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

Christian Wessler, B. Roessli, Karl W. Krämer, B. Delley, O. Waldmann, L. Keller, Denis V. Sheptyakov, Hans‐Benjamin Braun, M. Kenzelmann

Published Mar 5, 2020• 0 citations
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Abstract

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.

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

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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-neighbour interactions. We demonstrate that YbBr3 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.

•Jan 1, 2020•22 citations

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Abstract Quantum spin liquids are materials that feature quantum entangled spin correlations and avoid magnetic long-range order atT = 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 effectiveS = 1/2 Heisenberg honeycomb lattice with competing nearest and next-nearest-neighbour interactions. We demonstrate that YbBr3avoids order down to at leastT = 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.

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We explore the phase diagram of the Kitaev-Heisenberg model with nearest neighbor interactions on the honeycomb lattice using the exact diagonalization of finite systems combined with the cluster mean field approximation, and supplemented by the insights from analytic approaches: the linear spin-wave and second-order perturbation theories. This study confirms that by varying the balance between the Heisenberg and Kitaev term, frustrated exchange interactions stabilize in this model either one of four phases with magnetic long range order: N\'eel phase, ferromagnetic phase, and two other phases with coexisting antiferromagnetic and ferromagnetic bonds, zigzag and stripy phase, or one of two distinct spin-liquid phases. Out of these latter disordered phases, the one with ferromagnetic Kitaev interactions has a substantially broader range of stability as the neighboring competing ordered phases, ferromagnetic and stripy, have very weak quantum fluctuations. Focusing on the quantum spin-liquid phases, we study spatial spin correlations and dynamic spin structure factor of the model by the exact diagonalization technique, and discuss the evolution of gapped low-energy spin response across the quantum phase transitions between the disordered spin liquid and phases with long range magnetic order.

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Spin dynamics and continuum spectra of the honeycomb J 1 − J 2 antiferromagnetic Heisenberg model

Cheng Gu, Shun-Li Yu, Jian‐Xin Li

We employ the spin cluster perturbation theory to investigate the dynamical properties of the antiferromagnetic ${J}_{1}\text{\ensuremath{-}}{J}_{2}$ Heisenberg model on the honeycomb lattice. We obtain the excitation spectra for all possible phases in the phase diagram, including the N\'eel phase, plaquette valence-bond-solid phase, dimer valence-bond-solid phase, and stripe antiferromagnetic phase. In the N\'eel phase, besides the obvious renormalization of the magnon dispersion, we find that the spectrum exhibits a dome-shaped broad continuum around the second Brillouin zone (BZ) and the additional strong continuum close to the corner of the BZ. In the valence-bond-solid phases, the spectra are dominated by a strong broad continuum all the way down to below ${J}_{1}$ coexisting with the lowest-energy triplon modes characterizing the plaquette and dimer phases. We ascribe this strong broad continuum and the additional continuum close to the BZ corner in the N\'eel phase to the contributions of fractionalized spinon excitations. In the stripe phase, a clear difference from the linear-spin-wave approximation is that the spectrum is gapped at the $M$ point, while that obtained by the latter is gapless due to the strong quantum fluctuations. We point out that the features observed in the N\'eel phase are consistent with the recent neutron scattering experiments on ${\mathrm{YbCl}}_{3}$ and ${\mathrm{YbBr}}_{3}$.

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

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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.

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Competition between spin liquids and valence-bond order in the frustrated spin- 12 Heisenberg model on the honeycomb lattice

Francesco Ferrari, Samuel Bieri, Federico Becca

Using variational wave functions and Monte Carlo techniques, we study the antiferromagnetic Heisenberg model with first-neighbor ${J}_{1}$ and second-neighbor ${J}_{2}$ antiferromagnetic couplings on the honeycomb lattice. We perform a systematic comparison of magnetically ordered and nonmagnetic states (spin liquids and valence-bond solids) to obtain the ground-state phase diagram. N\'eel order is stabilized for small values of the frustrating second-neighbor coupling. Increasing the ratio ${J}_{2}/{J}_{1}$, we find strong evidence for a continuous transition to a nonmagnetic phase at ${J}_{2}/{J}_{1}\ensuremath{\approx}0.23$. Close to the transition point, the Gutzwiller-projected uniform resonating valence-bond state gives an excellent approximation to the exact ground-state energy. For $0.23\ensuremath{\lesssim}{J}_{2}/{J}_{1}\ensuremath{\lesssim}0.36$, a gapless ${Z}_{2}$ spin liquid with Dirac nodes competes with a plaquette valence-bond solid. In contrast, the gapped spin liquid considered in previous works has significantly higher variational energy. Although the plaquette valence-bond order is expected to be present as soon as the N\'eel order melts, this ordered state becomes clearly favored only for ${J}_{2}/{J}_{1}\ensuremath{\gtrsim}0.3$. Finally, for $0.36\ensuremath{\lesssim}{J}_{2}/{J}_{1}\ensuremath{\le}0.5$, a valence-bond solid with columnar order takes over as the ground state, being also lower in energy than the magnetic state with collinear order. We perform a detailed finite-size scaling and standard data collapse analysis, and we discuss the possibility of a deconfined quantum critical point separating the N\'eel antiferromagnet from the plaquette valence-bond solid.

