Inclusion Of Spin-orbit Coupling Research Articles

Topological insulating phase in nonsymmorphic bulk AX2 (A = Ca, Sr, or Ba; and X = As, Sb, or Bi) compounds

Owing to their unique topologically protected gapless boundary states, topological insulators (TIs) are attracting substantial interest in spintronics and quantum computing. Here, we discuss the structural, electronic, and topological properties of bulk alkaline earth di-pnictides AX2 (where A= Ca, Sr, or Ba and X= As, Sb, or Bi) using first-principles calculations under the hybrid functional approach. Our structural analysis based on phonon dispersion and molecular dynamics calculations establishes the thermodynamic stability of these materials and indicates their potential for synthesis. All investigated compounds are shown to host nontrivial phases upon including spin–orbit coupling. CaAs2, SrSb2, and BaSb2 are found to be strong TIs with sizable bandgaps of up to 213 meV. Nontrivial topology in the case of SrSb2 was further confirmed through surface state computations which showed the presence of gapless surface states. In addition, we demonstrate that using the hybrid functional approach can enhance the accuracy of the calculations to predict experimental findings. Finally, our study suggests that the alkaline earth di-pnictide family would provide a promising materials platform for developing applications of TIs.

Beyond the random phase approximation (RPA): First principles calculation of the valence EELS spectrum for KBr including local field, quasiparticle, excitonic and spin orbit coupling effects

The low energy region (< 50 eV) of the electron energy loss spectrum (EELS) can contain a great deal of spectral detail associated with excitations of the valence electrons. Calculation of the spectra from first principles can assist with interpretation and the most widely used method is the random phase approximation (RPA), usually neglecting local field effects (LFE). For KBr this approach is insufficient due to the importance of quasiparticle and excitonic effects. Calculations including these multi-electron effects are shown to give much improved agreement with the experimental spectra, and the inclusion of spin-orbit coupling (SOC) reproduces the excitonic doublet just above band-edge onset. A review of the complex theory behind these methods is given along with practical guidance on performing these calculations.

Exploring the electronic, magnetic and thermoelectric properties of TbPtBi half-Heusler: DFT study

Abstract In this investigation, we employed density functional theory to scrutinize the structural, electronic, magnetic, thermoelectric, and phonon properties of the topological half-Heusler (HH) TbPtBi compound. The stable phonon dispersion spectrum affirms the dynamical stability of the compound. The inclusion of spin-orbit coupling (SOC) significantly influenced the compound’s electronic and thermoelectric properties. The density of state (DOS) confirmed the impact of SOC on the topologically non-trivial metallic behavior of TbPtBi under the equilibrium lattice constant. The SOC altered the DOS at the Fermi level, leading to band splitting and a notable 70% reduction in state density. The Tb-4f electrons in the compound induce total magnetization in AFM (−5.93 µB/cell) and FM (5.94 µB/cell) phases, while SOC eliminates this magnetization. The thermoelectric performance of TbPtBi under compressive and tensile strain has been systematically studied. The result indicate that compressive strain causes a notable increment in Seebeck coefficient and Power factor (20.4 × 1011 W K−2 m−1) of this compound at room temperature. High thermoelectric performance under compressive strain in the HH compound TbPtBi might open new avenues for investigating other topological thermoelectric materials.

Multiple Topological Phases with Electronic Correlation in Intrinsic Ferromagnetic Semimetal VI3 Monolayer.

2D topological materials with magnetic ordering have become hot topics due to their nontrivial band topology and quantum states. In this work, the second-order topological states and evolution of linear band crossing are successfully predicted utilizing the effective k· p and tight binding models in the intrinsic ferromagnetic VI3 monolayer under various effective Hubble interaction Ueff. Upon inclusion of spin orbit coupling, a small bandgap (Eg-1) of 12.7 meV is opened with a Chern invariant C = -1 at Ueff = 0 eV. The Eg-1 undergoes a transition from the non-trivial state to trivial state at Ueff = 0.80 eV, accompanied by the appearance of Dirac cone. Remarkably, the increase of Ueff causes the band inversion and adjustment of crystal symmetry, resulting in two unreported coexistingtopological bandgaps (Eg-2 and Eg-3). Furthermore, a gapless node-loop appears at Ueff = 1.06 eV and disappears at Ueff = 1.09 eV around Γ point. Moreover, for the first time, the existence of second-order topological states with quantized corner fractional charges (e/3) is also observed in the VI3 monolayer at Ueff ≥0.96 eV. These results make the VI3 monolayer a compelling candidate for exploring topological devices.

