Spin-orbit coupling in {Mo${}_3$S${}_7$(dmit)${}_3$}

Abstract

Spin-orbit coupling in crystals is known to lead to unusual direction dependent exchange interactions, however understanding of the consequeces of such effects in molecular crystals is incomplete. Here we perform four component relativistic density functional theory computations on the multi-nuclear molecular crystal {Mo${}_3$S${}_7$(dmit)${}_3$} and show that both intra- and inter-molecular spin-orbit coupling are significant. We determine a long-range relativistic single electron Hamiltonian from first principles by constructing Wannier spin-orbitals. We analyse the various contributions through the lens of group theory. Intermolecular spin-orbit couplings like those found here are known to lead to quantum spin-Hall and topological insulator phases on the 2D lattice formed by the tight-binding model predicted for a single layer of {Mo${}_3$S${}_7$(dmit)${}_3$}.

References in corpus (22)

• $Z_2$ Topological Order and the Quantum Spin Hall Effect
• Anyons in an exactly solved model and beyond
• Maximally localized Wannier functions: Theory and applications
• Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
• Correlated quantum phenomena in the strong spin-orbit regime
• Mott physics and band topology in materials with strong spin-orbit interaction
• Topological Kondo Insulators
• Spin-Orbit Physics Giving Rise to Novel Phases in Correlated Systems: Iridates and Related Materials
• Quantum frustration in organic Mott insulators: from spin liquids to unconventional superconductors
• Interaction-driven topological insulators on the kagome and the decorated honeycomb lattices
• Strong electronic correlations in superconducting organic charge transfer salts
• Theories of phosphorescence in organo-transition metal complexes - from relativistic effects to simple models and design principles for organic light-emitting diodes
• Topological Insulators on the Decorated Honeycomb Lattice
• Ab initio two-dimensional multiband low-energy models of EtMe_3Sb[Pd(dmit)_2]_2 and κ-(BEDT-TTF)_2Cu(NCS)_2 with comparisons to single-band models
• Spin-orbit coupling and strong electronic correlations in cyclic molecules
• Topological spin liquid phase in a low-dimensional organic molecular compound
• Emergence of quasi-one-dimensional physics in Mo${}_3$S${}_7$(dmit)${}_3$, a nearly-isotropic three-dimensional molecular crystal
• Heisenberg and Dzyaloshinskii-Moriya interactions controlled by molecular packing in tri-nuclear organometallic clusters
• Importance of anisotropy in the spin-liquid candidate Me3EtSb[Pd(dmit)2]2
• Haldane insulator protected by reflection symmetry in the doped Hubbard model on the three-legged ladder
• Topological quantum phase transition driven by anisotropic spin-orbit coupling in trinuclear organometallic coordination crystals
• Deriving \textit{ab initio} model Hamiltonians for molecular crystals

Cited by in corpus (12)

• Role of quantum fluctuations on spin liquids and ordered phases in the Heisenberg model on the honeycomb lattice
• The contribution of intermolecular spin interactions to the London dispersion forces between chiral molecules
• Quantum anomalous Hall state from spatially decaying interactions on the decorated honeycomb lattice
• From quantum anomalous Hall phases to topological metals in interacting decorated honeycomb lattices
• Effects of anisotropy in spin molecular-orbital coupling on effective spin models of trinuclear organometallic complexes
• Unconventional superconductivity near a flat band in organic and organometallic materials
• Topological superconductivity from doping a triplet quantum spin liquid in a flat band system
• Magnetism and topological phases in an interacting decorated honeycomb lattice with spin-orbit coupling
• A theory of the quantum spin liquid in the hyper-honeycomb metal-organic framework [(C${}_2$H${}_5$)${}_3$NH]${}_2$Cu${}_2$(C${}_2$O${}_4$)${}_3$ from first principles
• Spin molecular-orbit coupling and magnetic properties of the decorated honeycomb layers of Mo3S7(dmit)3 crystals
• Gapless spinons and a field-induced soliton gap in the hyper-honeycomb Cu oxalate framework compound [(C${}_2$H${}_5$)${}_3$NH]${}_2$Cu${}_2$(C${}_2$O${}_4$)${}_3$
• Tunable Tradeoff between Quantum and Classical Computation via Nonunitary Zeno-like Dynamics