O p band, narrows the band gap, and optimizes both proton adsorption and electron transport. Empirical evidence is provided through the synthesis of Ru-MnO2 nanosheets, which display a marked increase in energy storage capacity, achieving 314.4 mAh g-1 at 0.2 A g-1 and maintaining high capacity after 2000 cycles. Our findings underscore the potential of QSEI to enhance the performance of TMO cathodes in ZIBs, pointing to new avenues for advancing battery technology.

Spinon Pairing Induced by Chiral In-Plane Exchange and the Stabilization of Odd-Spin Chern Number Spin Liquid in Twisted MoTe_{2}.

The unusual structure and symmetry of low-energy states in twisted transition metal dichalcogenides leads to large in-plane spin-exchange interactions between spin-valley locked holes. We demonstrate that this exchange interaction can stabilize a gapped spin-liquid phase with a quantized spin-Chern number of 3 when the twist angle is sufficiently small and the system lies in a Mott insulating phase. The gapped spin liquid may be understood as arising from spinon pairing in the DIII Altland-Zirnbauer symmetry class. Applying an out-of-plane electric field or increasing the twist angle is shown to drive a transition, respectively, to an anomalous Hall insulator or an in-plane antiferromagnet. Recent experiments indicate that a spin-Chern number 3 phase occurs in twisted MoTe_{2} at small twist angles with a transition to a quantum anomalous Hall phase as the twist angle is increased above a critical value of about 2.5° in the absence of an applied electric field.

Spin Exchange-Enabled Quantum Simulator for Large-Scale Non-Abelian Gauge Theories

A central requirement for the faithful implementation of large-scale lattice gauge theories (LGTs) on quantum simulators is the protection of the underlying gauge symmetry. Recent advancements in the experimental realizations of large-scale LGTs have been impressive, albeit mostly restricted to Abelian gauge groups. Guided by this requirement for gauge protection, we propose an experimentally feasible approach to implement large-scale non-Abelian SU(N) and U(N) LGTs with dynamical matter in d+1D, enabled by two-body spin-exchange interactions realizing local emergent gauge-symmetry stabilizer terms. We present two concrete proposals for 2+1DSU(2) and U(2) LGTs, including dynamical bosonic matter and induced plaquette terms, that can be readily implemented in current ultracold-molecule and next-generation ultracold-atom platforms. We provide numerical benchmarks showcasing experimentally accessible dynamics, and demonstrate the stability of the underlying non-Abelian gauge invariance. We develop a method to obtain the effective gauge-invariant model featuring the relevant magnetic plaquette and minimal gauge-matter coupling terms. Our approach paves the way towards near-term realizations of large-scale non-Abelian quantum link models in analog quantum simulators. Published by the American Physical Society 2024

Enhancing Magnetic Ordering in Two-Dimensional Metal-Organic Frameworks via Frontier Molecular Orbital Engineering.

Two-dimensional (2D) metal-organic frameworks (MOFs) have promise for use in lightweight permanent magnets in contrast to inorganic solid- or molecule-based magnets, but the realization of 2D MOF magnets with a high ordering temperature is limited by the typically weak spin exchange interactions. Here, we have proposed a frontier molecular orbital engineering strategy for modulating magnetism in 2D MOFs. It shows that the magnetic ground state can be mediated by two intra-atomic spin exchange pathways in organic ligands, akin to the Bloch and Heisenberg models, depending on the shape of the frontier orbitals of the organic ligands. By engineering the shape of the lowest unoccupied molecular orbital (LUMO) via chemical hydrogenation, we achieved a nearly 11-fold increase in the ordering temperature. In particular, a quantitative analysis shows that the ordering temperature increases linearly with the orbital delocalization index of the ligands' LUMO. This work suggests a general frontier orbital engineering approach for modulating the spin exchange interaction in 2D MOF magnets.

