Water Splitting with a Single-Atom Cu/TiO 2 Photocatalyst: Atomistic Origin of High Efficiency and Proposed Enhancement by Spin Selection
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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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Results for “Spin density functionals”
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Kramers nodal lines and Weyl fermions in SmAlSi
Kramers nodal lines (KNLs) have recently been proposed theoretically as a special type of Weyl line degeneracy connecting time-reversal invariant momenta. KNLs are robust to spin orbit coupling and are inherent to all non-centrosymmetric achiral crystal structures, leading to unusual spin, magneto-electric, and optical properties. However, their existence in in real quantum materials has not been experimentally established. Here we gather the experimental evidence pointing at the presence of KNLs in SmAlSi, a non-centrosymmetric metal that develops incommensurate spin density wave order at low temperature. Using angle-resolved photoemission spectroscopy, density functional theory calculations, and magneto-transport methods, we provide evidence suggesting the presence of KNLs, together with observing Weyl fermions under the broken inversion symmetry in the paramagnetic phase of SmAlSi. We discuss the nesting possibilities regarding the emergent magnetic orders in SmAlSi. Our results provide a solid basis of experimental observations for exploring correlated topology in SmAlSi.
36 MATERIALS SCIENCE↗
Infrared-active phonon modes in single-crystal thorium dioxide and uranium dioxide
The infrared-active phonon modes, in single-crystal samples of thorium dioxide (ThO 2 ) and uranium dioxide (UO 2 ), were investigated using spectroscopic ellipsometry and compared with density functional theory. Both ThO 2 and UO 2 are found to have one infrared-active phonon mode pair [consisting of one transverse optic (TO) and one associated longitudinal optic (LO) mode], which is responsible for the dominant features in the ellipsometric data. Furthermore, at room temperature, our results for the mode pair’s resonant frequencies and broadening parameters are comparable with previous reflectance spectroscopy characterizations and density functional theory predictions. For ThO 2 , our ellipsometry and density function theory results both show that the LO mode broadening parameter is larger than the TO mode broadening. This signifies mode anharmonicity, which can be attributed to the intrinsic phonon–phonon interaction. In addition to the main mode pair, a broad low-amplitude impurity-like vibrational mode pair is detected within the reststrahlen band for both ThO 2 and UO 2 . Elevated temperature measurements were performed for ThO 2 in order to study the mechanisms by which the phonon parameters evolve with increased heat. The observed change in the TO resonant frequency is in excellent agreement with previous density functional calculations, which only consider volume expansion of the crystal lattice. This suggests that the temperature-dependent change in the TO frequency is primarily due to volume expansion. The change in the main mode pair’s broadening parameters is nearly linear within the temperature range of this study, which indicates the intrinsic anharmonic scattering (via cubic anharmonicities) as the main decay mechanism.
36 MATERIALS SCIENCE↗
Magnetic frustration driven by conduction carrier blocking in Nd 2 Co 0.85 Si 2.88
The intermetallic compound Nd 2 Co 0.85 Si 2.88 having a triangular lattice could be synthesized in single phase only with defect crystal structure. Investigation through different experimental techniques indicate the presence of two magnetic transitions in the system. As verified experimentally and theoretically, the high-temperature transition $T_H$ ~ 140 K is associated with the development of ferromagnetic interaction between itinerant Co moments, whereas the low-temperature transition at $T_L$ ~ 6.5 K is due to the coupling among Nd–4$\textit{f}$ and Co–3$\textit{d}$ moments, which is antiferromagnetic in nature. Detailed studies of temperature-dependent dc magnetic susceptibility, field dependence of isothermal magnetization, nonequilibrium dynamical behavior, viz., magnetic relaxation, aging effect, magnetic-memory effect, and temperature dependence of heat capacity, along with density functional theory (DFT) calculations, suggest that the ground state is magnetically frustrated spin glass in nature, having competing magnetic interactions of equivalent energies. DFT results further reveal that the 3$\textit{d}$/5$\textit{d}$-conduction carriers are blocked in the system and act as a barrier for the 4$\textit{f}$–4$\textit{f}$ RKKY interactions, resulting in spin frustration. Presence of vacancy defects in the crystal are also conducive to the spin frustration. This is an unique mechanism of magnetic frustration, not emphasized so far in any of the ternary $R_2TX_3$ ($\textit{R}$ = rare earth, $\textit{T}$ = transition elements, and $\textit{X}$ = Si, Ge, In) type compounds. Due to the competing character of the itinerant 3$\textit{d}$ and localized 4$\textit{f}$ moments, the compound exhibits anomalous field dependence of magnetic coercivity. Further, the system also exhibits a considerable magnetic entropy change of –Δ$S_M$ ~ 13.3 J/kg K with a relative cooling power (RCP) of 220 J/kg and adiabatic temperature change $ΔT_{\text{ad}}$ of 6 K for magnetic field change of 70 kOe.
