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Shubhajyoti Mohapatra

Publications and source records attributed to Shubhajyoti Mohapatra.

17 recordsLinked to original sources

Spin-orbital order and excitations in $3d^4$, $4d^4$, and $5d^4$ systems: Application to $\rm BaFeO_3$, $\rm Sr_2RuO_4$, $\rm Sr_2YIrO_6$, and $\rm K_2OsCl_64$

Evolution of composite spin-orbital order and coupled spin-orbital excitations is studied in a variety of $d^4$ systems with $n$=$4$ electrons in the $t_{2g}$ orbital sector using the generalised self-consistent + fluctuations approach for a realistic interacting-electron model. Within this unified approach, applications are discussed to compounds with $3d$, $4d$, $5d$ transition-metal ions such as $\rm BaFeO_3$ ($\rm Fe^{4+}$), $\rm Ca_2RuO_4$ ($\rm Ru^{4+}$), $\rm Sr_2RuO_4$ ($\rm Ru^{4+}$), $\rm Sr_2YIrO_6$ ($\rm Ir^{5+}$), and $\rm K_2OsCl_6$ ($\rm Os^{4+}$). Continuous interpolation from the nominally $S=1$ antiferromagnetic order in $\rm Ca_2RuO_4$ (strong crystal field, intermediate spin-orbit coupling (SOC) and Coulomb interaction) to the $J=0$ state relevant for $5d^4$ compounds (strong SOC, weak Coulomb interaction) and to the half-metallic ferromagnetic order when crystal field is negligible as in $\rm BaFeO_3$ (weak SOC, strong Coulomb interaction) and $\rm Sr_2RuO_4$ (intermediate SOC and Coulomb interaction) provides new fundamental insights into the magnetism of spin-orbit coupled systems.

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Spin-orbit coupling and magnetism in $\rm Sr_2CrO_4$

With octahedrally coordinated $t_{\rm 2g}$ orbitals which are active at filling $n=2$, the $\rm Sr_2CrO_4$ compound exhibits rich interplay of spin-orbital physics with tetragonal distortion induced crystal field tuning by external agent such as pressure. Considering both reversed and restored crystal field regimes, collective spin-orbital excitations are investigated in the antiferromagnetic state using the generalized self consistent + fluctuations approach including spin-orbit coupling (SOC). A transition is found from staggered to entangled orbital order at critical SOC value in the realistic regime. Behavior of the calculated energy scales of collective excitations with crystal field is in striking similarity to that of the transition temperatures with pressure as obtained from susceptibility and resistivity anomalies in high-pressure studies.

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Orbital entangled antiferromagnetoc order and spin-orbit-distortion exciton in $\rm Sr_2VO_4$

With electron filling $n=1$ in the $\rm Sr_2VO_4$ compound, the octahedrally coordinated $t_{\rm 2g}$ orbitals are strongly active due to tetragonal distortion induced crystal field tuning by external agent such as pressure. Considering the full range of crystal field induced tetragonal splitting in a realistic three-orbital model, collective spin-orbital excitations are investigated using the generalized self consistent and fluctuation approach. The variety of self consistent states obtained including orbital entangled ferromagnetic and antiferromagnetic orders reflects the rich spin-orbital physics resulting from the interplay between the band, spin-orbit coupling, crystal field, and Coulomb interaction terms. The behavior of the calculated energy scales of collective excitations with crystal field is consistent with that of the transition temperatures with pressure as obtained from susceptibility and resistivity anomalies in high-pressure studies.

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Coupled spin-orbital fluctuations in a three orbital model for $4d$ and $5d$ oxides with electron fillings $n=3,4,5$ -- Application to $\rm NaOsO_3$, $\rm Ca_2RuO_4$, and $\rm Sr_2IrO_4$

A unified approach is presented for investigating coupled spin-orbital fluctuations within a realistic three-orbital model for strongly spin-orbit coupled systems with electron fillings $n=3,4,5$ in the $t_{2g}$ sector of $d_{yz},d_{xz},d_{xy}$ orbitals. A generalized fluctuation propagator is constructed which is consistent with the generalized self-consistent Hartree-Fock approximation where all Coulomb interaction contributions involving orbital diagonal and off-diagonal spin and charge condensates are included. Besides the low-energy magnon, intermediate-energy orbiton and spin-orbiton, and high-energy spin-orbit exciton modes, the generalized spectral function also shows other high-energy excitations such as the Hund's coupling induced gapped magnon modes. We relate the characteristic features of the coupled spin-orbital excitations to the complex magnetic behavior resulting from the interplay between electronic bands, spin-orbit coupling, Coulomb interactions, and structural distortion effects, as realized in the compounds $\rm NaOsO_3$, $\rm Ca_2RuO_4$, and $\rm Sr_2IrO_4$.