Above-room-temperature intrinsic ferromagnetism in ultrathin van der Waals crystal Fe3+xGaTe2

Two-dimensional (2D) van der Waals (vdW) magnets are crucial for ultra-compact spintronics. However, so far, no vdW crystal has exhibited tunable above-room-temperature intrinsic ferromagnetism in the 2D ultrathin regime. Here, we report the tunable above-room-temperature intrinsic ferromagnetism in ultrathin vdW crystal Fe3+xGaTe2 (x = 0 and 0.3). By increasing the Fe content, the Curie temperature (TC) and room-temperature saturation magnetization of bulk Fe3+xGaTe2 crystals are enhanced from 354 to 376 K and 43.9 to 50.4 emu·g−1, respectively. Remarkably, the robust anomalous Hall effect in 3-nm Fe3.3GaTe2 indicates a record-high TC of 340 K and a large room-temperature perpendicular magnetic anisotropy energy of 6.6 × 105 J m−3, superior to other ultrathin vdW ferromagnets. First-principles calculations reveal the asymmetric density of states and an additional large spin exchange interaction in ultrathin Fe3+xGaTe2 responsible for robust intrinsic ferromagnetism and higher TC. This work opens a window for above-room-temperature ultrathin 2D magnets in vdW-integrated spintronics.

Ground state magnetic structure and magnetic field effects in the layered honeycomb antiferromagnet YbOCl

YbOCl is a representative member of the van der Waals layered honeycomb rare-earth chalcohalide RChX (R = rare earth; Ch = O, S, Se, and Te; and X = F, Cl, Br, and I) family reported recently. Its spin ground state remains to be explored experimentally. We grew high-quality single crystals of YbOCl and conducted comprehensive thermodynamic, elastic, and inelastic neutron scattering experiments down to 50 mK. The experiments reveal an antiferromagnetic phase below 1.3 K which is identified as a spin ground state with an intralayer ferromagnetic and interlayer antiferromagnetic ordering. By applying sophisticated numerical techniques to a honeycomb (nearest-neighbor)–triangle (next-nearest-neighbor) model Hamiltonian which accurately describes the highly anisotropic spin system, we are able to simulate the experiments well and determine the diagonal and off-diagonal spin-exchange interactions. The simulations give an antiferromagnetic Kitaev term comparable to the Heisenberg one. The experiments under magnetic fields allow us to establish a magnetic field–temperature phase diagram around the spin ground state. Most interestingly, a relatively small magnetic field (∼0.3 to 3 T) can significantly suppress the antiferromagnetic order, suggesting an intriguing interplay of the Kitaev interaction and magnetic fields in the spin system. The present study provides fundamental insights into the highly anisotropic spin systems and opens a window to look into Kitaev spin physics in a rare-earth-based system. Published by the American Physical Society 2024

Two-axis twisting using Floquet-engineered XYZ spin models with polar molecules.

Polar molecules confined in an optical lattice are a versatile platform to explore spin-motion dynamics based on strong, long-range dipolar interactions1,2. The precise tunability3 of Ising and spin-exchange interactions with both microwave and d.c. electric fields makes the molecular system particularly suitable for engineering complex many-body dynamics4-6. Here we used Floquet engineering7 to realize new quantum many-body systems of polar molecules. Using a spin encoded in the two lowest rotational states of ultracold 40K87Rb molecules, we mutually validated XXZ spin models tuned by a Floquet microwave pulse sequence against those tuned by a d.c. electric field through observations of Ramsey contrast dynamics. This validation sets the stage for the realization of Hamiltonians inaccessible with static fields. In particular, we observed two-axis twisting8 mean-field dynamics, generated by a Floquet-engineered XYZ model using itinerant molecules in two-dimensional layers. In the future, Floquet-engineered Hamiltonians could generate entangled states for molecule-based precision measurement9 or could take advantage of the rich molecular structure for quantum simulation of multi-level systems10,11.

Quenching controlled spin exchange interactions and spin selective electron transfer for oxygen evolution reactions

The utilization of magnetic field to enhance electrocatalytic activity has become an effective strategy garnering significant attention in the field of electrocatalysis. Herein, we employ a combination of electrospinning and quenching techniques to successfully synthesize high-entropy oxide (HEO) (FeCoNiCrMn)3O4. The HEO exhibited ferromagnetic properties and further increased the saturation magnetization after the quenching process, primarily due to temperature-mediated magnetic exchange interactions. The OER performance is significantly improved by employing a ferromagnetic ordered catalyst as a spin polarizer in the presence of a magnetic field. The introduction of an exterior magnetic field (∼130 mT) significantly improved the OER performance of HEO-LN (HEO quenching in liquid nitrogen), reducing the overpotential by 39.4 mV at 10 mA cm-2. The improved OER performance is due to the presence of the magnetic field-enhanced electron spin polarization, reducing electron repulsion and enhancing orbital hybridization. These findings not only provide crucial insights into understanding reactions involving magnetic field-induced electrochemistry but also contribute to the rational design of electrocatalysts with magnetic effect.

