Competing Exchange Interactions Research Articles

Noncentrosymmetric Triangular Magnet CaMnTeO6: Strong Quantum Fluctuations and Role of s0 versus s2 Electronic States in Competing Exchange Interactions.

Noncentrosymmetric triangular magnets offer a unique platform for realizing strong quantum fluctuations. However, designing these quantum materials remains an open challenge attributable to a knowledge gap in the tunability of competing exchange interactions at the atomic level. Here, a new noncentrosymmetric triangular S=3/2 magnet CaMnTeO6 is created based on careful chemical and physical considerations. The model material displays competing magnetic interactions and features nonlinear optical responses with the capability of generating coherent photons. The incommensurate magnetic ground state of CaMnTeO6 with an unusually large spin rotation angle of 127°(1) indicates that the anisotropic interlayer exchange is strong and competing with the isotropic interlayer Heisenberg interaction. The moment of 1.39(1)µB, extracted from low-temperature heat capacity and neutron diffraction measurements, is only 46% of the expected value of the static moment 3µB. This reduction indicates the presence of strong quantum fluctuations in the half-integer spin S=3/2 CaMnTeO6 magnet, which is rare. By comparing the spin-polarized band structure, chemical bonding, and physical properties of AMnTeO6 (A=Ca, Sr, Pb), how quantum-chemical interpretation can illuminate insights into the fundamentals of magnetic exchange interactions, providing a powerful tool for modulating spin dynamics with atomically precise control is demonstrated.

Charge-density wave mediated quasi-one-dimensional Kondo lattice in stripe-phase monolayer 1T-NbSe2

The heavy fermion physics is dictated by subtle competing exchange interactions, posing a challenge to their understanding. One-dimensional (1D) Kondo lattice model has attracted special attention in theory, because of its exact solvability and expected unusual quantum criticality. However, such experimental material systems are extremely rare. Here, we demonstrate the realization of quasi-1D Kondo lattice behavior in a monolayer van der Waals crystal NbSe2, that is driven into a stripe phase via Se-deficient line defects. Spectroscopic imaging scanning tunneling microscopy measurements and first-principles calculations indicate that the stripe-phase NbSe2 undergoes a novel charge-density wave transition, creating a matrix of local magnetic moments. The Kondo lattice behavior is manifested as a Fano resonance at the Fermi energy that prevails the entire film with a high Kondo temperature. Importantly, coherent Kondo screening occurs only in the direction of the stripes. Upon approaching defects, the Fano resonance exhibits prominent spatial 1D oscillations along the stripe direction, reminiscent of Kondo holes in a quasi-1D Kondo lattice. Our findings provide a platform for exploring anisotropic Kondo lattice behavior in the monolayer limit.

Interplay between transition-metal K-edge XMCD, slight structural distortions and magnetism in a series of trimetallic (CoxNi(1-x))4[Fe(CN)6]3/8 Prussian blue analogues.

The magnetic properties of a series of trimetallic (Co,Ni)Fe Prussian blue analogues (PBAs) were investigated by SQUID magnetometry and X-ray magnetic circular dichroism (XMCD) at the three transition metal (TM) K-edges. In turn, the PBA trimetallic series was used as a tool in order to better understand the information contained in TM K-edge XMCD and particularly the chemical nature of the probed species (extended sub-lattice or localized entities). The results show that the magnetic behavior of the compounds is dictated by competing exchange interactions between the Co-Fe and Ni-Fe pairs, without spin frustration. They also show that XMCD at the TM K-edge is a local atomic probe of the element at the N side of the cyanide bridge and a local probe of the absorbing atom and its first magnetic neighbors on the C side of the bridge. At last, XMCD at the TM K-edge turns out to be highly sensitive to very small structural distortions.

Enhanced Exchange Bias in Epitaxial High-Entropy Oxide Heterostructures.