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Pseudo-spin rotation symmetry breaking by Coulomb interaction terms in spin-orbit coupled systems

By transforming from the pure-spin-orbital ($t_{\rm 2g}$) basis to the spin-orbital entangled pseudo-spin-orbital basis, the pseudo-spin rotation symmetry of the different Coulomb interaction terms is investigated under SU(2) transformation in pseudo-spin space. While the Hubbard and density interaction terms are invariant, the Hund's coupling and pair-hopping interaction terms explicitly break pseudo-spin rotation symmetry systematically. The form of the symmetry-breaking terms obtained from the transformation of the Coulomb interaction terms accounts for the easy $x$-$y$ plane anisotropy and magnon gap for the out-of-plane mode, highlighting the importance of mixing with the nominally non-magnetic $J$=3/2 sector, and providing a physically transparent approach for investigating magnetic ordering and anisotropy effects in perovskite ($\rm Sr_2 Ir O_4$) and other $d^5$ pseudo-spin compounds.

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Magnetic reorientation transition in a three orbital model for $\rm Ca_2 Ru O_4$ -- Interplay of spin-orbit coupling, tetragonal distortion, and Coulomb interactions

Including the orbital off-diagonal spin and charge condensates in the self consistent determination of magnetic order within a realistic three-orbital model for the $4d^4$ compound $\rm Ca_2 Ru O_4$, reveals a host of novel features including strong and anisotropic spin-orbit coupling (SOC) renormalization, coupling of strong orbital magnetic moments to orbital fields, and a magnetic reorientation transition. Highlighting the rich interplay between orbital geometry and overlap, spin-orbit coupling, Coulomb interactions, tetragonal distortion, and staggered octahedral tilting and rotation, our investigation yields a planar antiferromagnetic (AFM) order for moderate tetragonal distortion, with easy $a-b$ plane and easy $b$ axis anisotropies, along with small canting of the dominantly $yz,xz$ orbital moments. With decreasing tetragonal distortion, we find a magnetic reorientation transition from the dominantly planar AFM order to a dominantly $c$ axis ferromagnetic (FM) order with significant $xy$ orbital moment.

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Role of orbital off-diagonal spin and charge condensates in a three orbital model for $\rm Ca_2RuO_4$ -- Coulomb renormalized spin-orbit coupling, orbital moment, and tunable magnetic order

Strongly anisotropic spin-orbit coupling (SOC) renormalization and strongly enhanced orbital magnetic moments are obtained in the fully self consistent approach including the orbital off-diagonal spin and charge condensates. For moderate tetragonal distortion as in $\rm Ca_2 RuO_4$, dominantly planar antiferromagnetic (AFM) order with small canting of moments in and about the crystal $c$ axis are obtained. For reduced tetragonal distortion, we find a tunable regime wherein the magnetic order can be tuned (AFM or FM) by the bare SOC strength and octahedral tilting magnitude. In this regime, with decreasing tetragonal distortion, AFM order is maintained by progressively decreasing octahedral tilting, as observed in $\rm Ca_{2-x}Sr_x RuO_4$. For purely planar order, the only self consistent solution is FM order along crystal $b$ axis, which is relevant for the bilayer ruthenate compound $\rm Ca_3 Ru_2 O_7$.

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Correlated motion of particle-hole excitations across the renormalized spin-orbit gap in $\rm Sr_2 Ir O_4$

The high-energy collective modes of particle-hole excitations across the spin-orbit gap in $\rm Sr_2IrO_4$ are investigated using the transformed Coulomb interaction terms in the pseudo-spin-orbital basis constituted by the $J=1/2$ and $3/2$ states arising from spin-orbit coupling. With appropriate interaction strengths and renormalized spin-orbit gap, these collective modes yield two well-defined propagating spin-orbit exciton modes, with energy scale and dispersion in excellent agreement with resonant inelastic X-ray scattering (RIXS) measurements.