Evolution of structure, magnetism, and electronic/thermal-transports of Ti(Cr)-substituted Fe2CrV all-d-metal Heusler ferromagnets

All-d-metal full-Heusler alloys possess superior mechanical properties and high spin polarization, which would play an important role in spintronic applications. Despite this, their electrical and thermal transport properties have not been comprehensively investigated till now. In this work, we present an analysis on the evolution of structural, magnetic and transport properties of Cr- and Ti-substituted Fe2CrV all-d-metal Heusler alloys by combining theoretical calculations and experiments. Both series of alloys crystallize in Hg2CuTi-type structure. With increasing Ti doping, the calculated total magnetic moments of Fe50Cr25V25-xTix decrease linearly. The experimental saturation magnetization is highly consistent with theoretical calculations and Slater-Pauling rule when x < 4, indicating the highly ordered atomic occupation. The magnetization and Curie temperature can be significantly tuned by altering spin polarizations and exchange interactions. The introduction of the foreign atom, Ti, results in a linear increase in residual resistivity, while electron-phonon scattering keeps relatively constant. The maximum values for electrical and thermal transport properties are observed in the stoichiometric Fe2CrV composition.

Unveiling chiral states in the XXZ chain: finite-size scaling probing symmetry-enriched c = 1 conformal field theories

We study the low-energy properties of the one-dimensional spin-1/2 XXZ chain with time-reversal symmetry-breaking pseudo-scalar chiral interaction and propose a phase diagram for the model. In the integrable case of the isotropic Heisenberg model with the chiral interaction, we employ the thermodynamic Bethe ansatz to find “chiralization”, the response of the ground state versus the strength of the pseudo-scalar chiral interaction of a chiral Heisenberg chain. Unlike the magnetization case, the chirality of the ground state remains zero until the transition point corresponding to critical coupling αc = 2J/π with J being the antiferromagnetic spin-exchange interaction. The central-charge c = 1 conformal field theories (CFTs) describe the two phases with zero and finite chirality. We show for this particular case and conjecture more generally for similar phase transitions that the difference between two emergent CFTs with identical central charges lies in the symmetry of their ground state (lightest weight) primary fields, i.e., the two phases are symmetry-enriched CFTs. At finite but small temperatures, the non-chiral Heisenberg phase acquires a finite chirality that scales with the temperature quadratically. We show that the finite-size effect around the transition point probes the transition.

Spin-Phonon Coupling in Iron-Doped Ultrathin Bismuth Halide Perovskite Derivatives.

Spin in semiconductors facilitates magnetically controlled optoelectronic and spintronic devices. In metal halide perovskites (MHPs), doping magnetic ions is proven to be a simple and efficient approach to introducing a spin magnetic momentum. In this work, we present a facile metal ion doping protocol through the vapor-phase metal halide insertion reaction to the chemical vapor deposition (CVD)-grown ultrathin Cs3BiBr6 perovskites. The Fe-doped bismuth halide (Fe:CBBr) perovskites demonstrate that the iron spins are successfully incorporated into the lattice, as revealed by the spin-phonon coupling below the critical temperature Tc around 50 K observed through temperature-dependent Raman spectroscopy. Furthermore, the phonons exhibit significant softening under an applied magnetic field, possibly originating from magnetostriction and spin exchange interaction. The spin-phonon coupling in Fe:CBBr potentially provides an efficient way to tune the spin and lattice parameters for halide perovskite-based spintronics.

Momentum-exchange interactions in a Bragg atom interferometer suppress Doppler dephasing.

Large ensembles of laser-cooled atoms interacting through infinite-range photon-mediated interactions are powerful platforms for quantum simulation and sensing. Here we realize momentum-exchange interactions in which pairs of atoms exchange their momentum states by collective emission and absorption of photons from a common cavity mode, a process equivalent to a spin-exchange or XX collective Heisenberg interaction. The momentum-exchange interaction leads to an observed all-to-all Ising-like interaction in a matter-wave interferometer. A many-body energy gap also emerges, effectively binding interferometer matter-wave packets together to suppress Doppler dephasing in analogy to Mössbauer spectroscopy. The tunable momentum-exchange interaction expands the capabilities of quantum interaction-enhanced matter-wave interferometry and may enable the realization of exotic behaviors, including simulations of superconductors and dynamical gauge fields.

