Spin Exchange Coupling Research Articles

Tomography of entangling two-qubit logic operations in exchange-coupled donor electron spin qubits

Scalable quantum processors require high-fidelity universal quantum logic operations in a manufacturable physical platform. Donors in silicon provide atomic size, excellent quantum coherence and compatibility with standard semiconductor processing, but no entanglement between donor-bound electron spins has been demonstrated to date. Here we present the experimental demonstration and tomography of universal one- and two-qubit gates in a system of two weakly exchange-coupled electrons, bound to single phosphorus donors introduced in silicon by ion implantation. We observe that the exchange interaction has no effect on the qubit coherence. We quantify the fidelity of the quantum operations using gate set tomography (GST), and we use the universal gate set to create entangled Bell states of the electrons spins, with fidelity 91.3 ± 3.0%, and concurrence 0.87 ± 0.05. These results form the necessary basis for scaling up donor-based quantum computers.

Electronic structures, elastic behaviors and magnetic properties of monolayer [formula omitted] and [formula omitted] Ni[formula omitted]I[formula omitted]

This study investigates the electronic structures, elastic behaviors, and magnetic properties of monolayer Ni2I2 in two novel phases, P3̄m1 and P4/nmm, using first-principles calculations and Monte Carlo simulations. The electronic structures of P3̄m1 and P4/nmm phases show half-metallic properties with spin magnetic moments of 0.85 and 0.82 μB respectively. Both phases exhibit mechanical and dynamic stability. The P3̄m1 phase has isotropic elastic properties and good ductility, while the P4/nmm phase shows significant crystallographic anisotropy. The spin exchange coupling constants between the nearest and the next-nearest neighbor Ni ions in the P4/nmm phase are nearly an order of magnitude higher than those in the P3̄m1 phase, with the former having a Curie temperature close to room temperature at 296 K, significantly higher than the 27 K of the latter. The strain modulation range for structural and magnetic phase transitions between the P3̄m1 and P4/nmm phases is provided theoretically.

Nature of electrically detected magnetic resonance in highly nitrogen-doped 6H -SiC single crystals

This work focuses on unraveling electron paramagnetic resonance (EPR) and electrically detected magnetic resonance (EDMR) properties of n-type 6H silicon carbide (SiC) single crystals with high concentrations of uncompensated nitrogen (N) donors, which is essential for fundamental understanding of spin-related phenomena, developing spin-based devices, optimizing materials and devices, and advancing research in quantum information and spintronics. Utilizing low-temperature multifrequency EPR spectroscopy (9.4–395.12 GHz), we identified two intense signals labeled as S line and S1 line in the 6H-SiC crystals with ND–NA≈8×1018 and 4×1019cm−3. In addition, in 6H-SiC crystals with ND–NA≈8×1018cm−3, a low-intensity triplet from N donors substituting the quasicubic “k2” nonequivalent position (Nk2) was observed. The S line [g⊥=2.0029(2),g∥=2.0038(2)] was assigned to the exchange interaction of conduction electrons and Nk2, while the S1 line [g⊥=2.0030(2),g∥=2.0040(2)] is caused by the exchange spin coupling of localized N donors at the “k1” and “k2” positions. The S1 line was observed in high-frequency EDMR spectra of 6H-SiC with ND–NA≈8×1018cm−3, and its emergence was explained by an enhancement of the hopping conductivity due to the EPR-induced temperature increase mechanism. No EDMR spectra were found to occur in the 6H-SiC crystals with ND–NA≈4×1019cm−3, which is close to the critical donor concentration value for a semiconductor-metal transition. Thus it can be concluded that this N donor concentration is too high for the appearance of spin-dependent scattering and too low for the emergence of EPR-induced hopping mechanisms in 6H-SiC. Published by the American Physical Society 2024

Synthesis and annealing effect of structural, morphology, optical, and magnetic properties of tin telluride (SnTe)