arXiv:1706.07810•Physical review. B./Physical review. B•Sep 1, 2017•46 citations
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.
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-neighbour interactions. We demonstrate that YbBr3 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.
Abstract Quantum spin liquids are materials that feature quantum entangled spin correlations and avoid magnetic long-range order atT = 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 effectiveS = 1/2 Heisenberg honeycomb lattice with competing nearest and next-nearest-neighbour interactions. We demonstrate that YbBr3avoids order down to at leastT = 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 explore the phase diagram of the Kitaev-Heisenberg model with nearest neighbor interactions on the honeycomb lattice using the exact diagonalization of finite systems combined with the cluster mean field approximation, and supplemented by the insights from analytic approaches: the linear spin-wave and second-order perturbation theories. This study confirms that by varying the balance between the Heisenberg and Kitaev term, frustrated exchange interactions stabilize in this model either one of four phases with magnetic long range order: N\'eel phase, ferromagnetic phase, and two other phases with coexisting antiferromagnetic and ferromagnetic bonds, zigzag and stripy phase, or one of two distinct spin-liquid phases. Out of these latter disordered phases, the one with ferromagnetic Kitaev interactions has a substantially broader range of stability as the neighboring competing ordered phases, ferromagnetic and stripy, have very weak quantum fluctuations. Focusing on the quantum spin-liquid phases, we study spatial spin correlations and dynamic spin structure factor of the model by the exact diagonalization technique, and discuss the evolution of gapped low-energy spin response across the quantum phase transitions between the disordered spin liquid and phases with long range magnetic order.
We employ the spin cluster perturbation theory to investigate the dynamical properties of the antiferromagnetic ${J}_{1}\text{\ensuremath{-}}{J}_{2}$ Heisenberg model on the honeycomb lattice. We obtain the excitation spectra for all possible phases in the phase diagram, including the N\'eel phase, plaquette valence-bond-solid phase, dimer valence-bond-solid phase, and stripe antiferromagnetic phase. In the N\'eel phase, besides the obvious renormalization of the magnon dispersion, we find that the spectrum exhibits a dome-shaped broad continuum around the second Brillouin zone (BZ) and the additional strong continuum close to the corner of the BZ. In the valence-bond-solid phases, the spectra are dominated by a strong broad continuum all the way down to below J1{J}_{1}J1​ coexisting with the lowest-energy triplon modes characterizing the plaquette and dimer phases. We ascribe this strong broad continuum and the additional continuum close to the BZ corner in the N\'eel phase to the contributions of fractionalized spinon excitations. In the stripe phase, a clear difference from the linear-spin-wave approximation is that the spectrum is gapped at the MMM point, while that obtained by the latter is gapless due to the strong quantum fluctuations. We point out that the features observed in the N\'eel phase are consistent with the recent neutron scattering experiments on YbCl3{\mathrm{YbCl}}_{3}YbCl3​ and YbBr3{\mathrm{YbBr}}_{3}YbBr3​.
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.
Using variational wave functions and Monte Carlo techniques, we study the antiferromagnetic Heisenberg model with first-neighbor J1{J}_{1}J1​ and second-neighbor J2{J}_{2}J2​ antiferromagnetic couplings on the honeycomb lattice. We perform a systematic comparison of magnetically ordered and nonmagnetic states (spin liquids and valence-bond solids) to obtain the ground-state phase diagram. N\'eel order is stabilized for small values of the frustrating second-neighbor coupling. Increasing the ratio J2/J1{J}_{2}/{J}_{1}J2​/J1​, we find strong evidence for a continuous transition to a nonmagnetic phase at ${J}_{2}/{J}_{1}\ensuremath{\approx}0.23$. Close to the transition point, the Gutzwiller-projected uniform resonating valence-bond state gives an excellent approximation to the exact ground-state energy. For $0.23\ensuremath{\lesssim}{J}_{2}/{J}_{1}\ensuremath{\lesssim}0.36$, a gapless Z2{Z}_{2}Z2​ spin liquid with Dirac nodes competes with a plaquette valence-bond solid. In contrast, the gapped spin liquid considered in previous works has significantly higher variational energy. Although the plaquette valence-bond order is expected to be present as soon as the N\'eel order melts, this ordered state becomes clearly favored only for ${J}_{2}/{J}_{1}\ensuremath{\gtrsim}0.3$. Finally, for $0.36\ensuremath{\lesssim}{J}_{2}/{J}_{1}\ensuremath{\le}0.5$, a valence-bond solid with columnar order takes over as the ground state, being also lower in energy than the magnetic state with collinear order. We perform a detailed finite-size scaling and standard data collapse analysis, and we discuss the possibility of a deconfined quantum critical point separating the N\'eel antiferromagnet from the plaquette valence-bond solid.