Investigation of structural phase stability, modified magnetic spin order and low temperature spin glass-like phase transitions in Sc-doped M-type BaFe12O19 hexaferrite

This work used two approaches of mechanical alloying before high temperature solid state reaction to synthesize BaFe12-xScxO19 (x = 0.5 to 6.0) system. Rietveld refinement of X-ray diffraction patterns showed the formation of extra phases at higher Sc doping, along with the main magnetoplumbite structure. Raman spectroscopy suggested random distribution of Sc ions at the Fe-sites of hexaferrite structure. X-ray photoelectron spectroscopy (XPS) confirmed the +3 charge state at the Fe/Sc-sites. The Fe 3s band suggested dilution of ferromagnetic 3s-3d spin exchange interactions. The neutron diffraction study re-confirmed random occupancy of the non-magnetic Sc3+ ions at Fe3+ sites of the Sc doped Ba hexaferrite system. The transformation of magnetic spin order from collinear to non-collinear state has shown spin glass-like features at low temperature regime in the dc magnetization curves. This is an effect of dilution of Fe–O–Fe ferrimagnetic super exchange interactions and spin frustration in Sc-doped samples.

Motion of Two-Dimensional Excitons in Momentum Space Leads to Pseudospin Distribution Narrowing on the Bloch Sphere.

Motional narrowing implies narrowing induced by motion; for example, in nuclear magnetic resonance, the thermally induced random motion of the nuclei in an inhomogeneous environment leads to a counterintuitive narrowing of the resonance line. Similarly, the excitons in monolayer semiconductors experience magnetic inhomogeneity: the electron-hole spin-exchange interaction manifests as an in-plane pseudomagnetic field with a periodically varying orientation inside the exciton band. The excitons undergo random momentum scattering and pseudospin precession repeatedly in this inhomogeneous magnetic environment, typically resulting in fast exciton depolarization. On the contrary, we show that such magnetic inhomogeneity averages out at high scattering rates due to motional narrowing. Physically, a faster exciton scattering leads to a narrower pseudospin distribution on the Bloch sphere, implying a nontrivial improvement in exciton polarization. The in-plane nature of the pseudomagnetic field enforces a contrasting scattering dependence between the circularly and linearly polarized excitons, providing a spectroscopic way to gauge the sample quality.

Interlayer-Coupling-Driven High-Temperature Superconductivity in La_{3}Ni_{2}O_{7} under Pressure.

The newly discovered high-temperature superconductivity in La_{3}Ni_{2}O_{7} under pressure has attracted a great deal of attention. The essential ingredient characterizing the electronic properties is the bilayer NiO_{2} planes coupled by the interlayer bonding of 3d_{z^{2}} orbitals through the intermediate oxygen atoms. In the strong coupling limit, the low-energy physics is described by an intralayer antiferromagnetic spin-exchange interaction J_{∥} between 3d_{x^{2}-y^{2}} orbitals and an interlayer one J_{⊥} between 3d_{z^{2}} orbitals. Taking into account Hund's rule on each site and integrating out the 3d_{z^{2}} spin degree of freedom, the system reduces to a single-orbital bilayer t-J model based on the 3d_{x^{2}-y^{2}} orbital. By employing the slave-boson approach, the self-consistent equations for the bonding and pairing order parameters are solved. Near the physically relevant 1/4-filling regime (doping δ=0.3∼0.5), the interlayer coupling J_{⊥} tunes the conventional single-layer d-wave superconducting state to the s-wave one. A strong J_{⊥} could enhance the interlayer superconducting order, leading to a dramatically increased T_{c}. Interestingly, there could exist a finite regime in which an s+id state emerges.

Emergent Inflation of the Efimov Spectrum under Three-Body Spin-Exchange Interactions.