This study explored the structural, vibrational, morphological, optical, and magnetic characteristics of both as-grown and annealed single crystals of tin telluride (SnTe), employing diverse analytical techniques. X-ray powder diffraction (XRD) analysis shows the cubic lattice structure of SnTe with consistent lattice parameters across different temperatures, along with the phase transition phenomenon. Fourier Transform Infrared Spectroscopy (FTIR) elucidates temperature-induced shifts in vibrational modes, indicating sensitivity to thermal stimuli. Scanning electron microscopy (SEM) reveals layer-by-layer growth patterns and temperature-dependent variations in crystal morphology. Energy-dispersive X-ray analysis (EDAX) confirms the synthesized crystals' high purity and slight tellurium-rich composition. Optical band gap measurements demonstrate an increase in band gap upon annealing, attributed to valence band convergence. Field-dependent magnetization (M − H) curves exhibit ferromagnetic properties at ambient temperature, which escalate with increasing annealing temperature. Electron Paramagnetic Resonance (EPR) spectra reveal spin mobility and exchange coupling, with variations in the g-factor suggesting the presence of additional spin entropy. These observations offer significant insights into the complex properties of SnTe, which are crucial for its potential applications across various technological fields.

Vanadium embedded in monolayer silicene: Energetics and proximity-induced magnetism

Using the density-functional theory approach, including Hubbard U correction, we investigate the defect structures consisting of vanadium (V) atoms embedded in a monolayer silicene. Specifically, we consider V–V atom pairs in antiferromagnetic (AFM), ferromagnetic (FM), and non-magnetic states, which are embedded in substitutional and interstitial sites. We determine the ground-state structures, formation and binding energies, electronic structures, induced magnetization, as well as the spin-exchange coupling between the V–V pair. For the substitutional vanadium atom pair, the stability of the AFM and FM spin configurations depends on the sublattice sites in which the V atoms are sited. When the V pair is located on a similar sublattice site type, the AFM spin alignment is more energetically favored, whereas when the pair is located in a different sublattice site, the FM interactions are more stable. However, the relative stability of the AFM or FM configurations changes rapidly as the separation between the V pair increases. Regarding the interstitial-hole V–V pair configurations, the most stable structure is when the pair is at the nearest-neighbor hole sites and is in an FM alignment. Also, at larger separations, the AFM or FM hole configurations are approximately degenerate in energy. Furthermore, we elucidate on the Ruderman–Kittel–Kasuya–Yosida, direct-exchange, and the superexchange interaction mechanisms in the vanadium-embedded silicene. In addition, we estimate a Curie temperature (Tc) of up to ∼500 K for a silicene structure containing a V pair in the FM spin alignment. Such a high Tc, in addition to the stability of the material, suggests that vanadium-embedded silicene is a potential candidate material for spintronic device applications.

Programmable order by disorder effect and underlying phases through dipolar quantum simulators

In this work, we study two different quantum simulators composed of molecules with dipole-dipole interaction through various theoretical and numerical tools. Our first result provides knowledge of the quantum order by disorder effect of the S=1/2 system, which is programmable in a quantum simulator composed of circular Rydberg atoms in the triangular optical lattice with a controllable diagonal anisotropy. When the numbers of up spins and down spins are equal, a set of subextensive degenerate ground states is present in the classical limit, composed of continuous strings whose configuration enjoys a large degree of freedom. Among all possible configurations, we focus on the stripe (up and down spins aligning straightly) and kinked (up and down spins forming zigzag spin chains) patterns. Adopting the the real space perturbation theory, we estimate the leading order energy correction when the nearest-neighbor spin exchange coupling, J, is considered, and the overall model becomes an effective XXZ model with a spatial anisotropy. Our calculation demonstrates a lifting of the degeneracy, favoring the stripe configuration. When J becomes larger, we adopt the infinite projected entangled-pair state (iPEPS) and numerically check the effect of degeneracy lifting. The iPEPS results show that even when the spin exchange coupling is strong the stripe pattern is still favored. Next, we study the dipolar bosonic model with tilted polar angle which can be realized through a quantum simulator composed of cold atomic gas with dipole-dipole interaction in an optical lattice. By placing the atoms in a triangular lattice and tilting the polar angle, the diagonal anisotropy can also be realized in the bosonic system. With our cluster mean-field theory calculation, we provide various phase diagrams with different tilted angles, showing the abundant underlying phases including the supersolid. Our proposal indicates realizable scenarios through quantum simulators in studying the quantum effect as well as extraordinary phases. We believe that our results indicated here can also become a good benchmark for two-dimensional quantum simulators. Published by the American Physical Society 2024