High-entropy oxides (HEOs) have gained significant interest in recent years due to their unique structural characteristics and potential to tailor functional properties. However, the electronic structure of the HEOs currently remains vastly unknown. In this work, combining magnetometry measurements, scanning transmission electron microscopy, and element-specific X-ray absorption spectroscopy, the electronic structure and magnetic properties of the perovskite-HEO La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 epitaxial thin films are systemically studied. It is found that enhanced magnetic frustration emerges from competing exchange interactions of the five transition-metal cations with energetically favorable half-filled/full-filled electron configurations, resulting in an unprecedented large vertical exchange bias effect in the single-crystalline films. Furthermore, our findings demonstrate that the La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 layer with a thickness down to 1 nm can be used as a pinning layer and strongly coupled with a ferromagnetic La0.7Sr0.3MnO3 layer, leading to a notable exchange bias and coercivity enhancement in a cooling field as small as 5 Oe. Our studies not only provide invaluable insight into the electronic structure of HEOs but also pave the way for a new era of large bias materials for spintronics devices.

Coexistence of spin liquid state and magnetic correlations in 3d-5d based triangular-lattice antiferromagnet Sr3CuIr2O9

Here, we report detailed lattice structure, magnetization (dc and ac) and specific heat measurements on a 3d-5d based new triple-perovskite material Sr3CuIr2O9. The Sr/Cu forms a layered structure of triangular-lattice while the Ir forms Ir2O9 dimers which lie in chain as well as simultaneously makes layered triangular-lattice with neighboring atoms. Due to random site-sharing with Sr2+, the Cu2+ (3d 9, spin-1/2) forms a diluted magnetic lattice, thus giving a disordered in-plane exchange interaction. Opposed to conventional model, the Ir5+ (5d 4, = 0) is believed to be magnetic here which participates both in-chain and in-plane magnetic interactions. This complex lattice structure driven competing exchange interaction leads the ground state to a gapless quantum-spin-liquid state which coexists with (weak) ferromagnetic spin correlations. While underling the importance of spin state (spin-1/2), we believe that the combined effect of lattice structure, geometric frustration, spin–orbit coupling and spin state has given rise this interesting ground state in this material.

Fluctuating magnetic droplets immersed in a sea of quantum spin liquid

The search of quantum spin liquid (QSL), an exotic magnetic state with strongly fluctuating and highly entangled spins down to zero temperature, is a main theme in current condensed matter physics. However, there is no smoking gun evidence for deconfined spinons in any QSL candidate so far. The disorders and competing exchange interactions may prevent the formation of an ideal QSL state on frustrated spin lattices. Here we report comprehensive and systematic measurements of the magnetic susceptibility, ultralow-temperature specific heat, muon spin relaxation (μSR), nuclear magnetic resonance (NMR), and thermal conductivity for NaYbSe2 single crystals, in which Yb3+ ions with effective spin-1/2 form a perfect triangular lattice. All these complementary techniques find no evidence of long-range magnetic order down to their respective base temperatures. Instead, specific heat, μSR, and NMR measurements suggest the coexistence of quasi-static and dynamic spins in NaYbSe2. The scattering from these quasi-static spins may cause the absence of magnetic thermal conductivity. Thus, we propose a scenario of fluctuating ferrimagnetic droplets immersed in a sea of QSL. This may be quite common on the way pursuing an ideal QSL, and provides a brand new platform to study how a QSL state survives impurities and coexists with other magnetically ordered states.

