Goal:The goal of this project is to gain theoretical insight into magnetism in the presence of spin-orbit coupling (SOC) for multi-orbital Mott insulators.Inspired by the exact solution of the Kitaev model that harbors a quantum spin liquid with novel excitations and struck by its relevance for materials with anisotropic orbital interactions, the research will explore various new classes of 4d and 5d transition metal oxides and make Testable predictions for three experiments: nuclear magnetic resonance (NMR) and resonant x-ray scattering (RXS) to probe orbital ordering and pump-probe experiments to probe quantum dynamics will test the validity of these models for materials. Significant Achievements:Starting with all electron Hamiltonians, we derived minimal effective magnetic models.This description allowed us to understand the role played by orbital frustration, even in the absence of any geometric frustration, in creating orbitally ordered as well as spin-orbital liquid phases.Orbital frustration arises primarily from the directional or anisotropic nature of d-orbitals in contrast to the isotropic nature of the spin degree of freedom.These models were investigated by a variety of theoretical and numerical methods, including exact diagonalization, mean field theories, density matrix renormalization group, and quantum Monte Carlo methods.We discuss the main results below encapsulated in 12 papers, including several in high impact journals, during this grant period.They cover a range of topics from quantum spin liquids to superconductivity.
Goal:The goal of this project is to gain theoretical insight into magnetism in the presence of spin-orbit coupling (SOC) for multi-orbital Mott insulators.Inspired by the exact solution of the Kitaev model that harbors a quantum spin liquid with novel excitations and struck by its relevance for materials with anisotropic orbital interactions, the research will explore various new classes of 4d and 5d transition metal oxides and make Testable predictions for three experiments: nuclear magnetic resonance (NMR) and resonant x-ray scattering (RXS) to probe orbital ordering and pump-probe experiments to probe quantum dynamics will test the validity of these models for materials. Significant Achievements:Starting with all electron Hamiltonians, we derived minimal effective magnetic models.This description allowed us to understand the role played by orbital frustration, even in the absence of any geometric frustration, in creating orbitally ordered as well as spin-orbital liquid phases.Orbital frustration arises primarily from the directional or anisotropic nature of d-orbitals in contrast to the isotropic nature of the spin degree of freedom.These models were investigated by a variety of theoretical and numerical methods, including exact diagonalization, mean field theories, density matrix renormalization group, and quantum Monte Carlo methods.We discuss the main results below encapsulated in 12 papers, including several in high impact journals, during this grant period.They cover a range of topics from quantum spin liquids to superconductivity.
Quantum spin liquids (QSLs) are strongly correlated systems displaying fascinating phenomena like long-range entanglement and fractionalized excitations. The research on these states has since its beginning followed trends generated by the synthesis of new compounds and the construction of new theoretical tools. In coherence with this history, a manifold of new results about QSLs were established during the past decade due to studies on the integrable Kitaev model on the honeycomb lattice. This j = 1/2 model displays bond-dependent and anisotropic exchanges that are essential to stabilize its QSL ground state with Majorana fermion excitations and emergent Z2 gauge field. Even more interestingly, this model is relevant to understand the magnetism of a certain class of 4/5d5 Mott insulators with specific lattice constraints, t2g orbital degeneracy and strong spin-orbit coupling (SOC). This mechanism defining these so-called Kitaev materials can be applied to similar compounds based on transition metal ions in different electronic configurations. In this thesis, I investigate minimal models for two types of 4/5d1 Mott insulators: the ones on the ordered double perovskite structure (ODP) and the ones isostructural to the Kitaev materials. Their effective models generically show bond-dependent and anisotropic interactions involving multipoles of an effective j = 3/2 angular momentum. Such degrees of freedom are conveniently written in terms of pseudospin s and pseudo-orbital τ operators resembling spin and orbital operators of Kugel-Khomskii models with twofold orbital degeneracy. Despite their anisotropy, the two realistic models display continuous global symmetries in the limit of vanishing Hund\'s coupling enhancing quantum fluctuations and possibly stabilizing a QSL phase. Parton mean-field theory was used to propose fermionic QSLs that will be called quantum spin-orbital liquids (QSOLs) due their dependence with s and τ. On ODPs, I studied a chiral QSOL with Majorana fermion excitations and a gapless spectrum characterized by nodal lines along the edges of the Brillouin zone. These nodal lines are topological defects of a non-Abelian Berry connection and the system exhibits dispersing surface states. Several experimental responses of the chiral QSOL within the mean-field approximation are compared with the experimental data available for the spin liquid candidate Ba2YMoO6. Moreover, based on a symmetry analysis, I discuss the operators involved in resonant inelastic X-ray scattering (RIXS) amplitudes for 4/5d1 Mott insulators and show that the RIXS cross sections allow one to selectively probe pseudospin and pseudo-orbital degrees of freedom. For the chiral spin-orbital liquid in particular, these cross sections provide information about the spectrum for different flavors of Majorana fermions. The model for materials isostructural to the Kitaev materials has an emergent SU(4) symmetry that is made explicit by means of a Klein transformation on pseudospin degrees of freedom. The model is known to stabilize a QSOL on the honeycomb lattice and instigated the investigation of QSOLs on a generalization of this lattice to three dimensions. Parton mean-field theory was used once again to propose the liquid states, and a variational Monte Carlo (VMC) method was used to compute the energies of the projected wave functions. The numerical results show that the lowest-energy QSOL corresponds to a zero-flux state with a Fermi surface of four-color fermionic partons. Further VMC computations also revealed that this state is stable against formation of plaquette ordering (tetramerization). The energy of this QSOL is highly competitive even when Hund\'s coupling induced perturbations are included, as shown by comparison with simple ordered states. Extensions and perspectives for future work are discussed in the end of this thesis.
