arXiv subjects

B. J. Powell

Publications and source records attributed to B. J. Powell.

At least 37 records · Page 2Linked to original sources

arXiv2019

Low-energy effective theories of the two-thirds filled Hubbard model on the triangular necklace lattice

Motivated by Mo$_3$S$_7$(dmit)$_3$, we investigate the Hubbard model on the triangular necklace lattice at two-thirds filling. We show, using second order perturbation theory, that in the molecular limit, the ground state and the low energy excitations of this model are identical to those of the spin-one Heisenberg chain. The latter model is known to be in the symmetry protected topological Haldane phase. Away from this limit we show, on the basis of symmetry arguments and density matrix renormalization group (DMRG) calculations, that the low-energy physics of the Hubbard model on the triangular necklace lattice at two-thirds filling is captured by the ferromagnetic Hubbard-Kondo lattice chain at half filling. This is consistent with and strengthens previous claims that both the half-filled ferromagnetic Kondo lattice model and the two-thirds filled Hubbard model on the triangular necklace lattice are also in the Haldane phase. A connection between Hund's rules and Nagaoka's theorem is also discussed.

cond-mat.str-el↗

arXiv2019

Spin-state ice in geometrically frustrated spin-crossover materials

Spin crossover materials contain metal ions that can access two spin-states: one low-spin (LS), the other high-spin (HS). We propose that frustrated elastic interactions can give rise to spin-state ices -- phases of matter without long-range order, characterized by a local constraint or `ice rule'. The low-energy physics of spin-state ices is described by an emergent divergence-less gauge field with a gap to topological excitations that are deconfined quasi-particles with spin fractionalized midway between the spins of the LS and HS states.

cond-mat.str-el↗

arXiv2018

Spin molecular-orbit coupling and magnetic properties of the decorated honeycomb layers of Mo3S7(dmit)3 crystals

We explore the magnetic properties of isolated a-b planes of trinuclear organometallic crystals, Mo3S7(dmit)3, in which an interplay of strong electronic correlations and spin molecular-orbital coupling (SMOC) occurs. The magnetic properties can be described by a XXZ+120, S=1 Heisenberg model on a honeycomb lattice with single-spin anisotropy, D, which depends strongly on SMOC. Based on ab initio estimates of SMOC in Mo3S7(dmit)3 crystals, we predict that the honeycomb layers of Mo3S7(dmit)3 are Neel ordered. However, in materials with a greater degree of magnetic frustration, Neel order can give way to the large-D phase.

cond-mat.str-el↗

arXiv2018

Dynamical reduction of the dimensionality of exchange interactions and the "spin-liquid" phase of $κ$-(BEDT-TTF)$_2X$

We show that the anisotropy of the effective spin model for the dimer Mott insulator phase of $κ$-(BEDT-TTF)$_2X$ salts is dramatically different from that of the underlying tight-binding model. Intra-dimer quantum interference results in a model of coupled spin chains, where frustrated interchain interactions suppress long-range magnetic order. Thus, we argue, the "spin liquid" phase observed in some of these materials is a remnant of the Tomonaga-Luttinger physics of a single chain. This is consistent with previous experiments and resolves some outstanding puzzles. An erratum [Phys. Rev. Lett. 120, 199901 (2018).] is added as an appendix.

cond-mat.str-el↗

arXiv2018

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

We construct a tight-binding model of [(C$_2$H$_5$)$_3$NH]$_2$Cu$_2$(C$_2$O$_4$)$_3$ from Wannier orbital overlaps. Including interactions within the Jahn-Teller distorted Cu-centered $e_g$ Wannier orbitals leads to an effective Heisenberg model. The hyper-honeycomb lattice contains two symmetry distinct sublattices of Cu atoms arranged in coupled chains. One sublattice is strongly dimerized, the other forms isotropic antiferromagnetic chains. Integrating out the strongest (intradimer) exchange interactions leaves extremely weakly coupled Heisenberg chains, consistent with the observed low temperature physics.

cond-mat.str-el↗

arXiv2018

Phase Diagram of the Spin-$1/2$ Triangular $J_1$-$J_2$ Heisenberg Model on a 3-leg Cylinder

We study the phase diagram of the frustrated Heisenberg model on the triangular lattice with nearest and next-nearest neighbor spin exchange coupling, on 3-leg ladders. Using the density-matrix renormalization-group method, we obtain the complete phase diagram of the model, which includes quasi-long-range $120^\circ$ and columnar order, and a Majumdar-Ghosh phase with short-ranged correlations. All these phases are non-chiral and planar. We also identify the nature of phase transitions.