Phase transitions in the four-state Potts model with competing exchange interactions: Application of the Wang-Landau algorithm

Phase transitions in the four-state Potts model with competing exchange interactions: Application of the Wang-Landau algorithm

Phase diagram of the antiferromagnetic Ising model on a body-centered cubic lattice with competing exchange interactions under a magnetic field

Phase diagram of the antiferromagnetic Ising model on a body-centered cubic lattice with competing exchange interactions under a magnetic field

Spin Wave Spectra in Pseudoperovskite Manganites with Superexchange Interaction Competition

In compounds La1/3Ca2/3MnO3 and BiMnO3, a calculation of spin-wave dispersion dependences along pseudoperovskite directions of reciprocal space is made. The model includes orbitally dependent superexchange interaction and single-ion anisotropy. Considered compounds present competing exchange interactions within magnetic unit cell because of orbital or charge-orbital ordering. The nearest neighbor superexchange interaction is taken into account. The magnetic structure and dispersion dependences of spin waves frequencies are calculated within the framework of regular multi-sublattice model. The peculiarities of frustrated magnetic spin-wave spectra are found. It is shown, that crossing and splitting of spin-waves branches in non-symmetric points of magnetic Brillouin zone is a common feature of the spectra due to exchange competition. The band structure of Г-point spectra for both compounds are predicted.

Stability of hopfions in bulk magnets with competing exchange interactions

Magnetic hopfions are string-like three-dimensional topological solitons, characterised by the Hopf number. They serve as a fundamental prototype for three-dimensional magnetic quasiparticles and are an inspiration for novel device concepts in the field of spintronics. Based on a micromagnetic model and without considering temperature, the existence of such hopfions has been predicted in certain magnets with competing exchange interactions. However, physical realisation of freely moving hopfions in bulk magnets have so far been elusive. Here, we consider an effective Heisenberg model with competing exchange interactions and study the stability of small toroidal hopfions with Hopf number ${Q}_{\text{H}}=1$ by finding first-order saddle points on the energy surface representing the transition state for the decay of hopfions via the formation of two coupled Bloch points. We combine the geodesic nudged elastic band method and an adapted implementation of the dimer method to resolve the sharp energy profile of the reaction path near the saddle point. Our analysis reveals that the energy barrier can reach substantial height and is largely determined by the size of the hopfion relative to the lattice constant.

Lifetime, collapse, and escape paths for hopfions in bulk magnets with competing exchange interactions

The lifetimes of magnetic hopfions on a discrete lattice with competing exchange interactions are calculated within the framework of the transition state theory for magnetic degrees of freedom. Three sets of discrete model parameters corresponding to the same continuous micromagnetic model are considered. Minimal energy paths for hopfion collapses were found on the multidimensional energy surface of the system. The activation energies of the collapse processes have been calculated. It turned out that the activation energy differs significantly for the three considered values of the parameters, which indicates the importance of lattice effects, when the hopfion radius equals several lattice constants. Along with the collapse, the hopfion escape process through the sample boundary is studied. It is shown that this process does not require an activation energy. The lifetimes of hopfions are found and it is shown that they can exist only at temperatures of a few kelvins and practically cannot be generated due to thermal fluctuations.

Multiple-[formula omitted] instability under fourth-order inplane single-ion anisotropy

Multiple-Q instability under tetragonal single-ion anisotropy is theoretically investigated. By performing the simulated annealing for a spin model with the momentum-resolved interaction and fourth-order inplane single-ion anisotropy on a square lattice, we find that the interplay between the competing exchange interactions in momentum space and single-ion anisotropy leads to various field-induced double-Q states in the ground state. In particular, we show that a double-Q vortex crystal emerges when the interactions at high-harmonic wave vectors are comparable to those at wave vectors that give the dominant contributions. Our results underscore the importance of magnetic anisotropy, which brings about the multiple-Q instability in centrosymmetric magnets.

Evolution of anisotropic magnetic properties through helix-to-fan transition in helical antiferromagnetic EuCo2As2

A helimagnet comprises a noncollinear spin structure formed by competing exchange interactions. Recent advances in antiferromagnet-based functionalities have broadened the scope of target materials to include noncollinear antiferromagnets. However, a microscopic understanding of the magnetic anisotropy associated with the intricate evolution of noncollinear spin states has not yet been accomplished. Here, we have explored the anisotropic magnetic aspects in a layered helimagnet of EuCo2As2 by measuring the magnetic field and angle dependence of the magnetic torque. By adopting an easy-plane anisotropic spin model, we can visualize the detailed spin configurations that evolve in the presence of rotating magnetic fields. This is directly related to the two distinctive magnetic phases characterized by the reversal of the magnetic torque variation across the helix-to-fan transition. Our advanced approach provides an in-depth understanding of the anisotropic properties of noncollinear-type antiferromagnets and a useful guidance for potential applications in spin-processing functionalities.