In this doctoral dissertation, we consider the significance of spin-orbit coupling for the phases of matter which arise for strongly correlated electrons. We explore emergent behavior in quantum many-body systems, including symmetry-breaking orders, quantum spin liquids, and unconventional superconductivity. Our study is cemented by a particular class of Mott-insulating materials, centered around a family of two- and three-dimensional iridium oxides, whose honeycomb-like lattice structure admits peculiar magnetic interactions, the so-called Kitaev exchange. By analyzing recent experiments on these compounds, we show that this unconventional exchange is the key ingredient in describing their magnetism, and then use a combination of numerical and analytical techniques to investigate the implications for the phase diagram as well as the physics of the proximate three-dimensional quantum spin liquid phases. These long-ranged-entangled fractionalized phases should exhibit special features, including finite-temperature stability as well as unconventional high-Tc superconductivity upon charge-doping, which should aid future experimental searches for spin liquid physics. Our study explores the nature of frustration and fractionalization which can arise in quantum systems in the presence of strong spin-orbit coupling.
When sizable quantum fluctuations and strong frustration mechanisms act in concert to repel the formation of conventional long-range order in quantum magnets, they can make way for massively entangled spin liquid phases which may imbue the material with extraordinary properties. \nThe search for such curious phases of matter has proceeded for several decades, gaining extra momentum some fifteen years ago when Kitaev proposed an analytically solvable model for a quantum spin liquid with anyonic excitations on the basis of realistic microscopic spin exchange terms [Kitaev, Annals of Physics 321, 2 (2006)]. Attempts to identify different models or materials which harbor quantum spin liquid ground states have kept researchers -- experimentalists and theorists alike -- in suspense ever since. However, the simulation of quantum many-body systems poses a serious challenge even to modern numerical techniques, particularly in the case of frustrated quantum magnetism in three spatial dimensions. Such models evade tractability by many established approaches, leaving a methodological void. \n \nIn this thesis, we report on recent progress in cutting-edge implementations of the pseudo-fermion functional renormalization group (pf-FRG), which has originally been proposed by Reuther and Wölfle in the context of two-dimensional frustrated quantum magnetism with highly symmetric spin interactions [Reuther and Wölfle, Phys. Rev. B 81, 144410 (2010)]. Reflecting the growing interest in models with SU(2) symmetry-breaking spin exchange terms that has followed the unearthing of Kitaev's honeycomb model, we present a generalized implementation of the pf-FRG which is suited to numerically simulate arbitrary microscopic models with diagonal or off-diagonal two-spin interactions, even in three-dimensional frustrated quantum magnets. We provide insight into the inner workings of the method which has emerged over the course of the last couple of years, arguing that the pf-FRG formalism simultaneously combines aspects of a large-S expansion as well as a large-N expansion on equal footing, thus being able to resolve the subtle interplay between magnetic ordering tendencies and disruptive quantum fluctuations. \n \nMoreover, on a case by case basis we explore the stability of quantum spin liquids in paradigmatic models of frustrated quantum magnetism and elucidate the joint action of geometric frustration, exchange frustration, and quantum fluctuations to inhibit the formation of magnetic long-range order. Examples include: (i) a Heisenberg spin model on the three-dimensional diamond lattice where geometric frustration arises from antiferromagnetic next-nearest neighbor interactions. The additional competition with nearest neighbor interactions leads to an unusually large ground state degeneracy already on classical level. The quantum-to-classical transition is studied by systematically varying the spin length and the different roles of quantum fluctuations and thermal fluctuations are discussed. The theory is applied to interpret experiments on the spin-liquid candidate NiRh2O4; (ii) a Heisenberg antiferromagnet on the face centered cubic lattice which is augmented by competing bond-directional interactions, evolving around the concurrent manifestation of geometric frustration and exchange frustration. A situation is identified where both mechanisms collude to give rise to an unusually large degree of frustration over a wide parameter regime. We discuss related experimental findings on the highly frustrated iridate compound Ba2CeIrO6; (iii) a Heisenberg antiferromagnet on the kagome lattice with additional Dzyaloshinskii-Moriya interactions. The robustness of the unperturbed kagome antiferromagnet's spin liquid ground state against low-symmetry Dzyaloshinskii-Moriya interactions is investigated. Implications for the spin-liquid candidate herbertsmithite are discussed.
