The competition between kinematic, relativistic, and Coulomb interactions has spurred intense experimental and theoretical investigations in iridium-based oxides. Their electronic structure is mostly understood in terms of the spin-orbital coupled effective J state (Jeff). However, the role of the Ir charge state in shaping the strength of effective spin-orbit coupling and defining the stability of the Jeff ground state has not been thoroughly explored. We argue here that the iridium-ruthenium triple perovskites, Ba3MRuIrO9 (M=Li, Mg, and In), are of particular interest in this regard. Using ab initio theory, we show here that the nominal charge states of Ir can be tuned from +6 (5d3) to +4 (5d5) by choosing nonmagnetic M ions as Li(+1), Mg(+2), and In(+3), while the Ru ions always remain in nominal +5 (4d3) charge state. This variation modulates the influence of the spin-orbit coupling (SOC), which is found to be negligible in Ba3LiRuIrO9, moderate in Ba3MgRuIrO9, and determining in Ba3InRuIrO9. Our analysis classifies Ba3LiRuIrO9 as a correlation-driven insulator arising from Hubbard interactions and exchange-split t2g states, Ba3MgRuIrO9 as a SOC and correlation-driven insulator that does not conform to the commonly expected J=0 ground state and Ba3InRuIrO9 as Jeff=1/2 Mott-Hubbard insulator. In the data reported here, the correlational electronic structure theory results in sizable magnetic moments of both Ru and Ir atoms in these systems and atomistic spin-dynamics simulations capture the experimental Néel temperature for Ba3LiRuIrO9 and Ba3MgRuIrO9 and provide evidence for a phase transition for Ba3InRuIrO9 when T → 0 K, to a multivalley magnetic state with strong magnetic frustration. The theory identifies that strong SOC in Ba3InRuIrO9 induces bond-dependent magnetic couplings with significant Dzyaloshinskii-Moriya interaction, strong symmetric anisotropic exchange, and finite in-plane single-ion anisotropy. The realization of such strong anisotropic interactions helps to stabilize a particularly complex energy landscape of Ba3InRuIrO9, which opens up for exotic magnetic quantum phases such as quantum spin liquid. Thus, by comparing the electronic structure and magnetism of isostructural iridates with different Ir-charge states, we provided a theoretical framework to demonstrate the structural and electronic conditions that drive the deviations from conventional magnetic ordering, facilitating the emergence of exotic quantum phases.

This study presents a 3D version of multiscale approach for investigating magnetization dynamics in multiscale, hybrid micromagnetic-atomistic simulations. The present work introduces engineered discontinuities (i) a double-slit structure, which enables the study of domain wall and spin wave interference, and (ii) a tetrahedron shaped cluster of atoms with tunable anisotropy, which provides insights into how localized anisotropic perturbations influence domain wall pinning and skyrmion stability in fully three-dimensional (3D) hybrid simulations. We considered the dynamics of spin waves, domain walls, as well as 3D skyrmions, in the presence of these defects. The magnonic double-slit experiment demonstrates interference patterns analogous to electronic wave phenomena, offering potential applications in wave-based computing. Additionally, the results reveal the impact of the local anisotropy that leads to distinct transformations, including domain wall deformations, tubular and spherical structures, skyrmion annihilation, and breathing mode. The findings underscore the critical role of defect-induced anisotropic interactions in controlling domain wall motion, skyrmion topology, and spin wave propagation.

PdFe/Ir(111) has attracted tremendous attention for next-generation spintronics devices due to existence of magnetic skyrmions with the external magnetic field. Our density functional theoretical calculations in combination with spin dynamics simulation suggest that the spin spiral phase in fcc stacked PdFe/Ir(111) flips into the skyrmion lattice phase around B-ert similar to 6 T. This leads to the microscopic understanding of the thermodynamic and kinetic behaviours affected by the intrinsic spin-lattice couplings (SLCs) in this skyrmion material for magneto-mechanical properties. Here we calculate fully relativistic SLC parameters from first principle computations and investigate the effect of SLC on dynamical magnetic interactions in skyrmion multilayers PdFe/Ir(111). The exchange interactions arising from next nearest-neighbors (NN) in this material are highly frustrated and responsible for enhancing skyrmion stability. We report the larger spin-lattice effect on both dynamical Heisenberg exchanges and Dzyaloshinskii-Moriya interactions for next NN compared to NN which is in contrast with recently observed spin-lattice effect in bulk bcc Fe and CrI3 monolayer. Based on our analysis, we find that the effective measures of SLCs in fcc (hcp) stacking of PdFe/Ir(111) are similar to 2.71(similar to 2.36) and similar to 14.71(similar to 21.89) times stronger for NN and next NN respectively, compared to bcc Fe. The linear regime of displacement for SLC parameters is <= 0.02 angstrom which is 0.72% of the lattice constant for PdFe/Ir(111). The microscopic understanding of SLCs provided by our current study could help in designing spintronic devices based on thermodynamic properties of skyrmion multilayers.

The V-based kagome systems AV3Sb5 (A=Cs, Rb, and K) are unique by virtue of the intricate interplay of nontrivial electronic structure, topology, and intriguing fermiology, rendering them to be a playground of many mutually dependent exotic phases like charge-order and superconductivity. Despite numerous recent studies, the interconnection of magnetism and other complex collective phenomena in these systems has yet not arrived at any conclusion. Using first-principles tools, we demonstrate that their electronic structures, complex fermiologies and phonon dispersions are strongly influenced by the interplay of dynamic electron correlations, nontrivial spin-polarization and spin-orbit coupling. An investigation of the first-principles-derived intersite magnetic exchanges with the complementary analysis of q dependence of the electronic response functions and the electron-phonon coupling indicate that the system conforms as a frustrated spin cluster, where the occurrence of the charge-order phase is intimately related to the mechanism of electron-phonon coupling, rather than the Fermi-surface nesting.