Ab inito investigation on structural, electronic, and optical characteristics of HfClI Janus monolayer

Utilizing ab initio calculations based on density functional theory, this study delves into the structural, electronic, and optical properties of the HfClI Janus monolayer. Our comprehensive analysis demonstrates the monolayer's dynamical stability, evident from the absence of negative modes in its phonon dispersion spectra. Furthermore, structural analysis reveals no significant bond disruptions or reconstructions, thereby confirming the monolayer's ability to sustain its configuration even at elevated temperatures up to 600 K. In terms of electronic structure, HSE calculations reveal an indirect band gap of 1.359 eV, which undergoes a reduction to 1.281 eV upon inclusion of spin-orbit coupling (SOC). Particularly, the HfClI Janus monolayer exhibit ultrahigh carrier mobilities, ranging from 1257 cm2/sV to 3125 cm2/sV, displaying ultrahigh carrier mobilities. Notably, the monolayer exhibits remarkable absorption capabilities spanning the visible and ultraviolet spectra, hinting at its potential for nano-optoelectronic applications, especially in the realm of electromagnetic radiation absorption and detection. These findings underscore the promising characteristics of the HfClI Janus monolayer, positioning it as a viable candidate for future technological advancements and advancements in nano-optoelectronics.

Endless Dirac nodal lines and high mobility in kagome semimetal Ni3In2Se2 : a theoretical and experimental study

Kagome-lattice crystal is crucial in quantum materials research, exhibiting unique transport properties due to its rich band structure and the presence of nodal lines and rings. Here, we investigate the electronic transport properties and perform first-principles calculations for Ni3In2Se2kagome topological semimetal. First-principles calculations of the band structure without the inclusion of spin-orbit coupling (SOC) shows that three bands are crossing the Fermi level (EF), indicating the semi-metallic nature. With SOC, the band structure reveals a gap opening of the order of 10 meV.Z2index calculations suggest the topologically nontrivial natures (ν0;ν1ν2ν3) = (1;111) both without and with SOC. Our detailed calculations also indicate six endless Dirac nodal lines and two nodal rings with aπ-Berry phase in the absence of SOC. The temperature-dependent resistivity is dominated by two scattering mechanisms:s-dinterband scattering occurs below 50 K, while electron-phonon (e-p) scattering is observed above 50 K. The magnetoresistance (MR) curve aligns with the theory of extended Kohler's rule, suggesting multiple scattering origins and temperature-dependent carrier densities. A maximum MR of 120% at 2 K and 9 T, with a maximum estimated mobility of approximately 3000 cm2V-1s-1are observed. Ni3In2Se2is an electron-hole compensated topological semimetal, as we have carrier density of electron (ne) and hole (nh) arene≈nh, estimated from Hall effect data fitted to a two-band model. Consequently, there is an increase in the mobility of electrons and holes, leading to a higher carrier mobility and a comparatively higher MR. The quantum interference effect leading to the two dimensional (2D) weak antilocalization effect (-σxx∝ln(B)) manifests as the diffusion of nodal line fermions in the 2D poloidal plane and the associated encircling Berry flux of nodal-line fermions.