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Anti-PT-symmetric qubit: Decoherence and Entanglement Entropy
Anti-PT symmetry; Comparison with PT-symmetric and Hermitian cases; Density Matrix: Time Dependent Dyson Map; Decoherence Function; von Neumann Entropy; Fisher Information; Spin Vector Representation; Conclusion
97 MATHEMATICS AND COMPUTING↗
Nonorthogonal natural orbitals from open-shell configuration-interaction calculations.
Natural orbitals calculated from spin free one density matrix of open shell limited configuration-interaction wave function constructed from nonorthogonal basis
Heaton, M.↗
Bond Dissociation Energies of the Tungsten Fluorides and Their Singly-Charged Ions: A Density Functional Survey
The dissociation of WF6 and the related singly-charged cations and anions into the lower fluorides and fluorine atoms has been investigated theoretically using density functional theory (B3LYP) and relativistic effective core potentials, with estimates of spin-orbit effects included using a simple model. The inclusion of spin-orbit is essential for a correct description of the thermochemistry. The total atomization energy of the neutral and anionic WF6 is reproduced to within 25 kcal/mol, but comparison of individual bond dissociation energies with available experimental data shows discrepancies of up to 10 kcal/mol. The results are nevertheless useful to help resolve discrepancies in experimental data and provide estimates of missing data.
Dyall, Kenneth G.↗
Magnetism and its coexistence with superconductivity in CaK(Fe 0.949 Ni 0.051 ) 4 As 4 : Muon spin rotation/relaxation studies
Here, the magnetic response of Ca K ( Fe 0.949 Ni 0.051 ) 4 As 4 was investigated by means of the muon spin rotation/relaxation. The long-range commensurate magnetic order sets in below the Néel temperature T N = 50.0 ( 5 ) K. The density-functional theory calculations have identified three possible muon stopping sites. The experimental data were found to be consistent with only one type of magnetic structure, namely, the long-range magnetic spin-vortex-crystal order with the hedgehog motif within the a b plane and the antiferromagnetic stacking along the c direction. The value of the ordered magnetic moment at T ≈ 3 K was estimated to be m Fe = 0.38 ( 11 ) μ B ( μ B is the Bohr magneton). A microscopic coexistence of magnetic and superconducting phases accompanied by a reduction of the magnetic order parameter below the superconducting transition temperature T c ≃ 9 K is observed. Comparison with 11, 122, and 1144 families of Fe-based pnictides points to existence of correlation between the reduction of the magnetic order parameter at T → 0 and the ratio of the transition temperatures T c / T N . Such correlations were found to be described by Machida's model for coexistence of itinerant spin-density-wave magnetism and superconductivity [K. Machida, J. Phys. Soc. Jpn. 50 , 2195 (1981) ; S. L. Bud'ko et al. , Phys. Rev. B 98 , 144520 (2018) ].
36 MATERIALS SCIENCE↗
Strongly correlated itinerant magnetism near superconductivity in NiTa 4 Se 8
Metallic ferromagnets with strongly interacting electrons often exhibit remarkable electronic phases such as ferromagnetic superconductivity, complex spin textures, and nontrivial topology. Here, in this report, we discuss the synthesis of a layered magnetic metal NiTa 4 Se 8 (or Ni 1/4 TaSe 2 ) with a Curie temperature of 58 Kelvin. Magnetization data and density functional theory calculations indicate that the nickel atoms host uniaxial ferromagnetic order of about 0.7µ B per atom, while an even smaller moment is generated in the itinerant tantalum conduction electrons. Strong correlations are evident in flat bands near the Fermi level, a high heat capacity coefficient, and a high Kadowaki-Woods ratio. Density functional theory calculations suggest that electron and hole Fermi surfaces in the ferromagnetic phase are associated with opposite spin polarization. When the system is diluted of magnetic ions, the samples become superconducting below about 2 Kelvin. We discuss possible mechanisms for superconductivity in this family.