Study of the spin effect and exchange coupling of magnetocaloric effect in bilayer systems: a Monte Carlo study

Study of the spin effect and exchange coupling of magnetocaloric effect in bilayer systems: a Monte Carlo study

Deciphering the doublet luminescence mechanism in neutral organic radicals: spin-exchange coupling, reversed-quartet mechanism, excited-state dynamics.

Neutral organic radical molecules have recently attracted considerable attention as promising luminescent and quantum-information materials. However, the presence of a radical often shortens their excited-state lifetime and results in fluorescence quenching due to enhanced intersystem crossing (EISC). Recently, an experimental report introduced an efficient luminescent radical molecule, tris(2,4,6-trichlorophenyl)methyl-carbazole-anthracene (TTM-1Cz-An). In this study, we systematically performed quantum theoretical calculations combined with the path integral approach to quantitatively calculate the excited-state dynamics processes and spectral characteristics. Our theoretical findings suggest that the sing-doublet D1 state, originating from the anthracene excited singlet state, is quickly converted to the doublet (trip-doublet) state via EISC, facilitated by a significant nonequivalence exchange interaction, with ΔJ ST = 0.174 cm-1. The formation of the quartet state (Q1, trip-quartet) was predominantly dependent on the exchange coupling 3/2J TR = 0.086 cm-1 between the triplet spin electrons of anthracene and the TTM-1Cz radical. Direct spin-orbit coupling ISC to the Q1 state was minimal due to the nearly identical spatial wavefunctions of the and Q1 levels. The effective occurrence of reverse intersystem crossing (RISC) from the Q1 to D1 state is a critical step in controlling the luminescence of TTM-1Cz-An. The calculated RISC rate k RISC, including the Herzberg-Teller effect, was 3.64 × 105 s-1 at 298 K, significantly exceeding the phosphorescence and nonradiative rates of the Q1 state, thus enabling the D1 repopulation. Subsequently, a strong electronic coupling of 37.4 meV was observed between the D1 and D2 states, along with a dense manifold of doublet states near the D1 state energy, resulting in a larger reverse internal conversion rate k RIC of 9.26 × 1010 s-1. Distributed to the D2 state, the obtained emission rate of k f = 2.98-3.18 × 107 s-1 was in quite good agreement with the experimental value of 1.28 × 107 s-1, and its temperature effect was not remarkable. Our study not only provides strong support for the experimental findings but also offers valuable insights for the molecular design of high-efficiency radical emitters.

Modulation of the Bonding between Copper and a Redox-Active Ligand by Hydrogen Bonds and Its Effect on Electronic Coupling and Spin States.

The exchange coupling of electron spins can strongly influence the properties of chemical species. The regulation of this type of electronic coupling has been explored within complexes that have multiple metal ions but to a lesser extent in complexes that pair a redox-active ligand with a single metal ion. To bridge this gap, we investigated the interplay among the structural and magnetic properties of mononuclear Cu complexes and exchange coupling between a Cu center and a redox-active ligand over three oxidation states. The computational analysis of the structural properties established a relationship between the complexes' magnetic properties and a bonding interaction involving a dx2-y2 orbital of the Cu ion and π orbital of the redox-active ligand that are close in energy. The additional bonding interaction affects the geometry around the Cu center and was found to be influenced by intramolecular H-bonds introduced by the external ligands. The ability to synthetically tune the d-π interactions using H-bonds illustrates a new type of control over the structural and magnetic properties of metal complexes.