Transition metal compounds have been central to the study of quantum magnetism in recent years. The multi-orbital nature of these compounds together with the interplay between electron-electron interactions, crystal field effects and spin-orbit coupling leads to spin-orbit entangled wave functions, known as pseudospins. Pseudospins depend highly on the electron filling of the transition metal, and are highly spatially anisotropic which leads to frustrated, bond-dependent exchange interactions. These interactions manifest themselves in a variety of non-trivial ways, depending on the structure and dimensionality of the underlying lattice, which we explore in this thesis. In one dimension we show that CoNb2O6, thought to be the best known candidate for the 1D transverse field Ising model, is an example of a rare 1D Kitaev chain where the bond-dependent pseudospin interactions are responsible for the transverse field Ising behaviour. On the two dimensional honeycomb lattice we propose a mechanism to generate the bond-dependent, exactly solvable, Yao-Lee interaction among others. We show at the exactly solveable point of our model, the ground state is a quantum spin-orbital liquid with emergent fermionic octupolar excitations. Finally, we study the three dimensional 5d double-perovskites (DPs), which have been proposed to be the first d-orbital candidates exhibiting hidden octupolar order. We develop a microscopic theory for these materials, and determine several microscopic mechanisms that may be responsible for stabilizing octupolar order.
In the quest for materials hosting Kitaev spin liquids, much of the efforts have been focused on the fourth- and fifth-row transition metal compounds, which are spin-orbit coupling--assisted Mott insulators. Here we study the structural and magnetic properties of 3d transition metal oxides, Na2Co2TeO6 and Na3Co2SbO6. The partial occupancy of sodium in former compound is addressed using a cluster expansion, and a honeycomb lattice of sodiums is found to be energetically favored. Starting from the ab initio band structures, a many-body second-order perturbation theory leads to a pseudospin-21 Hamiltonian with estimated magnetic interactions. We show that the experimentally observed zigzag magnetic state is stabilized only when the first-neighbor Kitaev coupling dominates over the Heisenberg term, both of which are highly suppressed due to presence of eg orbitals. A third-neighbor Heisenberg interaction is found dominant in both these compounds. We also present a phase diagram for Na2Co2TeO6 by varying the electron-electron and spin-orbit interactions. The computed spin excitation spectra are found to capture essential features of recent experimental magnon spectrum, lending support to our results.
ABSTRACT Quantum spin liquids (QSLs) are magnetically frustrated phases characterized by spin fractionalization, emergent gauge fields, and long‐range entanglement. Quantum spin–orbital liquids (QSOLs) form a subset of QSLs with fluctuating orbital degrees of freedom, normally adding a layer of complexity to an already involved research field. This topical review provides guidelines for understanding a specific type of QSOL in which the orbital operators facilitate the analysis of quantum liquids, thereby providing adequate starting points for /exploring these phases. Such models are extensions of the spin‐1/2 Kitaev honeycomb model (KHM), in the sense that their exact solutions depend on an extensive number of conserved quantities, combined with a mapping to a problem of Majorana fermions hopping on a static gauge field. The starting points to understand such models are classical Hamiltonians characterized by bond‐dependent Ising interactions. Such classical models are exactly solvable in spin basis thanks to their extensive symmetries and can be directly connected to classical spin ice (CSI) systems that satisfy a Gauss law. QSOLs are easily stabilized in these models by applying a transverse field or introducing other exchange mechanisms that preserve the conserved local operators. The theory of such Ising QSOLs bridges the KHM to specific types of CSIs, thus providing further insight into paradigmatic forms of spin liquids. Furthermore, bond‐dependent Ising models are related to minimal Hamiltonians describing Rydberg‐atom simulations, which provide experimental grounds for investigating them.