We resolve the unexpected and long-standing disagreement between experiment and theory in the Efimovian three-body spectrum of ^{7}Li, commonly referred to as the lithium few-body puzzle. Our results show that the discrepancy arises out of the presence of strong nonuniversal three-body spin-exchange interactions, which enact an effective inflation of the universal Efimov spectrum. This conclusion is obtained from a thorough numerical solution of the quantum mechanical three-body problem, including precise interatomic interactions and all spin degrees of freedom for three alkali-metal atoms. Our results show excellent agreement with the experimental data regarding both the Efimov spectrum and the absolute rate constants of three-body recombination, and in addition reveal a general product propensity for such triatomic reactions in the Paschen-Back regime, stemming from Wigner's spin conservation rule.

Electric-field-driven ferromagnetic response in Janus MnReX3 (X = Se, S) monolayer via asymmetric interface orbital hybridization

Abstract Regulating spin-related electronic structures of two dimensional (2D) materials by an external electric field plays a substantial role in achieving spintronic and multistate information storage. However, electric-field-dependent ferromagnetic behavior at atomic-thick 2D materials is very difficult to be realized due to their intrinsic inversion symmetry, in which the symmetric spatial distribution of charge density makes it become insensitive to spontaneous polarization from external electric field. Herein, a new-type Janus MnReX3 (X = Se, S) monolayer with noncentrosymmetric configuration in which their orbital hybridization at internal interface can be engineered by rearranging the spatial symmetry of out-of-plane charge density. As a result, the spin exchange interaction among magnetic sites can be regulated by the electric-field-driven charge density redistribution, leading to a controllable ferromagnetic behavior at room temperature. Our results not only suggest a promising strategy to regulate the ferromagnetic response by reducing the crystal symmetry, but also provide a new insight into designing 2D magnetic materials.

Does Mn2+-Mn2+ Spin-Exchange Interaction Involve Mn2+ Luminescence of Mn2+-Doped/Concentrated Materials?

Mn2+-doped luminescent quantum dots play a vital role in the fields of optoelectronic materials and devices. The presence of five unpaired d electrons in Mn2+ ions facilitates spin-exchange interactions, profoundly influencing the spin state of the exciton and thereby impacting the optical behaviors. However, the involvement and specific effects of spin-exchange interactions on optical properties of Mn2+ in insulating bulk phosphors remain a subject of controversy, attributed to the scarcity of solid evidence and the interference of various factors. In this Perspective, we delve into the fundamentals and recent advancements concerning the Mn2+-Mn2+ spin-exchange interaction in Mn2+ luminescent materials. The discussion encompasses various aspects, such as types of magnetic coupling, the coupling mechanism in optical ground state and excited state, as well as effective measures for verification. This Perspective underscores the existing knowledge gaps in Mn2+-doped bulk phosphors, highlighting significant opportunities for further exploration and advancement in both fundamental and applied research within this domain.

Ortho-positronium annihilation processes in Y zeolites under different environments by measurements of the energy spectra of the positron annihilation radiation

Measurements of the energy distribution of the positron annihilation radiation in Y zeolites are carried out to elucidate the various ortho-positronium annihilation processes that take place in these microporous materials and relate them to the ortho-positronium lifetime components observed by positron annihilation lifetime spectroscopy in earlier studies. Y zeolites with various Si/Al ratios in the range from 2.6 to 40 are investigated under a controlled atmosphere of N2 gas and after exposure to the atmosphere. The ortho-positronium annihilation modes are characterized by analyzing the γ-ray spectra through the use of the f3γ index, which represents the fraction of 3γ-annihilation, and the S parameter. The proportion of ortho-positronium self-annihilation is found to be no less than 15% in N2 gas, but drastically decreases by the physisorption of water molecules and possibly positronium spin exchange interaction with oxygen in the atmosphere. The presence of water molecules suppresses ortho-positronium intrinsic annihilation and, at the same time, promotes ortho-positronium pick-off annihilation in the pores. Similarly, the S parameter rises due to an increased contribution from para-positronium annihilation and ortho-positronium pick-off annihilation, which is also consistent with the physisorption of water and positronium spin exchange. In conjunction with the previously measured ortho-positronium lifetime components, the specific ortho-positronium annihilation sites and processes in these porous materials under different environments are determined and a complete picture of the ortho-positronium behavior in Y zeolites is obtained.Graphical abstractγ-ray energy spectra of Y zeolites with a Si/Al ratio = 2.6 measured in N2 gas and water-saturated zeolites