Magnetic Toroidal Moment under Partial Magnetic Order in Hexagonal Zigzag-Chain Compound Ce3TiBi5

We theoretically investigate an antiferromagnetic structure in a hexagonal zigzag-chain compound Ce$_3$TiBi$_5$, which shows a linear magnetoelectric effect in metals and an unfamiliar temperature dependence of magnetic susceptibility. We find a partial magnetic order as a coexistence of a nonmagnetic zigzag chain and staggered antiferromagnetic zigzag chains. The latter accompany in-plane magnetic toroidal dipole moments which are responsible for the observed behaviors. We show that magnetic frustration arising from competing exchange interactions plays an important role to realize such a partial magnetic order. Furthermore, we present the important spin-orbit coupling parameters to induce the physical phenomena driven by the magnetic toroidal dipole moment, such as the linear magnetoelectric effect and nonlinear transport.

Quantum Phase Diagram of a Frustrated Spin-1/2 Ferro-Antiferromagnetic Normal Ladder.

In this work, we consider a frustrated two-leg spin-1/2 ladder composed of Heisenberg ferromagnetic and antiferromagnetic spin-1/2 chains, and nearest spins from different legs interact via Heisenberg type rung exchange interactions that can be either ferromagnetic or antiferromagnetic in nature. The competing exchange interactions in the system lead to five different quantum phases like ferromagnetic, non-collinear ferrimagnetic (NCF), , antiferromagnetic and dimer phases. The quantum phase diagram is constructed for the Heisenberg spin-1/2 model and the phases are characterized using the correlation functions which are calculated by the density matrix renormalization group method. We also analyze the stability of phase and calculate the pitch angle in the NCF phase.

On the magnetic-structure origin of giant magnetostrictive effect in MnCoSi-based metallic helimagnets

Giant magnetostrictive effect, the huge volume and/or shape change of a material under an external magnetic field, is recently discovered in helimagnets with large magnetoelastic interactions. Here we revisit this effect in MnCoSi, a helical metamagnet with a unique Lifshitz tricritical point. By introducing minimal amount of Ni, the modified competing exchange interaction simultaneously lowers the tricritical temperature and even critical field of metamagnetism, leading to a giant, reversible, low-field magnetostrictive effect at ambient temperature. When applying a cyclic low field of 0.5 T, a giant reversible magnetostriction of 550 ppm can be achieved and maintained at 300 K. Interestingly, by advanced 3D-vector magnetic field measurement, a strong relation is found between magnetocrystalline anisotropy and the critical field of magnetostrictive effect. In-situ neutron powder diffraction results further reveal that the incommensurate helical antiferromagnetic structure with moment lying in ab plane transits into a ferromagnetic structure along b axis with increasing magnetic fields. During this metamagnetic transition, dramatical spin rotation triggers sharp anisotropic lattice change via strong magnetoelastic coupling, resulting in giant magnetostrictive effect. The saturated magnetostriction value is closely related with the amplitude of spin rotations. These findings not only design of a potential MnCoSi-based magnetostrictive material but also uncover the specific evolution of magnetic structures in the metamagnetic transition and the possible mechanism behind the macroscopic size change.

