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Robust singlet dimers with fragile ordering in two-dimensional honeycomb lattice of Li2RuO3

Junghwan Park, Teck‐Yee Tan, Devashibhai Thakarshibhai Adroja, Aziz Daoud‐Aladine, Seongil Choi, Deok‐Yong Cho, Sanghyun Lee, Jiyeon Kim, Hasung Sim, Tamaki Morioka, Hiroyuki Nojiri, Krishnamurthy, V. V., Pascal Manuel, M. R. Lees, Sergey V Streltsov, Daniel I. Khomskii, Je‐Geun Park

Published Jan 1, 2016• 31 citations
OpenAlex

Abstract

When an electronic system has strong correlations and a large spin-orbit interaction, it often exhibits a plethora of mutually competing quantum phases. How a particular quantum ground state is selected out of several possibilities is a very interesting question. However, equally fascinating is how such a quantum entangled state breaks up due to perturbation. This important question has relevance in very diverse fields of science from strongly correlated electron physics to quantum information. Here we report that a quantum entangled dimerized state or valence bond crystal (VBC) phase of Li2RuO3 shows nontrivial doping dependence as we perturb the Ru honeycomb lattice by replacing Ru with Li. Through extensive experimental studies, we demonstrate that the VBC phase melts into a valence bond liquid phase of the RVB (resonating valence bond) type. This system offers an interesting playground where one can test and refine our current understanding of the quantum competing phases in a single compound.

Related papers

Robust singlet dimers with fragile ordering in two-dimensional honeycomb lattice of Li2RuO3

Junghwan Park, Teck-Yee Tan, D. T. Adroja +14 more

When an electronic system has strong correlations and a large spin-orbit interaction, it often exhibits a plethora of mutually competing quantum phases. How a particular quantum ground state is selected out of several possibilities is a very interesting question. However, equally fascinating is how such a quantum entangled state breaks up due to perturbation. This important question has relevance in very diverse fields of science from strongly correlated electron physics to quantum information. Here we report that a quantum entangled dimerized state or valence bond crystal (VBC) phase of Li2RuO3 shows nontrivial doping dependence as we perturb the Ru honeycomb lattice by replacing Ru with Li. Through extensive experimental studies, we demonstrate that the VBC phase melts into a valence bond liquid phase of the RVB (resonating valence bond) type. This system offers an interesting playground where one can test and refine our current understanding of the quantum competing phases in a single compound.

arXiv:1604.04019•Scientific Reports•May 4, 2016•33 citations

Kitaev meets Affleck-Kennedy-Lieb-Tasaki: Competing quantum disorder in spin-3/2 honeycomb systems

Sogen Ikegami, Kiyu Fukui, Rico Pohle +1 more

We investigate an S=3/2 quantum spin model on a two-dimensional honeycomb lattice that continuously interpolates between two paradigmatic quantum disordered states with distinct entanglement structures: the Kitaev quantum spin liquid and the Affleck-Kennedy-Lieb-Tasaki (AKLT) valence bond solid. Combining classical, semi-classical, and exact diagonalization approaches, we map out the ground-state phase diagram and elucidate the role of quantum fluctuations across the entire parameter range. While classical and semi-classical frameworks predict noncoplanar orders competing with a collinear Néel state, we find these phases to be fragile: once full quantum fluctuations are included, they melt into a quantum-entangled state characterized by suppressed spin correlations and enhanced entanglement entropy. Our findings highlight how competition between qualitatively different quantum disordered phases provides a fertile playground for unconventional phases emerging from their interplay and quantum fluctuations.

arXiv:2512.06322•Physical review. B./Physical review. B•Mar 16, 2026•1 citation

Observation of valence bond fluctuations in the spin-1/2 honeycomb lattice

Christian Wessler, B. Roessli, Karl W. Krämer +6 more

Quantum spin liquids are materials that feature quantum entangled spin correlations and avoid magnetic long-range order at T = 0 K. Particularly interesting are two-dimensional honeycomb spin lattices where a plethora of exotic quantum spin liquids have been predicted. Here, we experimentally study an effective S=1/2 Heisenberg honeycomb lattice with competing nearest and next-nearest neighbor interactions. We demonstrate that YbBr$_3$ avoids order down to at least T=100 mK and features a dynamic spin-spin correlation function with broad continuum scattering typical of quantum spin liquids near a quantum critical point. The continuum in the spin spectrum is consistent with plaquette type fluctuations predicted by theory. Our study is the experimental demonstration that strong quantum fluctuations can exist on the honeycomb lattice even in the absence of Kitaev-type interactions, and opens a new perspective on quantum spin liquids.