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Magnetic order and anisotropic interactions induced by mixing between the $J=1/2$ and $3/2$ sectors in spin-orbit coupled honeycomb-lattice compounds

Novel magnetic ordering on the honeycomb lattice due to emergent weak anisotropic interactions generated by the mixing between the $J=1/2$ sector and the magnetically inactive 3/2 sector is investigated in a three-orbital interacting electron model in the absence of Hund's coupling. Self-consistent determination of magnetic order yields anisotropic Néel and zigzag orders for different parameter regimes, highlighting the effect of the emergent single-ion anisotropy. Study of magnon excitations shows extremely small magnon energy scale compared to the hopping energy scale, and enhancement of anisotropy effects for smaller spin-orbit coupling. These results account for several features of the honeycomb lattice compounds such as $\rm Na_2 Ir O_3$ and $\rm Ru Cl_3$, where the leading order anisotropic interactions within the magnetically active $J=1/2$ sector are completely quenched due to the edge-sharing octahedra.

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Octahedral tilting induced isospin reorientation transition in iridate heterostructures

Iridate heterostructures are gaining interest as their magnetic properties are much more sensitive to structural distortion compared to pure spin systems due to spin-orbital entanglement induced by strong spin-orbit coupling. While bulk monolayer and bilayer iridates show $ab$-plane canted and $c$-axis antiferromagnetic (AFM) order, recent experiments on layered iridate superlattices (SL) have revealed striking properties, especially in the bilayer SL. A spin model is presented including the tilting induced Kitaev type interactions, which illustrates the proclivity towards $ab$-plane canted AFM order. A realistic Hubbard model including spin-dependent hopping terms arising from octahedral rotation and tilting is constructed for the bilayer SL in isospin space, and magnetic excitations are investigated in the self-consistently determined magnetic state. The Hubbard model analysis confirms the spin model results and shows strongly reduced magnon energy gap and an isospin reorientation transition from $c$-axis to $ab$-plane canted AFM order with increasing tilting.

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Intra- and inter-orbital correlated electron spin dynamics in $\rm Sr_2 Ir O_4$: spin-wave gap and spin-orbit exciton

Transformation of Coulomb interaction terms to the pseudo-orbital basis constituted by $J=1/2$ and $3/2$ states arising from spin-orbit coupling provides a versatile tool. This formalism is applied to investigate magnetic anisotropy effects on low-energy spin-wave excitations as well as high-energy spin-orbit exciton modes in $\rm Sr_2 Ir O_4$. The Hund's coupling term explictly yields easy-plane anisotropy, resulting in gapless (in-plane) and gapped (out-of-plane) modes, in agreement with recent resonant inelastic x-ray scattering (RIXS) measurements. The collective mode of inter-orbital, spin-flip, particle-hole excitations with appropriate interaction strengths and renormalized spin-orbit gap yields two well-defined propagating spin-orbit exciton modes, with energy scale and dispersion in good agreement with RIXS studies.

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Spin waves and stability of zigzag order in the Hubbard model with spin-dependent hopping terms - Application to the honeycomb lattice compounds ${\rm Na_2 Ir O_3}$ and ${\rm α- Ru Cl_3}$

Spin waves in the zigzag ordered state on a honeycomb lattice are investigated within a Hubbard model with spin-dependent hopping terms. Roles of the emergent Kitaev, Heisenberg, Dzyaloshinskii-Moriya, and symmetric-off-diagonal spin interactions are investigated on the stability of the zigzag order. While the DM interactions are found to destabilize the zigzag order, the secondary spin-dependent hopping terms (associated with structural distortions) are shown to strongly stabilize the zigzag order and account for magnetocrystalline anisotropy, easy axis, and spin wave gap. The calculated spin wave dispersion and energy scale are in good agreement with inelastic neutron scattering measurements on $\rm α- RuCl_3$ and $\rm Na_2 Ir O_3$.