Mathematical analysis of spin transport in topological insulators to optimize memory devices performance using numerical simulations

Understanding spin transport in topological insulators (TIs) is crucial for the development of spin-based technologies, such as magnetic memory, sensors, and quantum bits. To optimize memory device performance, we developed a comprehensive mathematical model that describes the evolution of spin density, as a function of space and time, taking into account spin-momentum locking, spin-orbit coupling, spin dynamics, and diffusive transport processes (including phonon and impurity scattering). Using numerical simulations (finite element method and Backward Euler Method) implemented in Python, we analyzed the spin transport in TIs. Our study demonstrated a critical dependence of spin transport efficiency on device length, with a maximum efficiency of 75% at a length of 8 micrometers. Beyond a critical length of 10 micrometers, efficiency recovered, reaching 80% at 14 micrometers. We observed oscillatory behavior in spin polarization, with amplitude modulation indicating constructive and destructive interference patterns. The inclusion of spin-orbit coupling and Dirac terms in our model revealed a non-uniform spin polarization distribution, with a 30% increase in polarization near the center. Defects and boundaries significantly impacted spin transport, reducing polarization by 40% near the defect region. Through optimization, we achieved a 25% increase in spin transport efficiency and a 20% enhancement in memory device performance. Our results demonstrate the crucial role of optimizing device length, material quality, and interface engineering in achieving efficient spin transport and improved memory device performance, paving the way for the development of high-performance spin-based technologies.

Relativistic Douglas–Kroll–Hess calculations of hyperfine interactions within first-principles multireference methods

A relativistic magnetic hyperfine interaction Hamiltonian based on the Douglas–Kroll–Hess (DKH) theory up to the second order is implemented within the ab initio multireference methods, including spin–orbit coupling in the Molcas/OpenMolcas package. This implementation is applied to calculate relativistic hyperfine coupling (HFC) parameters for atomic systems and diatomic radicals with valence s or d orbitals by systematically varying active space size in the restricted active space self-consistent field formalism with restricted active space state interaction for spin–orbit coupling. The DKH relativistic treatment of the hyperfine interaction reduces the Fermi contact contribution to the HFC due to the presence of kinetic factors that regularize the singularity of the Dirac delta function in the nonrelativistic Fermi contact operator. This effect is more prominent for heavier nuclei. As the active space size increases, the relativistic correction of the Fermi contact contribution converges well to the experimental data for light and moderately heavy nuclei. The relativistic correction, however, does not significantly affect the spin-dipole contribution to the hyperfine interaction. In addition to the atomic and molecular systems, the implementation is applied to calculate the relativistic HFC parameters for large trivalent and divalent Tb-based single-molecule magnets (SMMs), such as Tb(III)Pc2 and Tb(II)(CpiPr5)2 without ligand truncation using well-converged basis sets. In particular, for the divalent SMM, which has an unpaired valence 6s/5d hybrid orbital, the relativistic treatment of HFC is crucial for a proper description of the Fermi contact contribution. Even with the relativistic hyperfine Hamiltonian, the divalent SMM is shown to exhibit strong tunability of HFC via an external electric field (i.e., strong hyperfine Stark effect).

Ab Initio Calculation of UV-vis Absorption of Parent Mg, Fe, Co, Ni, Cu, and Zn Metalloporphyrins.

Relativistic restricted active space (RAS) second-order multireference perturbation theory (MRPT2) methods, incorporating spin-orbit (SO) coupling perturbatively via state interaction (SO-MRPT2/RASSCF), were used to reproduce the absorption spectra of parent metalloporphyrins containing the Mg2+, Zn2+, Co2+, Ni2+, Cu2+, or FeCl2+ ions in the 12,500-40,000 cm-1 region. Particular attention was paid to the interaction between the porphyrin ring and the metal 3d electrons in states of different multiplicities (we used metal 3d and double d-shell or 3d' orbitals). For this class of compounds, the N-electron valence state perturbation theory (NEVPT2) method is superior to the complete active space perturbation theory (CASPT2) and successfully reproduces the energies of all four characteristic transitions (Q, B, N, and L) of closed-shell metalloporphyrins. Inclusion of SO coupling was found to have very little effect on excitation energies and oscillator strengths. For FeCl2+ porphyrin, we treated ligand-to-metal charge-transfer (LMCT; π,d), metal ligand field (d,d), and metal-to-ligand charge-transfer (MLCT; d,π*) transitions within the same framework. The broad and intense spectral features associated with its B (Soret) band are attributed to multiconfigurational LMCT (d,π*) bands involving strong metal-ligand orbital mixing.