•Mar 5, 2020•0 citations

Topological spin liquids: Robustness under perturbations

Mohsin Iqbal, Helena Casademunt, Norbert Schuch

We study the robustness of the paradigmatic kagome resonating valence bond (RVB) spin liquid and its orthogonal version, the quantum dimer model. The nonorthogonality of singlets in the RVB model and the induced finite length scale not only makes it difficult to analyze, but can also significantly affect its physics, such as how much noise resilience it exhibits. Surprisingly, we find that this is not the case: The amount of perturbations which the RVB spin liquid can tolerate is not affected by the finite correlation length, making the dimer model a viable model for studying RVB physics under perturbations. Remarkably, we find that this is a universal phenomenon protected by symmetries: First, the dominant correlations in the RVB are spinon correlations, making the state robust against doping with visons. Second, reflection symmetry stabilizes the spin liquid against doping with spinons, by forbidding mixing of the initially dominant correlations with those which lead to the breakdown of topological order.

arXiv:1910.06355•Physical review. B./Physical review. B•Mar 2, 2020•7 citations

Phase diagram of a frustrated quantum antiferromagnet on the honeycomb lattice: Magnetic order versus valence-bond crystal formation

A. Fabricio Albuquerque, David R. Schwandt, Balázs Hetényi +3 more

We present a comprehensive computational study of the phase diagram of the frustrated $S=1/2$ Heisenberg antiferromagnet on the honeycomb lattice, with second-nearest $({J}_{2})$ and third-neighbor $({J}_{3})$ couplings. Using a combination of exact diagonalizations (EDs) of the original spin model, of the Hamiltonian projected into the nearest-neighbor short-range valence-bond basis, and of an effective quantum dimer model, as well as a self-consistent cluster mean-field theory, we determine the boundaries of several magnetically ordered phases in the region ${J}_{2},{J}_{3}\ensuremath{\in}[0,1]$, and find a sizable magnetically disordered region in between. We characterize part of this magnetically disordered phase as a plaquette valence-bond crystal phase. At larger ${J}_{2}$, we locate a sizable region in which staggered valence-bond crystal correlations are found to be important, either due to genuine valence-bond crystal (VBC) ordering or as a consequence of magnetically ordered phases, which break lattice rotational symmetry. Furthermore, we find that a particular parameter-free Gutzwiller projected tight-binding wave function has remarkably accurate energies compared to finite-size extrapolated ED energies along the transition line from conventional N\'eel to plaquette VBC phases, a fact that points to possibly interesting critical behavior---such as a deconfined critical point---across this transition. We also comment on the relevance of this spin model to model the spin liquid region found in the half filled Hubbard model on the honeycomb lattice.

arXiv:1102.5325•Physical Review B•Jul 6, 2011•204 citations

Multicolored quantum dimer models, resonating valence-bond states, color visons, and the triangular-lattice t2g spin-orbital system

Bruce Normand

The spin-orbital model for triply degenerate ${t}_{2g}$ electrons on a triangular lattice has been shown to be dominated by dimers. The phase diagram contains both strongly resonating, compound spin-orbital dimer states and quasistatic, spin-singlet valence-bond (VB) states. To elucidate the nature of the true ground state in these different regimes, the model is mapped to a number of quantum dimer models (QDMs), each of which has three dimer colors. The generic multicolored QDM, illustrated for the two- and three-color cases, possesses a topological color structure, ``color vison'' excitations, and broad regions of resonating VB phases. The specific models are analyzed to gain further insight into the likely ground states in the superexchange and direct-exchange limits of the electronic Hamiltonian, and they suggest a strong tendency toward VB order in all cases.

