We show that the quantum geometry of the Fermi surface can be numerically described by a 3-dimensional discrete quantum manifold. This approach not only avoids singularities in the Fermi sea, but it also enables the precise computation of the intrins
ic Hall conductivity resolved in spin, as well as any other local properties of the Fermi surface. The method assures numerical accuracy when the Fermi level is arbitrarily close to singularities, and it remains robust when Kramers degeneracy is protected by symmetry. The approach is demonstrated by calculating the anomalous Hall and spin Hall conductivities of a 2-band lattice model of a Weyl semimetal and a full-band ab-initio model of zincblende GaAs.
Anomalous Hall effect (AHE) is the key transport signature unlocking topological properties of magnetic materials. While AHE is usually proportional to the magnetization, the nonlinearity suggests the existence of complex magnetic and electron orders
. Nonlinear AHE includes the topological Hall effect (THE) that has been widely used to identify the presence of spin chirality in real space. But it can in principle be induced by band structure evolution via Berry curvatures in the reciprocal space. This effect has been largely overlooked due to the intertwined mechanisms in both real and reciprocal spaces. Here, we observed a giant nonlinear AHE with the resistivity up to 383.5 uohm cm, contributing unprecedentedly 97% of the total Hall response in EuCd2As2. Moreover, it can be further enhanced by tilting the magnetic field 30{deg} away from [001] direction, reaching a large anomalous Hall angle up to 21%. Although it shows exactly the same double-peak feature as THE, our scaling analysis and first-principles calculations reveal that the Berry phase is extremely sensitive to the spin canting, and nonlinear AHE is a consequence of band structure evolution under the external magnetic fields. When the spins gradually tilt from the in-plane antiferromagnetic ground state to out-of-plane direction, band crossing and band inversion occur, introducing a bandgap at {Gamma} point at a canting angle of 45{deg}. That contributes to the enhancement of Berry curvature and consequently a large intrinsic Hall conductivity. Our results unequivocally reveal the sensitive dependence of band structures on spin tilting process under external magnetic fields and its pronounced influence on the transport properties, which also need to be taken into consideration in other magnetic materials.
In light of the potential use of single-molecule magnets (SMMs) in emerging quantum information science initiatives, we report first-principles calculations of the magnetic exchange interactions in [$mathrm{Mn}_{3}$]$_{2}$ dimers of $mathrm{Mn}_3$ SM
Ms, connected by covalently-attached organic linkers, that have been synthesized and studied experimentally by magnetochemistry and EPR spectroscopy. Energy evaluations calibrated to experimental results give the sign and order of magnitude of the exchange coupling constant ($J_{12}$) between the two $mathrm{Mn}_{3}$ units that match with fits of magnetic susceptibility data and EPR spectra. Downfolding into the $mathrm{Mn}$ $d$-orbital basis, Wannier function analysis has shown that magnetic interactions can be channeled by ligand groups that are bonded by van der Waals interaction and/or by the linkers via covalent bonding of specific systems, and effective tight-binding Hamiltonians are obtained. We call this long-range coupling that involves a group of atoms a collective exchange. Orbital projected spin density of states and alternative Wannier transformations support this observation. To assess the sensitivity of $J_{12}$ to external pressure, stress-strain curves have been investigated for both hydrostatic and uniaxial pressure, which have revealed a switch of $J_{12}$ from ferromagnetic to antiferromagnetic with increasing pressure.
We use density functional theory to study the structural, magnetic and electronic structure of the organo-metallic quantum magnet $mathrm{NiCl_2-4SC(NH_2)_2}$ (DTN). Recent work has demonstrated the quasi-1D nature of the molecular crystal and its qu
antum phase transitions at low temperatures. This includes a magneto-electric coupling and, when doped with Br, the presence of an exotic Bose-glass state. We systematically show that, by using the generalized gradient approximation (GGA) with inclusion of a van der Waals term to account for weak inter-molecular forces and by introducing a Hubbard $U$ term to the total energy, our calculations reproduce the magnetic anisotropy, the inter-molecular exchange coupling strength and the magneto-electric effect in DTN, which were observed in previous experiments. Further analysis into the electronic structure gives insight into the underlying magnetic interactions, including what mechanisms may be causing the ME effect. Using this computationally efficient model, we predict what effect applying an electric field might have on the magnetic properties of this quantum magnet.