The Study of $${\text{Br}}_{{\text{2}}}^{ + }$$ with Equation-of-Motion Coupled-Cluster Methods Including Spin-Orbit Coupling

The Study of $${\text{Br}}_{{\text{2}}}^{ + }$$ with Equation-of-Motion Coupled-Cluster Methods Including Spin-Orbit Coupling

The electronic structures and optical properties induced by spin-orbit-coupling in LiPbPO4 compound

Phosphate materials are excellent candidates for nonlinear optical materials, thus necessitating a comprehensive and in-depth study of them. Here, inspired by the interesting phenomenon induced by the spin-orbit coupling (SOC) effect, we extend it to LiPbPO4 compounds using a first-principles approach to probe the influence of SOC on the electronic structure and optical properties of post-transition metal compounds. The results show that only the bottom of the conduction band shows an energy level splitting with the inclusion of SOC, which is analyzed to come from the SOC in the Pb 6p state since the SOC in the O 2p state is very weak. The splitting of the conduction band triggers the decrease of the band gap and the change of the optical properties. The performance analysis shows that both the refractive index and the second harmonic generation (SHG) coefficient are enhanced with the inclusion of SOC, however, the change in the birefringence is insignificant, and it is further found that the enhanced SHG coefficient values are closer to the experimental values. In conclusion, our study reveals the impact of SOC effect on the electronic structure and optical properties of LiPbPO4 compounds, contributing to a deeper understanding of the nonlinear optical in post-transition metal compounds.

Investigation of Isolated IrF5 -, IrF6 - Anions and M[IrF6] (M=Na, K, Rb, Cs) Ion Pairs by Matrix-Isolation Spectroscopy and Relativistic Quantum-Chemical Calculations.

The molecular IrF5 -, IrF6 - anions and M[IrF6] (M=Na, K, Rb, Cs) ion pairs were prepared by co-deposition of laser-ablated alkali metal fluorides MF with IrF6 and isolated in solid neon or argon matrices under cryogenic conditions. The free anions were obtained as well by co-deposition of IrF6 with laser-ablated metals (Ir or Pt) as electron sources. The products were characterized in a combined analysis of matrix IR spectroscopy and electronic structure calculations using two-component quasi-relativistic DFT methods accounting for spin-orbit coupling (SOC) effects as well as multi-reference configuration-interaction (MRCI) approaches with SOC. Inclusion of SOC is crucial in the prediction of spectra and properties of IrF6 - and its alkali-metal ion pairs. The observed IR bands and the computations show that the IrF6 - anion adopts an Oh structure in a nondegenerate ground state stabilized by SOC effects, and not a distorted D4h structure in a triplet ground state as suggested by scalar-relativistic calculations. The corresponding "closed-shell" M[IrF6] ion pairs with C3v symmetry are stabilized by coordination of an alkali metal ion to three F atoms, and their structural change in the series from M=Na to Cs was proven spectroscopically. There is no evidence for the formation of IrF7, IrF7 - or M[IrF7] (M=Na, K, Rb, Cs) ion pairs in our experiments.

Critical assessment of G0W0 calculations for 2D materials: the example of monolayer MoS2

Two-dimensional (2D) materials combine many fascinating properties that make them more interesting than their three-dimensional counterparts for a variety of applications. For example, 2D materials exhibit stronger electron-phonon and electron-hole interactions, and their energy gaps and effective carrier masses can be easily tuned. Surprisingly, published band gaps of several 2D materials obtained with the GW approach, the state-of-the-art in electronic-structure calculations, are quite scattered. The details of these calculations, such as the underlying geometry, the starting point, the inclusion of spin-orbit coupling, and the treatment of the Coulomb potential can critically determine how accurate the results are. Taking monolayer MoS2 as a representative material, we employ the linearized augmented planewave + local orbital method to systematically investigate how all these aspects affect the quality of G0W0 calculations, and also provide a summary of literature data. We conclude that the best overall agreement with experiments and coupled-cluster calculations is found for G0W0 results with HSE06 as a starting point including spin-orbit coupling, a truncated Coulomb potential, and an analytical treatment of the singularity at q = 0.