Systematic determination of coupling constants in spin clusters from broken-symmetry mean-field solutions.

Quantum-chemical calculations aimed at deriving magnetic coupling constants in exchange-coupled spin clusters commonly utilize a broken-symmetry (BS) approach. This involves calculating several distinct collinear spin configurations, predominantly by density-functional theory. The energies of these configurations are interpreted in terms of the Heisenberg model, H̃=∑i<jJijs̃i⋅s̃j, to determine coupling constants Jij for spin pairs. However, this energy-based procedure has inherent limitations, primarily in its inability to provide information on isotropic spin interactions beyond those included in the Heisenberg model. Biquadratic exchange or multi-center terms, for example, are usually inaccessible and hence assumed to be negligible. The present work introduces a novel approach employing BS mean-field solutions, specifically Hartree-Fock wave functions, for the construction of effective spin Hamiltonians. This expanded method facilitates the extraction of a broader range of coupling parameters by considering not only the energies, but also Hamiltonian and overlap elements between different BS states. We demonstrate how comprehensive s=12 Hamiltonians, including multi-center terms, can be straightforwardly constructed from a complete set of BS solutions. The approach is exemplified for small clusters within the context of the half-filled single-band Hubbard model. This allows to contrast the current strategy against exact results, thereby offering an enriched understanding of the spin-Hamiltonian construction from BS solutions.

Magnetization Process in Bilayer Honeycomb Spin Lattice

The magnetization process of the AA-stacked bilayer honeycomb spin lattice in the out-of-plane applied field is examined in the framework of the Ising model and mean field approximation. Competition between different kinds (antiferromagnetic: AF, or ferromagnetic: FM) of intra-layer and inter-layer spin exchange couplings could lead to the first order magnetization process, characterized by sharp jumps in magnetization curves occurring in critical external fields (spin-flop and spin- flip fields). There is only the spin-flip field at very low temperature and its magnitude depends not only on the intra-layer frustration level but also exchange coupling between spin layers. During the magnetization process, the initial AF bilayer honeycomb spin lattice may undergo ferrimagnetic or week-ferromagnetic states before reaching full ferromagnetic saturation state by the spin-flip field. The results of this work can be applied for an explanation of the spin-flip phenomenon registered in the AF bilayer CrI3.

Crystal Structure and Ferromagnetism of the CeFe9Si4Intermetallic Compound

We have determined the crystal structure and the magnetic state of the CeFe9Si4 intermetallic compound. Our revised structural model (fully ordered tetragonal unit cell, I4/mcm) agrees with the previous literature report, except for some minor quantitative differences. Magnetically, the CeFe9Si4 undergoes a ferromagnetic transition at the temperature TC ≈ 94 K. Ferromagnetism in the combined Ce-Fe spin system is a result of interplay between the localized magnetism of the Ce sublattice and the Fe band (itinerant) magnetism. Ferromagnetic ordering obeys the rather general rule that the exchange spin coupling between atoms possessing more than half-full d shells with atoms possessing less than half-full d shells is antiferromagnetic (where the Ce atoms are considered as light d elements). Since in rare-earth metals from the light half of the lanthanide series, the magnetic moment is directed opposite to the spin, this results in ferromagnetism. The magnetoresistance and the magnetic specific heat show an additional temperature-dependent feature (a shoulder) deep inside the ferromagnetic phase that is considered to originate from the influence of the magnetization on the electronic band structure via the magnetoelastic coupling, which alters the Fe band magnetism below TC. The ferromagnetic phase of CeFe9Si4 is magnetically soft.