30 DIRECT ENERGY CONVERSION↗
Scattering neutrinos, spin models, and permutations
We consider a class of Heisenberg all-to-all coupled spin models inspired by neutrino interactions in a supernova with N degrees of freedom. These models are characterized by a coupling matrix that is relatively simple in the sense that there are only a few, relative to N , nontrivial eigenvalues, in distinction to the classic Heisenberg spin-glass models, leading to distinct behavior in both the high-temperature and low-temperature regimes. When the momenta of the neutrinos are uniform and random in directions, we can calculate the large- N partition function for the quantum Heisenberg model. In particular, the high-temperature partition function predicts a non-Gaussian density of states, providing interesting counterexamples showing the limits of general theorems on the density of states for quantum spin models. We can repeat the same argument for classical Heisenberg models, also known as rotor models, and we find the high-temperature expansion is completely controlled by the eigenvalues of the coupling matrix, and again predicts non-Gaussian behavior for the density of states as long as the number of eigenvalues does not scale linearly with N . Indeed, we derive the amusing fact that these partition functions are essentially the generating function for counting permutations in the high-temperature regime. Finally, for the case relevant to neutrinos in a supernova, we identify the low-temperature phase as a unique state with the direction of the momenta of the neutrino dictating its coherent state in flavor-space, a state we dub the “flavor-momentum-locked” state. Published by the American Physical Society 2025
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
Localization in the SCAN meta-generalized gradient approximation functional leading to broken symmetry ground states for graphene and benzene
Density functional theory calculations play a central role in understanding chemical and solid-state systems. Progress depends on density functionals that accurately reproduce both energies, for thermochemistry, and properly describe ground states and other properties that are of interest. The Cr dimer, benzene and graphene are especially important benchmark systems for quantum chemistry and condensed matter physics. The Strongly Constrained and Appropriately Normed (SCAN) functional, which is an advanced meta-generalized gradient approximation functional that significantly improves molecular energies is shown to perform poorly for the Cr dimer. This is connected with its poor performance for itinerant solid-state magnets and is a consequence of over localization of electrons, thus illustrating an analogy between the Cr dimer and itinerant magnets. The Cr dimer is a notoriously difficult system for density functionals. However, we additionally find that SCAN predicts an incorrect symmetry broken ground state for 2D graphene and for the benzene molecule, which is surprising considering that ground states of these are known to be well described even by the simplest local density approximation. We show that SCAN overly favors localized spin polarized states, which is a serious deficiency of this approach. Thus, the challenge of finding density functionals that accurately treat both localized and delocalized electronic systems remains.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Critical role of magnetic moments in heavy-fermion materials: Revisiting mysteries of SmB 6
Heavy-fermion family exhibits fascinating and often puzzling properties due to the presence of open-shell f ions and the complexity of the associated charge, orbital, and spin degrees of freedom. SmB 6 is a prototypical heavy-fermion compound that is electrically insulating but yet it displays quantum oscillations, which are a telltale signature of the metallic state. Adding to the enigma is the possibility that SmB 6 is a topological Kondo insulator. Here, by treating the spin degree of freedom on an equal footing with other degrees of freedom using the parameter-free strongly-constrained and appropriately-normed (SCAN) density functional, we explore the ground-state electronic structure of SmB6. A number of competing magnetic phases lying very closely in energy are found, indicating the key role of spin fluctuations in the material. The computed band structure, crystal-field splittings in the f-electron complex, the heavy effective electron mass at the Fermi energy, and the large specific heat are all in good agreement with the corresponding experimental results. In particular, our predicted FS explains the experimentally observed bulk quantum oscillations as well as the low electrical conductivity of SmB 6 . The topological Kondo state of SmB6 is shown to be robust regardless of its magnetic configuration. The excellent performance of SCAN in heavy-fermion systems is explained in terms of its ability to treat self-interaction errors and symmetry breaking within the framework of the density functional theory. Our study provides a new approach for modeling heavy-fermion materials
36 MATERIALS SCIENCE↗
Emergent multiferroism with magnetodielectric coupling in EuTiO 3 created by a negative pressure control of strong spin-phonon coupling
Negative pressure has emerged as a powerful tool to tailor the physical properties of functional materials. However, a negative pressure control of spin-phonon coupling for engineering magnetism and multiferroicity has not been explored to date. Here, using uniform three-dimensional strain-induced negative pressure in nanocomposite films of (EuTiO 3 ) 0.5 :(MgO) 0.5 , we demonstrate an emergent multiferroicity with magnetodielectric coupling in EuTiO 3 , matching exactly with density functional theory calculations. Density functional theory calculations are further used to explore the underlying physics of antiferromagnetic-paraelectric to ferromagnetic-ferroelectric phase transitions, the spin-phonon coupling, and its correlation with negative pressures. The observation of magnetodielectric coupling in the EuTiO 3 reveals that an enhanced spin-phonon coupling originates from a negative pressure induced by uniform three-dimensional strain. Our work provides a route to creating multiferroicity and magnetoelectric coupling in single-phase oxides using a negative pressure approach.