We have investigated the dynamical magnetic properties of the V-based kagome stibnite compounds by combining the ab initio-extracted magnetic parameters of a spin-Hamiltonian, like inter-site exchange parameters, magnetocrystalline anisotropy and site projected magnetic moments, with full-fledged simulations of atomistic spin- dynamics. Our calculations reveal that, in addition to a ferromagnetic order along the [001] direction, the system hosts a complex landscape of magnetic configurations comprised of commensurate and incommensurate spin spirals along the [010] direction. The presence of such chiral magnetic textures may be the key toward solving the mystery about the origin of the experimentally observed inherent breaking of the C6 rotational, mirror, and the time-reversal symmetry.

This paper reports the first experimental observation of phonons and their softening on single crystalline LaPt2Si2 via inelastic neutron scattering. From the temperature dependence of the phonon frequency in close proximity to the charge density wave (CDW) q-vector, we obtain a CDW transition temperature of TCDW = 230 K and a critical exponent β = 0.28 ± 0.03. This value is suggestive of a non-conventional critical behavior for the CDW phase transition in LaPt2Si2, compatible with a scenario of CDW discommensuration (DC). The DC would be caused by the existence of two CDWs in this material, propagating separately in the non equivalent (Si1–Pt2–Si1) and (Pt1–Si2–Pt1) layers, respectively, with transition temperatures TCDW−1 = 230 K and TCDW−2 = 110 K. A strong q-dependence of the electron-phonon coupling has been identified as the driving mechanism for the CDW transition at TCDW−1 = 230 K while a CDW with 3-dimensional character, and Fermi surface quasi-nesting as a driving mechanism, is suggested for the transition at TCDW−2 = 110 K. Our results clarify some aspects of the CDW transition in LaPt2Si2 which have been so far misinterpreted by both theoretical predictions and experimental observations and give direct insight into its actual temperature dependence.

X-ray absorption and resonant inelastic x-ray scattering spectra of LaPt₂Si₂ single crystal at the Si 2p and La 4d edges are presented. The data are interpreted in terms of density functional theory, showing that the Si spectra can be described in terms of Si s and d local partial density of states (LPDOS), and the La spectra are due to quasi-atomic local 4f excitations. Calculations show that Pt d-LPDOS dominates the occupied states, and a sharp localized La f state is found in the unoccupied states, in line with the observations.

Since thermal fluctuations become more important as dimensions shrink, it is expected that low-dimensional magnets are more sensitive to atomic displacement and phonons than bulk systems are. Here we present a fully relativistic first-principles study on the spin-lattice coupling, i.e., how the magnetic interactions depend on atomic displacement, of the prototypical two-dimensional ferromagnet CrI3. We extract an effective measure of the spin-lattice coupling in CrI3, which is up to ten times larger than what is found for bcc Fe. The magnetic exchange interactions, including Heisenberg and relativistic Dzyaloshinskii-Moriya interactions, are sensitive both to the in-plane motion of Cr atoms and out-of-plane motion of ligand atoms. We find that significant magnetic pair interactions change sign from ferromagnetic (FM) to antiferromagnetic (AFM) for atomic displacements larger than 0.16 (0.18) angstrom for Cr (I) atoms. We explain the observed strong spin-lattice coupling by analyzing the orbital decomposition of isotropic exchange interactions, involving different crystal-field-split Cr-3d orbitals. The competition between the AFM t(2g)-t(2g) and FM t(2g)-e(g) contributions depends on the bond angle formed by Cr and I atoms as well as Cr-Cr distance. In particular, if a Cr atom is displaced, the FM-AFM sign changes when the I-Cr-I bond angle approaches 90 degrees. The obtained spin-lattice coupling constants, along with the microscopic orbital analysis, can act as a guiding principle for further studies of the thermodynamic properties and combined magnon-phonon excitations in two-dimensional magnets.

Persistent homology (PH) is a relatively new field in applied mathematics that studies the components and shapes of discrete data. In this paper, we demonstrate that PH can be used as a universal framework to identify phases of classical spins on a lattice. This demonstration includes hidden order such as spin-nematic ordering and spin liquids. By converting a small number of spin configurations to barcodes we obtain a descriptive picture of configuration space. Using dimensionality reduction to reduce the barcode space to color space leads to a visualization of the phase diagram.

The Organic Materials Database (OMDB) is an open database hosting about 22 000 electronic band structures, density of states, and other properties for stable and previously synthesized three-dimensional organic crystals. The web interface of the OMDB offers various search tools for the identification of novel functional materials such as band structure pattern matching and density of states similarity search. In this work, the OMDB is extended to include magnetic excitation properties. For inelastic neutron scattering, we focus on the dynamic structure factor S(q, omega) which contains information on the excitation modes of the material. We introduce a new dataset containing atomic magnetic moments and Heisenberg exchange parameters for which we calculate the spin wave spectra and dynamic structure factor with linear spin wave theory and atomistic spin dynamics. We thus develop the materials informatics tools to identify novel functional organic and metalorganic magnets.