Magnetic hopfions in solids

Hopfions are an intriguing class of string-like solitons, named according to a classical topological concept classifying three-dimensional direction fields. The search for hopfions in real physical systems has been ongoing for nearly half a century, starting with the seminal work of Faddeev. However, so far, realizations in bulk solids are missing. Here, we show that hopfions appear as emergent particles of the classical Heisenberg model with competing exchange interactions. This requires going beyond the model approach used in prior work and deriving a general micromagnetic energy functional directly from a spin-lattice Hamiltonian. We present a definite parameter space in which the existence of hopfions is possible. This opens a concrete vista to combine computational approaches such as density functional theory with material informatics to find magnetic crystals that can host hopfions. As proof of principle, we show how zero-field hopfions can be visualized by the means of off-axis electron holography in a transmission electron microscope.

Possible coexistence of short-range resonating valence bond and long-range stripe correlations in the spatially anisotropic triangular-lattice quantum magnet Cu2 (OH) 3NO3

We show that short-range resonating valence bond correlations and long-range order can coexist in the ground state (GS) of a frustrated spin system. Our study comprises a comprehensive investigation of the quantum magnetism on the structurally disorder-free single crystal of ${\mathrm{Cu}}_{2}{(\mathrm{OH})}_{3}{\mathrm{NO}}_{3}$, which realizes the $s$ = 1/2 Heisenberg model on a spatially anisotropic triangular lattice. Competing exchange interactions determined by fitting the magnetization measured up to 55 T give rise to an exotic GS wave function with the coexistence of the dominant short-range resonating valence bond correlations and weak long-range stripe order (ordered moment ${M}_{0}=|\ensuremath{\langle}{s}_{i}^{z}\ensuremath{\rangle}|\ensuremath{\sim}0.02$). At low temperatures, a first-order spin-flop transition is visible at $\ensuremath{\sim}$1--3 T. As the applied field further increases, another two magnetic field induced quantum phase transitions are observed at $\ensuremath{\sim}$14--19 and $\ensuremath{\sim}$46--52 T, respectively. Simulations of the Heisenberg exchange model show semiquantitative agreement with the magnetic-field modulation of these unconventional phases, as well as the absence of visible magnetic reflections in neutron diffraction, thus supporting the GS of the spin system of ${\mathrm{Cu}}_{2}{(\mathrm{OH})}_{3}{\mathrm{NO}}_{3}$ may be approximate to a quantum spin liquid. Our study establishes structurally disorder-free magnetic materials with spatially anisotropic exchange interactions as a possible arena for spin liquids.

Sign-tunable anisotropic magnetoresistance and electrically detectable dual magnetic phases in a helical antiferromagnet

Emerging from competing exchange interactions, the helimagnetic order describes a noncollinear spin texture of antiferromagnets. Although collinear antiferromagnets act as the elemental building blocks of antiferromagnetic (AFM) spintronics, until now, the potential of implementing spintronic functionality in noncollinear antiferromagnets has not been clarified. Here, we propose an AFM helimagnet of EuCo2As2 as a novel single-phase spintronic material that exhibits a remarkable sign reversal of anisotropic magnetoresistance (AMR). The contrast in the AMR arises from two electrically distinctive magnetic phases with spin reorientation that is driven by the magnetic field prevailing in the easy plane, which converts the AMR from positive to negative. Furthermore, based on an easy-plane anisotropic spin model, we theoretically identified various AFM memory states associated with the evolution of the spin structure under magnetic fields. The results revealed the potential of noncollinear antiferromagnets for application in the development of spintronic devices.

Theoretical Design of Optimal Molecular Qudits for Quantum Error Correction.

We pinpoint the key ingredients ruling decoherence in multispin clusters, and we engineer the system Hamiltonian to design optimal molecules embedding quantum error correction. These are antiferromagnetically coupled systems with competing exchange interactions, characterized by many low-energy states in which decoherence is dramatically suppressed and does not increase with the system size. This feature allows us to derive optimized code words, enhancing the power of the quantum error correction code by orders of magnitude. We demonstrate this by a complete simulation of the system dynamics, including the effect of decoherence driven by a nuclear spin bath and the full sequence of pulses to implement error correction and logical gates between protected states.