36 MATERIALS SCIENCE↗
Long-range current-induced spin accumulation in chiral crystals
Abstract Chiral materials, similarly to human hands, have distinguishable right-handed and left-handed enantiomers which may behave differently in response to external stimuli. Here, we use for the first time an approach based on the density functional theory (DFT)+PAOFLOW calculations to quantitatively estimate the so-called collinear Rashba–Edelstein effect (REE) that generates spin accumulation parallel to charge current and can manifest as chirality-dependent charge-to-spin conversion in chiral crystals. Importantly, we reveal that the spin accumulation induced in the bulk by an electric current is intrinsically protected by the quasi-persistent spin helix arising from the crystal symmetries present in chiral systems with the Weyl spin–orbit coupling. In contrast to conventional REE, spin transport can be preserved over large distances, in agreement with the recent observations for some chiral materials. This allows, for example, the generation of spin currents from spin accumulation, opening novel routes for the design of solid-state spintronics devices.
Roy, Arunesh↗
Optically controlling the competition between spin flips and intersite spin transfer in a Heusler half-metal on sub–100-fs time scales
The direct manipulation of spins via light may provide a path toward ultrafast energy-efficient devices. However, distinguishing the microscopic processes that can occur during ultrafast laser excitation in magnetic alloys is challenging. Here, we study the Heusler compound Co 2 MnGa, a material that exhibits very strong light-induced spin transfers across the entire M-edge. By combining the element specificity of extreme ultraviolet high-harmonic probes with time-dependent density functional theory, we disentangle the competition between three ultrafast light-induced processes that occur in Co 2 MnGa: same-site Co-Co spin transfer, intersite Co-Mn spin transfer, and ultrafast spin flips mediated by spin-orbit coupling. By measuring the dynamic magnetic asymmetry across the entire M-edges of the two magnetic sublattices involved, we uncover the relative dominance of these processes at different probe energy regions and times during the laser pulse. Our combined approach enables a comprehensive microscopic interpretation of laser-induced magnetization dynamics on time scales shorter than 100 femtoseconds.
36 MATERIALS SCIENCE↗
Spin-phonon interaction and short-range order in Mn 3 Si 2 Te 6
The vibrational properties of ferrimagnetic Mn 3 Si 2 Te 6 single crystals are investigated using Raman spectroscopy and density functional theory calculations. Eighteen Raman-active modes are identified, 14 of which are assigned according to the trigonal symmetry. Four additional peaks, obeying the A 1g selection rules, are attributed to the overtones. The unconventional temperature evolution of the A$^{5}_{1g}$ mode self-energy suggests a competition between different short-range magnetic correlations that significantly impact the spin-phonon interaction in Mn 3 Si 2 Te 6 . This research provides comprehensive insight into the lattice properties, studies their temperature dependence, and shows arguments for the existence of competing short-range magnetic phases in Mn 3 Si 2 Te 6 .
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
A Polar Magnetic and Insulating Double Corundum Oxide: Mn2MnSbO6 with Ordered Mn(II) and Mn(III) Ions
A new magnetic insulator Mn2MnSbO6 with a polar crystal structure and an ordered Mn2+ and Mn3+ arrangement was synthesized under a high pressure of 7.5 GPa and 1300 degrees C. The crystal structure of Mn2MnSbO6, investigated by synchrotron powder X-ray diffraction, was found to be isomorphous with that of Ni3TeO6-type, space group R3. The non-centrosymmetric structure was confirmed by the second-harmonic generation measurements. The X-ray absorption near-edge spectroscopy measurement confirmed the nominal oxidation states of Mn22+Mn3+SbO6. Magnetic measurements indicate that Mn2MnSbO6 orders antiferromagnetically below 44 K and undergoes a field-induced spin-flop transition at 5 K. First-principles calculations indicate an antiferromagnetic ground state with up/up/up/down/down/down (uuuddd) spin configuration of the six crystallographically unique Mn ions in the c-axis doubled magnetic structure. The density functional theory calculations also substantiate the experimentally observed charge ordering of the Mn2+/Mn3+ ions and the insulating behavior due to a bandgap of 0.52 eV. To the best of our knowledge, this is the first double corundum oxide containing Jahn-Teller active Mn3+ ions.
Feng, Hai L.↗
Hierarchical excitations from correlated spin tetrahedra on the breathing pyrochlore lattice
The hierarchy of the coupling strengths in a physical system often engenders an effective model at low energies where the decoupled high-energy modes are integrated out. Here, using neutron scattering, we show that the spin excitations in the breathing pyrochlore lattice compound CuInCr 4 S 8 are hierarchical and can be approximated by an effective model of correlated tetrahedra at low energies. At higher energies, intratetrahedron excitations together with strong magnon-phonon couplings are observed, which suggests the possible role of the lattice degree of freedom in stabilizing the spin tetrahedra. Finally, our work illustrates the spin dynamics in CuInCr 4 S 8 and demonstrates a general effective-cluster approach to understand the dynamics on the breathing-type lattices.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