Non-Hermitian dynamics for a two-spin system with PT symmetry

A system of interacting spins that are under the influence of spin-polarized currents can be described using a complex functional, or a non-Hermitian (NH) Hamiltonian. We study the dynamics of two exchange-coupled spins on the Bloch sphere. In the case of currents leading to PT symmetry, an exceptional point that survives also in the nonlinear system is identified. The nonlinear system is bistable for small currents and it exhibits stable oscillating motion or it can relax to a fixed point. The oscillating motion of the two spins is akin to synchronized spin-torque oscillators. For the full nonlinear system, we derive two conserved quantities that furnish a geometric description of the spin trajectories in phase space and indicate stability of the oscillating motion. Our analytical results provide tools for the description of the dynamics of NH systems that are defined on the Bloch sphere.

Quantum spin liquid in an RKKY-coupled two-impurity Kondo system

We consider a 2-impurity Kondo system with spin-exchange coupling within the conduction band. Our numerical renormalization group calculations show that for strong intraband spin correlations the competition of these correlations with Kondo spin screening stabilizes a metallic spin-liquid phase of the localized spins without geometric frustration. For weak Kondo coupling the spin liquid and the Kondo singlet phase are separated by two quantum phase transitions and an intermediate RKKY spin-dimer phase, while beyond a critical coupling they are connected by a crossover. The results suggest how a quantum spin liquid may be realized in heavy-fermion systems near a spin-density wave instability.

The Influence of Annealing and Film Thickness on the Specific Properties of Co40Fe40Y20 Films

Cobalt Iron Yttrium (CoFeY) magnetic film was made using the sputtering technique in order to investigate the connection between the thickness and annealing procedures. The sample was amorphous as a result of an insufficient thermal driving force according to X-ray diffraction (XRD) examination. The maximum low-frequency alternate-current magnetic susceptibility (χac) values were raised in correlation with the increased thickness and annealing temperatures because the thickness effect and Y addition improved the spin exchange coupling. The best value for a 50 nm film at annealing 300 °C for χac was 0.20. Because electron carriers are less constrained in their conduction at thick film thickness and higher annealing temperatures, the electric resistivity and sheet resistance are lower. At a thickness of 40 nm, the film's maximum surface energy during annealing at 300 °C was 28.7 mJ/mm2. This study demonstrated the passage of photon signals through the film due to the thickness effect, which reduced transmittance. The best condition was found to be 50 nm with annealing at 300 °C in this investigation due to high χac, strong adhesion, and low resistivity, which can be used in magnetic fields.

Spin and spin current—From fundamentals to recent progress

Along with the progress of spin science and spintronics research, the flow of electron spins, i.e., spin current, has attracted interest. New phenomena and electronic states were explained in succession using the concept of spin current. Moreover, as many of the conventionally known spintronics phenomena became well organized based on spin current, it has rapidly been recognized as an essential concept in a wide range of condensed matter physics. In this article, we focus on recent developments in the physics of spin, spin current, and their related phenomena, where the conversion between spin angular momentum and different forms of angular momentum plays an essential role. Starting with an introduction to spin current, we first discuss the recent progress in spintronic phenomena driven by spin-exchange coupling: spin pumping, topological Hall torque, and emergent inductor. We, then, extend our discussion to the interaction/interconversion of spins with heat, lattice vibrations, and charge current and address recent progress and perspectives on the spin Seebeck and Peltier effects. Next, we review the interaction between mechanical motion and electron/nuclear spins and argue the difference between the Barnett field and rotational Doppler effect. We show that the Barnett effect reveals the angular momentum compensation temperature, at which the net angular momentum is quenched in ferrimagnets.