Metal-bonded perovskite lead hydride with phonon-mediated superconductivity exceeding 46 K under ambient pressure

In the search for high-temperature superconductivity in hydrides, a plethora of multi-hydrogen superconductors have been theoretically predicted, and some have been synthesized experimentally under ultrahigh pressures of several hundred GPa. However, the impracticality of these high-pressure methods has been a persistent issue. In response, we propose a new approach to achieve high-temperature superconductivity under ambient pressure by implanting hydrogen into lead to create a stable few-hydrogen binary perovskite, Pb4H. This approach diverges from the popular design methodology of multi-hydrogen covalent high critical temperature (Tc ) superconductors under ultrahigh pressure. By solving the anisotropic Migdal–Eliashberg equations, we demonstrate that perovskite Pb4H presents a phonon-mediated superconductivity exceeding 46 K with inclusion of spin–orbit coupling, which is six times higher than that of bulk Pb (7.22 K) and comparable to that of MgB2, the highest Tc achieved experimentally at ambient pressure under the Bardeen, Cooper, and Schrieffer framework. The high Tc can be attributed to the strong electron–phonon coupling strength of 2.45, which arises from hydrogen implantation in lead that induces several high-frequency optical phonon modes with a relatively large phonon linewidth resulting from H atom vibration. The metallic-bonding in perovskite Pb4H not only improves the structural stability but also guarantees better ductility than the widely investigated multi-hydrogen, iron-based and cuprate superconductors. These results suggest that there is potential for the exploration of new high-temperature superconductors under ambient pressure and may reignite interest in their experimental synthesis in the near future.

Two-dimensional antiferromagnetic nodal-line semimetal and spin Hall effect in MnC4

Nodal-line semimetals, characterized by Dirac-like crossings along one dimensional k-space lines, represent a unique class of topological materials. In this study, we investigate the intriguing properties of room-temperature antiferromagnetic MnC4 and its nodal-line features both with and without spin–orbit coupling (SOC). In the absence of SOC, we identify a doubly degenerate Dirac-nodal line, robustly protected by a combination of time-reversal, mirror, and partial-translation symmetries. Remarkably, this nodal line withstands various external perturbations, including isotropic and anisotropic strain, and torsional deformations, due to the ionic-like bonding between Mn atoms and C clusters. With the inclusion of SOC, we observe a distinctive quasi-Dirac-nodal line that emerges due to the interplay between antiferromagnetism and SOC-induced spin-rotation symmetry breaking. Finally, we observed a robust spin Hall conductivity that aligns with the energy range where the quasi-nodal line appears. This study presents a compelling example of a robust symmetry-protected Dirac-nodal line antiferromagnetic monolayer, which has potential for applications in next-generation spintronic devices.

Study of electronic and transport properties of some topological semimetals XPtBi(X=Gd,Nd,Y) compounds

We have reported the electronic and thermoelectric properties of rare-earth half-Heusler XPtBi(X = Gd,Nd,Y) topological semimetals(TSMs)compounds from the perspective of density functional theory. We have reported that the inclusion of spin orbit coupling (SOC) made more dense bands near fermi level which will be able to tune the electronic bands and well controlled twisting of the spin order which is mostly applicable to spintronic applications. Our results show that the band gap crossing is more near fermi level by the inclusion of SOC. We have reported that LSDA + U has strong effect on unfilled X-f states and hence shifts the bands towards Fermi level. We have found different topological states in these compounds in spin up and spin down states for GdPtBi, NdPtBi and YPtBi. We have further reported the transport properties of these TSMs with and without SOC in terms of figure of merit. Our results confirm that with the inclusion of SOCs in YPtBi power factor get enhanced appreciably for thermoelectric uses.

Size effects on polaron formation in lead chloride perovskite thin films

Lead halide perovskites (LHP) are of interest for light-emitting applications due to the tunability of their bandgap across the visible and near-infrared spectrum (IR) coupled with efficient photoluminescence quantum yields (PLQY). It is widely speculated that photoexcited electrons and holes spatially separate into large negative (electron) and positive (hole) polarons. Polarons are expected to be optically active. With the observed optoelectronic signatures expecting to show potential excited states within the polaronic potential well. From the polaron excited-state we predict that large polarons should be capable of spontaneous emission, photoluminescence, in the mid-IR to far-IR regime based on the concept of inverse occupations within the polaron potential well. Here we use density functional theory (DFT), including spin–orbit coupling interactions, for calculations on a two-dimensional Dion-Jacobson (DJ) lead chloride perovskite atomistic model of various sizes as a host material for either negative or positive polarons to examine the effects of size on polaron formation. This work provides computational evidence that polaron formation through selective charge injection does not show the same level of localisation for positive and negative polarons.