cond-mat.str-el↗

arXiv2018

Magnetic excitations of the Cu$^{2+}$ quantum spin chain in Sr$_3$CuPtO$_6$

We report the magnetic excitation spectrum as measured by inelastic neutron scattering for a polycrystalline sample of Sr$_3$CuPtO$_6$. Modeling the data by the 2+4 spinon contributions to the dynamical susceptibility within the chains, and with interchain coupling treated in the random phase approximation, accounts for the major features of the powder-averaged structure factor. The magnetic excitations broaden considerably as temperature is raised, persisting up to above 100 K and displaying a broad transition as previously seen in the susceptibility data. No spin gap is observed in the dispersive spin excitations at low momentum transfer, which is consistent with the gapless spinon continuum expected from the coordinate Bethe ansatz. However, the temperature dependence of the excitation spectrum gives evidence of some very weak interchain coupling.

cond-mat.str-el↗

arXiv2017

Effects of anisotropy in spin molecular-orbital coupling on effective spin models of trinuclear organometallic complexes

We consider layered decorated honeycomb lattices at two-thirds filling, as realized in some trinuclear organometallic complexes. Localized $S=1$ moments with a single-spin anisotropy emerge from the interplay of Coulomb repulsion and spin molecular-orbit coupling (SMOC). Magnetic anisotropies with bond dependent exchange couplings occur in the honeycomb layers when the direct intracluster exchange and the spin molecular-orbital coupling are both present. We find that the effective spin exchange model within the layers is an XXZ + 120$^\circ$ honeycomb quantum compass model. The intrinsic non-spherical symmetry of the multinuclear complexes leads to very different transverse and longitudinal spin molecular-orbital couplings, which greatly enhances the single-spin and exchange coupling anisotropies. The interlayer coupling is described by a XXZ model with anisotropic biquadratic terms. As the correlation strength increases the systems becomes increasingly one-dimensional. Thus, if the ratio of SMOC to the interlayer hopping is small this stabilizes the Haldane phase. However, as the ratio increases there is a quantum phase transition to the topologically trivial `$D$-phase'. We also predict a quantum phase transition from a Haldane phase to a magnetically ordered phase at sufficiently strong external magnetic fields.

cond-mat.str-el↗

arXiv2017

Nuclear Magnetic Resonance in Low-Symmetry Superconductors

We consider the nuclear spin-lattice relaxation rate, $1/T_1T$ in superconductors with accidental nodes. We show that a Hebel-Slichter-like peak occurs even in the absence of an isotropic component of the superconducting gap. The logarithmic divergence found in clean, non-interacting models is controlled by both disorder and electron-electron interactions. However, for reasonable parameters, neither of these effects removes the peak altogether.

cond-mat.supr-con↗

arXiv2017

Heisenberg and Dzyaloshinskii-Moriya interactions controlled by molecular packing in tri-nuclear organometallic clusters

Motivated by recent synthetic and theoretical progress we consider magnetism in crystals of multi-nuclear organometallic complexes. We calculate the Heisenberg symmetric exchange and the Dzyaloshinskii-Moriya antisymmetric exchange. We show how, in the absence of spin-orbit coupling, the interplay of electronic correlations and quantum interference leads to a quasi-one dimensional effective spin model in a typical tri-nuclear complex, Mo$_3$S$_7$(dmit)$_3$, despite its underlying three dimensional band structure. We show that both intra- and inter-molecular spin-orbit coupling can cause an effective Dzyaloshinskii-Moriya interaction. Furthermore, we show that, even for an isolated pair of molecules the relative orientation of the molecules controls the nature of the Dzyaloshinskii-Moriya coupling. We show that interference effects also play a crucial role in determining the Dzyaloshinskii-Moriya interaction. Thus, we argue, that multi-nuclear organometallic complexes represent an ideal platform to investigate the effects of Dzyaloshinskii-Moriya interactions on quantum magnets.

cond-mat.str-el↗

arXiv2017

Topological frustration and structural balance in strongly correlated itinerant electron systems: an extension of Nagaoka's theorem

We prove that Nagaoka's theorem, that the large-$U$ Hubbard model with exactly one hole is ferromagnetic, holds for any balanced Hamiltonian. Simply put, if a positive bond encodes friendship and a negative bond encodes enmity, then balance implies when that enemy of one's enemy is one's friend. We argue that, in itinerant electron systems, a balanced Hamiltonian, rather than bipartite lattice, defines an unfrustrated system. The proof is valid for multi-orbital models with arbitrary two-orbital interactions provided that no exchange interactions are antiferromagnetic: a class of models including the Kanomori Hamiltonian.

cond-mat.str-el↗

arXiv2017

Spin-orbit coupling and strong electronic correlations in cyclic molecules

In atoms spin-orbit coupling (SOC) cannot raise the angular momentum above a maximum value or lower it below a minimum. Here we show that this need not be the case in materials built from nanoscale structures including multi-nuclear coordination complexes, materials with decorated lattices, or atoms on surfaces. In such cyclic molecules the electronic spin couples to currents running around the molecule. For odd-fold symmetric molecules (e.g., odd membered rings) the SOC is highly analogous to the atomic case; but for even-fold symmetric molecules every angular momentum state can be both raised and lowered. These differences arise because for odd-fold symmetric molecules the maximum and minimum molecular orbital angular momentum states are time reversal conjugates, whereas for even-fold symmetric molecules they are aliases of the same single state. We show, from first principles calculations, that in suitable molecules this molecular SOC is large, compared to the energy differences between frontier molecular orbitals. Finally, we show that, when electronic correlations are strong, molecular SOC can cause highly anisotropic exchange interactions and discuss how this can lead to effective spin models with compass Hamiltonians.