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Spin-orbit coupling induced magnetic anisotropy and large spin wave gap in $\rm Na Os O_3$

The role of spin-orbit coupling and Hund's rule coupling on magnetic ordering, anisotropy, and excitations are investigated within a minimal three-orbital model for the $5d^3$ compound $\rm Na Os O_3$. Asymmetry between the magnetic moments for the $xy$ and $xz,yz$ orbitals, arising from the hopping asymmetry generated by the $\rm Os O_6$ octahedral tilting and rotation, together with the weak correlation effect, are shown to be crucial for the large SOC induced magnetic anisotropy and spin wave gap observed in this compound. Due to the intrinsic SOC-induced changes in the electronic densities under rotation of the staggered field, their coupling with the orbital energy offset is also found to contribute significantly to the magnetic anisotropy energy.

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Effects of the structural distortion on the electronic band structure of {\boldmath $\rm Na Os O_3$} studied within density functional theory and a three-orbital model

Effects of the structural distortion associated with the $\rm OsO_6$ octahedral rotation and tilting on the electronic band structure and magnetic anisotropy energy for the $5d^3$ compound NaOsO$_3$ are investigated using the density functional theory (DFT) and within a three-orbital model. Comparison of the essential features of the DFT band structures with the three-orbital model for both the undistorted and distorted structures provides insight into the orbital and directional asymmetry in the electron hopping terms resulting from the structural distortion. The orbital mixing terms obtained in the transformed hopping Hamiltonian resulting from the octahedral rotations are shown to account for the fine features in the DFT band structure. Staggered magnetization and the magnetic character of states near the Fermi energy indicate weak coupling behavior.

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Magnetic excitations in a three-orbital model for the strongly spin-orbit coupled iridates: Effect of mixing between the J=1/2 and 3/2 sectors

A three-orbital-model approach for studying spin wave excitations in the strongly spin-orbit coupled layered perovskite iridates is presented which provides a unified description of magnetic excitations as well as the electronic band structure. The calculated spin wave dispersions with realistic three-band parameters are in excellent agreement with the RIXS data for iridates, including the strong AF zone boundary dispersion in the single-layer compound $\rm Sr_2 Ir O_4$ and the large anisotropy gap in the bilayer compound $\rm Sr_3 Ir_2 O_7$. The RIXS spin wave data is shown to provide evidence of mixing between the J=1/2 and 3/2 sectors in both compounds.

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Spin waves in the AF state of the $t$-$t'$ Hubbard model on the fcc lattice: competing interactions, frustration, and instabilities

Spin waves in the type-III ordered antiferromagnetic state of the frustrated $t$-$t'$ Hubbard model on the fcc lattice are calculated to investigate finite-$U$-induced competing interaction and frustration effects on magnetic excitations and instabilities. Particularly strong competing interactions generated due to interplay of fcc lattice geometry and magnetic order result in significant spin wave softening. The calculated spin wave dispersion is found to be in qualitative agreement with the measured spin wave dispersion in the pyrite mineral $\rm Mn S_2$ obtained from inelastic neutron scattering experiments. Instabilities to other magnetic orders (type I, type II, spiral, non-collinear), as signalled by spin wave energies turning negative, are also discussed.

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Multi-orbital quantum antiferromagnetism in iron pnictides --- effective spin couplings and quantum corrections to sublattice magnetization

Towards understanding the multi-orbital quantum antiferromagnetism in iron pnictides, effective spin couplings and spin fluctuation induced quantum corrections to sublattice magnetization are obtained in the $(π,0)$ AF state of a realistic three band interacting electron model involving $xz$, $yz$, and $xy$ Fe 3d orbitals. The $xy$ orbital is found to be mainly responsible for the generation of strong ferromagnetic spin coupling in the $b$ direction, which is critically important to fully account for the spin wave dispersion as measured in inelastic neutron scattering experiments. The ferromagnetic spin coupling is strongly suppressed as the $xy$ band approaches half filling, and is ascribed to particle-hole exchange in the partially filled $xy$ band. The strongest AF spin coupling in the $a$ direction is found to be in the orbital off diagonal sector involving the $xz$ and $xy$ orbitals. First order quantum corrections to sublattice magnetization are evaluated for the three orbitals, and yield a significant $37\%$ average reduction from the Hartree-Fock value.

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