First-principles calculation of electron-phonon coupling in doped KTaO3.

Background: Motivated by the recent experimental discovery of strongly surface-plane-dependent superconductivity at surfaces of KTaO 3 single crystals, we calculate the electron-phonon coupling strength, λ, of doped KTaO 3 along the reciprocal-space high-symmetry directions. Methods:Using the Wannier-function approach implemented in the EPW package, we calculate λ across the experimentally covered doping range and compare its mode-resolved distribution along the [001], [110] and [111] reciprocal-space directions. Results: We find that the electron-phonon coupling is strongest in the optical modes around the Γ point, with some distribution to higher k values in the [001] direction. The electron-phonon coupling strength as a function of doping has a dome-like shape in all three directions and its integrated total is largest in the [001] direction and smallest in the [111] direction, in contrast to the experimentally measured trends in critical temperatures. Conclusions: This disagreement points to a non-BCS character of the superconductivity. Instead, the strong localization of λ in the soft optical modes around Γ suggests an importance of ferroelectric soft-mode fluctuations, which is supported by our findings that the mode-resolved λ values are strongly enhanced in polar structures. The inclusion of spin-orbit coupling has negligible influence on our calculated mode-resolved λ values.

A Comprehensive Study of Electronic, Optical, and Thermoelectric Characteristics of Cs2PbI2Br2 Inorganic Layered Ruddlesden-Popper Mixed Halide Perovskite through Systematic First-Principles Analysis.

In this research, we present a comprehensive study on the influence of layer-dependent structural, electronic, and optical properties in the two-dimensional (2D) Ruddlesden-Popper (RP) perovskite Cs2PbI2Br2. Employing first-principles computations within the density functional theory method, including spin orbit coupling contribution, we examine the impact of various factors on the material. Our results demonstrate that the predicted 2D-layered RP perovskite Cs2PbI2Br2 structures exhibit remarkable stability both structurally and energetically, making them promising candidates for experimental realization. Furthermore, we observe that the electronic band gap and optical absorption coefficients of Cs2PbI2Br2 strongly depend on the thickness variation of the layers. Interestingly, Cs2PbI2Br2 exhibits a notable absorption coefficient in the visible region. Using a combination of density functional theory and Boltzmann transport theory, the thermoelectric properties were forecasted. The calculation involved determining the Seebeck coefficient (S) and other associated thermoelectric characteristics, such as electronic and thermal conductivities, as they vary with the chemical potential at room temperature. These findings open up exciting opportunities for the application of this 2D RP perovskite in solar cells and thermoelectric devices, owing to its unique properties.

Transition probabilities of the AgS(A[formula omitted][formula omitted] X[formula omitted]) emission including spin–orbit coupling effects and evidence of a novel band system

A systematic spectroscopic work using multireference configuration interaction (MRCI) and coupled cluster (CC) calculations was performed in conjunction with large basis sets for AgS. As a result, a more accurate dissociation energy of 17,542 cm−1 is predicted for the X2Π using an analytical potential energy curve, including spin–orbit effects. The calculated energy separation Te(A)∼ 10,500 cm−1 suggests that the AgS(A2Σ+→ X2Π) band system is in near-IR. An unobserved 32Π→ X2Π band system is predicted with Einstein coefficient for spontaneous emission of the orders of 104–105 s−1 in the UV region (342 nm). The radiative lifetimes for the A2Σ+ are of the order of ∼100 microseconds. The AgS(A) state presents a possible predissociation channel caused by interactions with the quartet 14Σ− and 14Π states. The spin–orbit coupling effects are considered in this work by utilizing the Breit–Pauli operator. The present findings are good references for future spectroscopic research concerning heavy-element sulfides.