cond-mat.str-el↗

arXiv2016

Haldane insulator protected by reflection symmetry in the doped Hubbard model on the three-legged ladder

We demonstrate the existence of an insulating phase in the three-legged Hubbard ladder at two-thirds filling. In this phase chargons are bound because the physics within a unit cell favors the formation of triplets. The resultant moments lead to a ground state in the Haldane phase, a symmetry protected topological state of matter. In this purely fermionic model, reflection is protecting but time reversal and dihedral symmetries are not, in contrast to spin models.

cond-mat.str-el↗

arXiv2016

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

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)$_3$}.

cond-mat.str-el↗

arXiv2016

Topological quantum phase transition driven by anisotropic spin-orbit coupling in trinuclear organometallic coordination crystals

We show how quasi-one-dimensional correlated insulating states arise at two-thirds filling in organometallic multinuclear coordination complexes described by layered decorated honeycomb lattices. The interplay of spin-orbit coupling and electronic correlations leads to pseudospin-1 moments arranged in weakly coupled chains with highly anisotropic exchange and a large trigonal splitting. This leads to a quantum phase transition from a Haldane phase to a topologically trivial phase as the relative strength of the spin-orbit coupling increases.

cond-mat.str-el↗

arXiv2015

When is the Kadowaki-Woods ratio universal?

We calculate the Kadowaki-Woods ratio (KWR) in Fermi liquids with arbitrary band structures. We find that, contrary to the single band case, the ratio is not generally independent of the effects of electronic correlations (universal). This is very surprising given the experimental findings of a near universal KWR in many multiband metals. We identify a limit where the universality of the ratio, which has been observed experimentally in many strongly correlated electron systems, is recovered. We discuss the KWR in Dirac semimetals in two and three dimensions. In the two-dimensional case we also generalize the KWR to account for the logarithmic factor in the self-energy. In both cases we find that the KWR is independent of correlations, but strongly dependent on the doping of the system: for massless fermions the KWR is proportional to the inverse square of the carrier density, whereas the KWR for systems with massive quasiparticles is proportional to the inverse of the carrier density.

cond-mat.str-el↗

arXiv2015

Theories of phosphorescence in organo-transition metal complexes - from relativistic effects to simple models and design principles for organic light-emitting diodes

We review theories of phosphorescence in cyclometalated complexes. We focus primarily on pseudooctahedrally coordinated $t_{2g}^6$ metals (e.g., [Os(II)(bpy)$_3$]$^{2+}$, Ir(III)(ppy)$_3$ and Ir(III)(ptz)$_3$) as, for reasons that are explored in detail, these show particularly strong phosphorescence. We discuss both first principles approaches and semi-empirical models, e.g., ligand field theory. We show that together these provide a clear understanding of the photophysics and in particular the lowest energy triplet excitation, T$_1$. In order to build a good model relativistic effects need to be included. The role of spin-orbit coupling is well-known, but scalar relativistic effects are also large - and are therefore also introduced and discussed. No expertise in special relativity or relativistic quantum mechanics is assumed and a pedagogical introduction to these subjects is given. It is shown that, once both scalar relativistic effects and spin-orbit coupling are included, time dependent density functional theory (TDDFT) provides quantitatively accurate predictions of the radiative decay rates of the substates of T$_1$ in phosphorescent organotranstion-metal complexes. We describe the pseudo-angular momentum model, and show that it reproduces the key experimental findings. For example, this model provides a simple explanation of the relative radiative rates of the substates of T$_1$, which differ by orders of magnitude. Special emphasis is placed on materials with potential applications as active materials in organic light-emitting diodes (OLEDs) and principles for the design of new complexes are identified on the basis of the insights provided by the theories reviewed. We discuss the remaining theoretical challenges, which include deepening our understanding of solvent effects and, vitally, understanding and predicting non-radiative decay rates.

physics.chem-ph↗

arXiv2015

Emergence of quasi-one-dimensional physics in Mo$_3$S$_7$(dmit)$_3$, a nearly-isotropic three-dimensional molecular crystal

We report density functional theory calculations for Mo$_3$S$_7$(dmit)$_3$. We derive an ab initio tight-binding model from overlaps of Wannier orbitals; finding a layered model with interlayer hopping terms $\sim3/4$ the size of the in-plane terms. The in-plane Hamiltonian interpolates the kagomé and honeycomb lattices. It supports states localized to dodecahedral rings within the plane, which populate one-dimensional (1D) bands and lead to a quasi-1D spin-one model on a layered honeycomb lattice once interactions are included. Two lines of Dirac cones also cross the Fermi energy.

cond-mat.str-el↗