arXiv:1009.5140•Physical Review B•Feb 17, 2011•22 citations
When an electronic system has strong correlations and a large spin-orbit interaction, it often exhibits a plethora of mutually competing quantum phases. How a particular quantum ground state is selected out of several possibilities is a very interesting question. However, equally fascinating is how such a quantum entangled state breaks up due to perturbation. This important question has relevance in very diverse fields of science from strongly correlated electron physics to quantum information. Here we report that a quantum entangled dimerized state or valence bond crystal (VBC) phase of Li2RuO3 shows nontrivial doping dependence as we perturb the Ru honeycomb lattice by replacing Ru with Li. Through extensive experimental studies, we demonstrate that the VBC phase melts into a valence bond liquid phase of the RVB (resonating valence bond) type. This system offers an interesting playground where one can test and refine our current understanding of the quantum competing phases in a single compound.
When an electronic system has strong correlations and a large spin-orbit interaction, it often exhibits a plethora of mutually competing quantum phases. How a particular quantum ground state is selected out of several possibilities is a very interesting question. However, equally fascinating is how such a quantum entangled state breaks up due to perturbation. This important question has relevance in very diverse fields of science from strongly correlated electron physics to quantum information. Here we report that a quantum entangled dimerized state or valence bond crystal (VBC) phase of Li2RuO3 shows nontrivial doping dependence as we perturb the Ru honeycomb lattice by replacing Ru with Li. Through extensive experimental studies, we demonstrate that the VBC phase melts into a valence bond liquid phase of the RVB (resonating valence bond) type. This system offers an interesting playground where one can test and refine our current understanding of the quantum competing phases in a single compound.
We investigate an S=3/2 quantum spin model on a two-dimensional honeycomb lattice that continuously interpolates between two paradigmatic quantum disordered states with distinct entanglement structures: the Kitaev quantum spin liquid and the Affleck-Kennedy-Lieb-Tasaki (AKLT) valence bond solid. Combining classical, semi-classical, and exact diagonalization approaches, we map out the ground-state phase diagram and elucidate the role of quantum fluctuations across the entire parameter range. While classical and semi-classical frameworks predict noncoplanar orders competing with a collinear Néel state, we find these phases to be fragile: once full quantum fluctuations are included, they melt into a quantum-entangled state characterized by suppressed spin correlations and enhanced entanglement entropy. Our findings highlight how competition between qualitatively different quantum disordered phases provides a fertile playground for unconventional phases emerging from their interplay and quantum fluctuations.
Quantum spin liquids are materials that feature quantum entangled spin correlations and avoid magnetic long-range order at T = 0 K. Particularly interesting are two-dimensional honeycomb spin lattices where a plethora of exotic quantum spin liquids have been predicted. Here, we experimentally study an effective S=1/2 Heisenberg honeycomb lattice with competing nearest and next-nearest neighbor interactions. We demonstrate that YbBr3_33​ avoids order down to at least T=100 mK and features a dynamic spin-spin correlation function with broad continuum scattering typical of quantum spin liquids near a quantum critical point. The continuum in the spin spectrum is consistent with plaquette type fluctuations predicted by theory. Our study is the experimental demonstration that strong quantum fluctuations can exist on the honeycomb lattice even in the absence of Kitaev-type interactions, and opens a new perspective on quantum spin liquids.
We study the robustness of the paradigmatic kagome resonating valence bond (RVB) spin liquid and its orthogonal version, the quantum dimer model. The nonorthogonality of singlets in the RVB model and the induced finite length scale not only makes it difficult to analyze, but can also significantly affect its physics, such as how much noise resilience it exhibits. Surprisingly, we find that this is not the case: The amount of perturbations which the RVB spin liquid can tolerate is not affected by the finite correlation length, making the dimer model a viable model for studying RVB physics under perturbations. Remarkably, we find that this is a universal phenomenon protected by symmetries: First, the dominant correlations in the RVB are spinon correlations, making the state robust against doping with visons. Second, reflection symmetry stabilizes the spin liquid against doping with spinons, by forbidding mixing of the initially dominant correlations with those which lead to the breakdown of topological order.
We present a comprehensive computational study of the phase diagram of the frustrated S=1/2S=1/2S=1/2 Heisenberg antiferromagnet on the honeycomb lattice, with second-nearest (J2)({J}_{2})(J2​) and third-neighbor (J3)({J}_{3})(J3​) couplings. Using a combination of exact diagonalizations (EDs) of the original spin model, of the Hamiltonian projected into the nearest-neighbor short-range valence-bond basis, and of an effective quantum dimer model, as well as a self-consistent cluster mean-field theory, we determine the boundaries of several magnetically ordered phases in the region ${J}_{2},{J}_{3}\ensuremath{\in}[0,1]$, and find a sizable magnetically disordered region in between. We characterize part of this magnetically disordered phase as a plaquette valence-bond crystal phase. At larger J2{J}_{2}J2​, we locate a sizable region in which staggered valence-bond crystal correlations are found to be important, either due to genuine valence-bond crystal (VBC) ordering or as a consequence of magnetically ordered phases, which break lattice rotational symmetry. Furthermore, we find that a particular parameter-free Gutzwiller projected tight-binding wave function has remarkably accurate energies compared to finite-size extrapolated ED energies along the transition line from conventional N\'eel to plaquette VBC phases, a fact that points to possibly interesting critical behavior---such as a deconfined critical point---across this transition. We also comment on the relevance of this spin model to model the spin liquid region found in the half filled Hubbard model on the honeycomb lattice.
The spin-orbital model for triply degenerate t2g{t}_{2g}t2g​ electrons on a triangular lattice has been shown to be dominated by dimers. The phase diagram contains both strongly resonating, compound spin-orbital dimer states and quasistatic, spin-singlet valence-bond (VB) states. To elucidate the nature of the true ground state in these different regimes, the model is mapped to a number of quantum dimer models (QDMs), each of which has three dimer colors. The generic multicolored QDM, illustrated for the two- and three-color cases, possesses a topological color structure, ``color vison'' excitations, and broad regions of resonating VB phases. The specific models are analyzed to gain further insight into the likely ground states in the superexchange and direct-exchange limits of the electronic Hamiltonian, and they suggest a strong tendency toward VB order in all cases.