Three high-spin phases recently discovered in the spin-crossover system Mn(taa) are identified through analysis by a combination of first-principles calculations and Monte Carlo simulation as a low-temperature Jahn-Teller ordered (solid) phase, an in
termediate-temperature dynamically correlated (liquid) phase, and an uncorrelated (gas) phase. In particular, the Jahn-Teller liquid phase arises from competition between mixing with low-spin impurities, which drive the disorder, and inter-molecular strain interactions. The latter are a key factor in both the spin-crossover phase transition and the magnetoelectric coupling. Jahn-Teller liquids may exist in other spin-crossover materials and materials that have multiple equivalent Jahn-Teller axes.
Non-trivial topology in a two-dimensional frustrated spin system with the Dzyaloshinskii-Moriya (DM) interaction was investigated by Monto Carlo simulations. At finite temperatures, thermally driven topology was discovered and was found to be dominan
t at low magnetic field. This topological charge has a quadratic relation with the DM interaction and linear realtions with the external magnetic field or the uniaxial magnetic anisotropy. We also proposed a real frustrated system, the Mn-Bi mono-layer film with exceedingly large DM interaction, to enable thermally driven topology. Other topological non-trivial phases in high magnetic field region were also discussed in this real system.
Based on first principles calculations, this study reveals that magnetism in otherwise non-magnetic materials can originate from the partial occupation of antibonding states. Since the antibonding wavefunctions are spatially antisymmetric, the spin w
avefunctions should be symmteric according to the exchange antisymmetric principle of quantum mechanics. We demonstrate that this phenomenon can be observed in a graphitic carbon nitride material, $g$-C$_4$N$_3$, which can be experimentally synthesized and seen as a honeycomb structure with a vacancy. Three dangling bonds of N atoms pointing to the vacancy site interact with each other to form one bonding and two antibonding states. As the two antibonding states are near the Fermi level, and electrons should partially occupy the antibonding states in spin polarization, this leads to 1~$mu_B$ magnetic moment.
Large perpendicular magnetic anisotropy (PMA) in transition metal thin films provides a pathway for enabling the intriguing physics of nanomagnetism and developing broad spintronics applications. After decades of searches for promising materials, the
energy scale of PMA of transition metal thin films, unfortunately, remains only about 1 meV. This limitation has become a major bottleneck in the development of ultradense storage and memory devices. We discovered unprecedented PMA in Fe thin-film growth on the $(000bar{1})$ N-terminated surface of III-V nitrides from first-principles calculations. PMA ranges from 24.1 meV/u.c. in Fe/BN to 53.7 meV/u.c. in Fe/InN. Symmetry-protected degeneracy between $x^2-y^2$ and $xy$ orbitals and its lift by the spin-orbit coupling play a dominant role. As a consequence, PMA in Fe/III-V nitride thin films is dominated by first-order perturbation of the spin-orbit coupling, instead of second-order in conventional transition metal/oxide thin films. This game-changing scenario would also open a new field of magnetism on transition metal/nitride interfaces.
We show that the spin-orbit coupling (SOC) in alpha-MnTe impacts the transport behavior by generating an anisotropic valence-band splitting, resulting in four spin-polarized pockets near Gamma. A minimal k-dot-p model is constructed to capture this s
plitting by group theory analysis, a tight-binding model and ab initio calculations. The model is shown to describe the rotation symmetry of the zero-field planer Hall effect (PHE). The upper limit of the PHE percentage is shown to be fundamentally determined by the band shape, and is quantitatively estimated to be roughly 31% by first principles.
Chiral magnets give rise to the anti-symmetric Dzyaloshinskii-Moriya (DM) interaction, which induces topological nontrivial textures such as magnetic skyrmions. The topology is characterized by integer values of the topological charge. In this work,
we performed the Monte-Carlo calculation of a two-dimensional model of the chiral magnet. A surprising upturn of the topological charge is identified at high fields and high temperatures. This upturn is closely related to thermal fluctuations at the atomic scale, and is explained by a simple physical picture based on triangulation of the lattice. This emergent topology is also explained by a field-theoretic analysis using $CP^{1}$ formalism.