Co40Fe40Y20 Nanofilms’ Structural, Magnetic, Electrical, and Nanomechanical Characteristics as a Function of Annealing Temperature and Thickness

To investigate the correlations between different thicknesses and heat treatments, this study used a sputtering method to create CoFeY films. The results of X-ray diffraction (XRD) revealed the appearance of oxide peaks at 2θ = 47.7°, 54.5°, and 56.3° in agreement with YFeO3 (212), Co2O3 (422), and Co2O3 (511), respectively. The findings also demonstrated a relationship between the low-frequency alternative-current magnetic susceptibility (χac) values and the thickness of the CoFeY thin films. At a thickness of 50 nm and an annealing temperature of 300 °C, the ideal value of ac was 0.159. The presence of Y and the thickness impact were both evident in the χac value, which improved spin-exchange coupling as well as grain refining. With increasing thickness, the resistance decreased. At 300 °C and 40 nm in thickness, this film has a maximum surface energy of 31.2 mJ/mm2. The hardness of the 50-nm films reached a maximum of 16.67 GPa when annealed at 100 °C. Due to the high χac, strong adhesion, good nanomechanical properties, and low resistivity, the optimal conditions were determined to be 50 nm with annealing at 300 °C.

The effect of hetero-atoms on spin exchange coupling pathways (ECPs): a computational investigation.

The effect of heteroatoms on exchange coupling pathways and the presence of more than one coupling paths are investigated. The lone pairs of sp2-hybridized heteroatoms contribute to aromaticity but do not play any pivotal role in the spin coupling between two spin centers. A conceptual model to describe this behavior of heteroatoms has been introduced, and we name it as the hetero-atom blocking effect. With the occurrence of two π-orbital exchange coupling pathways (ECPs) via bridgehead heteroatoms (B-, N-, O-, or S-), the magnetic exchange coupling constants (J) can be viewed as a signed sum of different individual pathways. The effect of σ-electron coupling is also investigated in this work.

High-field EPR of copper(II)-nitroxide compound exhibiting three-step phase transition: structural insights from the field-induced sample orientation.

Copper(II)-nitroxide based Cu(hfac)2LR compounds exhibit unusual magnetic behavior that can be induced by various stimuli. In many aspects, the magnetic phenomena observed in Cu(hfac)2LR are similar to classical spin-crossover behavior. However, these phenomena originate from polynuclear exchange-coupled spin clusters Cu2+-O˙-N< or >N-˙O-Cu2+-O˙-N<. Such peculiarities may result in additional multifunctionality of Cu(hfac)2LR compounds, making them promising materials for spintronic applications. Herein, we investigate the Cu(hfac)2LMeMe material, which demonstrates a three-step temperature-induced magnetostructural transition between high-temperature, low-temperature, and intermediate states, as revealed by magnetometry. Two main steps were resolved using variable-temperature Fourier-transform infrared and Q-band electron paramagnetic resonance (EPR) spectroscopies. The intermediate-temperature states (∼40-90 K) are characterized by the coexistence of two types of copper(II)-nitroxide clusters, corresponding to the low-temperature and high-temperature phases. High-field EPR experiments revealed the effect of partial alignment of Cu(hfac)2LMeMe microcrystals in a strong (>20 T) magnetic field. This effect was used to unveil the structural features of the low-temperature phase of Cu(hfac)2LMeMe, which were inaccessible using single-crystal X-ray diffraction (XRD) technique. In particular, high-field EPR allowed us to determine the relative direction of the Jahn-Teller axes in CuO6 and CuO4N2 units.

Long-Range Magnetic Order in Nickel Hydroxide-Functionalized Graphene Quantum Dots.

In this work, we demonstrate the prospect of chemically synthesizing transition metal (Ni) doped magnetic graphene quantum dots (GQDs) with the sole aim of shedding light on their magnetic properties. Our results show that adsorption of nickel hydroxide on predominantly paramagnetic GQDs reveals antiferromagnetic ordering in the M-T profile around 10 K with change of the spin exchange coupling deviating from J = 1/2 to J = 1, mainly arising from the d-p mixing hybridization between the p orbital of carbon from the GQD and the d orbital of Ni. Furthermore, our results are well complemented by ab initio simulations showing asymmetry of the up and down spins around the Fermi level for nickel hydroxide-doped GQDs with long-range spin polarization. Furthermore, the magnitude of the net magnetic moment generated for doped GQDs on the carbon atoms is found to be site-dependent (surface or edge).