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arXiv:2408.03372 · Nature Physics

A resonant valence bond spin liquid in the dilute limit of doped frustrated Mott insulators

Cecilie Glittum, Antonio Štrkalj, D. Prabhakaran, Paul Goddard, Cristian D. Batista, Claudio Castelnovo

Published May 29, 2025• 16 citations
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Abstract

Ideas about resonant valence bond liquids and spin-charge separation have led to key concepts in physics such as quantum spin liquids, emergent gauge symmetries, topological order and fractionalization. Despite extensive efforts to demonstrate the existence of a resonant valence bond phase in the Hubbard model that originally motivated the concept, a definitive realization has yet to be achieved. Here we present a solution to this long-standing problem by uncovering a resonant valence bond phase exhibiting spin-charge separation in realistic Hamiltonians. We show analytically that this ground state emerges in the dilute-doping limit of a half-filled Mott insulator on corner-sharing tetrahedral lattices with frustrated hopping, in the absence of exchange interactions. We confirm numerically that the results extend to finite exchange interactions, finite-sized systems and finite dopant density. Although much attention has been devoted to the emergence of unconventional states from geometrically frustrated interactions, our work demonstrates that kinetic energy frustration in doped Mott insulators may be essential for stabilizing robust, topologically ordered states in real materials.

DOI
10.1038/s41567-025-02923-8

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Ideas about resonant valence bond liquids and spin-charge separation have led to key concepts in physics such as quantum spin liquids, emergent gauge symmetries, topological order and fractionalization. Despite extensive efforts to demonstrate the existence of a resonant valence bond phase in the Hubbard model that originally motivated the concept, a definitive realization has yet to be achieved. Here we present a solution to this long-standing problem by uncovering a resonant valence bond phase exhibiting spin-charge separation in realistic Hamiltonians. We show analytically that this ground state emerges in the dilute-doping limit of a half-filled Mott insulator on corner-sharing tetrahedral lattices with frustrated hopping, in the absence of exchange interactions. We confirm numerically that the results extend to finite exchange interactions, finite-sized systems and finite dopant density. Although much attention has been devoted to the emergence of unconventional states from geometrically frustrated interactions, our work demonstrates that kinetic energy frustration in doped Mott insulators may be essential for stabilizing robust, topologically ordered states in real materials.
We propose a class of ground states for doped Mott insulators in the electron second quantization representation. They are obtained from a bosonic resonating valence bond (RVB) theory of the $t\text{\penalty1000-\hskip0pt}J$ model. At half filling, the ground state describes spin correlations of the S=1∕2S=1∕2S=1∕2 Heisenberg model very accurately. Its spin degrees of freedom are characterized by RVB pairing of spins, the size of which decreases continuously as holes are doped into the system. Charge degrees of freedom emerge upon doping and are described by twisted holes in the RVB background. We show that the twisted holes exhibit an off diagonal long range order (ODLRO) in the pseudogap ground state, which has a finite pairing amplitude, but is short of phase coherence. Unpaired spins in such a pseudogap ground state behave as free vortices, preventing superconducting phase coherence. The existence of nodal quasiparticles is also ensured by such a hidden ODLRO in the ground state, which is non-Fermi liquidlike in the absence of superconducting phase coherence. Two distinct types of spin excitations can also be constructed. The superconducting instability of the pseudogap ground state is discussed and a ddd-wave superconducting ground state is obtained. This class of pseudogap and superconducting ground states unifies antiferromagnetism, pseudogap, superconductivity, and Mott physics into a new state of matter.
The Hubbard model encapsulates the physics of strongly correlated quantum systems in its most basic form. It has been studied intensively in the context of the high-temperature superconductivity. A number of novel phases were recently proposed for Hubbard-like models on the honeycomb lattice, the structure of graphene. We analyzed the Hubbard model of spin- 12\frac{1}{2}21​ fermions on the honeycomb lattice at half-filling using large-scale quantum Monte Carlo simulations. We find that the weak coupling semimetal and the antiferromagnetic Mott insulator at strong interaction are separated by an extended gapped phase in an intermediate coupling regime. Exploring excitation gaps, various correlation functions as well as probing for flux quantization, we conclude that a quantum spin liquid, lacking any conventional order, emerges with local charge and spin correlations, best described by a resonating valence bonds state.
We investigate the ground state of the d1{d}^{1}d1 spin-orbital model for triply degenerate t2g{t}_{2g}t2g​ orbitals on a triangular lattice that unifies intrinsic frustration of spin and orbital interactions with geometrical frustration. Using full or Lanczos exact diagonalization of finite clusters, we establish that the ground state of the spin-orbital model that interpolates between superexchange and direct exchange interactions on the bonds is characterized by valence-bond correlations. In the absence of Hund's exchange the model describes a competition between various possible valence-bond states. By considering the clusters with open boundary conditions we demonstrate that orbital interactions are always frustrated, but this frustration is removed by pronounced spin singlet correlations that coexist with dimer orbital correlations supporting them. Such local configurations contribute to the disordered ground states found for the clusters with periodic boundary conditions that interpolate between a highly resonating, dimer-based, entangled spin-orbital liquid phase and a valence-bond state with completely static spin-singlet states. We argue that these states are also realized for the infinite lattice and anticipate that pronounced transitions between different regimes found for particular geometries will turn out to smooth crossovers in the properties of the spin-orbital liquid in the thermodynamic limit. Finally, we provide evidence that the resonating spin-orbital liquid phase involves entangled states on the bonds. In such a phase classical considerations based on the mean-field theory cannot be used, spin exchange interactions do not determine spin bond correlations, and quantum fluctuations play a crucial role in the ground states and magnetic transitions.
Understanding ferromagnetism mechanism in doped Mott insulators on frustrated lattices remains challenging at intermediate coupling and finite doping. Here, we study the itinerant ferromagnetism and propose its mechanism in doped Mott insulators on a geometrically frustrated triangular lattice. Using large-scale density matrix renormalization group (DMRG) and unrestricted Hartree–Fock mean-field methods, we reveal that itinerant ferromagnetism appears at intermediate coupling (10 ≲ U ≪ ∞) near 50% electron doping in the triangular-lattice Hubbard model. By analyzing all microscopic hopping processes, we find that doublon-singlon exchange alone drives the fully polarized ferromagnetism and uncovers the particle-hole asymmetry. We also establish the magnetic phase diagram and compare local spin correlations with recent experiments. Random phase approximation and DMRG calculations consistently confirm that the ferromagnetism persists when SU(2) symmetry is explicitly broken by magnetic anisotropy. These results clarify a microscopic route to itinerant ferromagnetism at intermediate coupling and finite doping in doped Mott insulators. Understanding the mechanism of ferromagnetism in strongly correlated systems is an ongoing theoretical challenge and the Hubbard model is typically adopted to investigate such systems. Here, the authors numerically investigate the doped triangular Fermi-Hubbard model and show ferromagnetism at intermediate coupling and finite doping, which results from the interplay of kinetic doublon-singlon exchange and lattice geometry.
We study the hole-doped Kitaev-Heisenberg chain using the density-matrix renormalization group. In the Kitaev-only limit, the bond-directional exchange itself promotes pairing, favoring spin-singlet and spin-triplet superconducting tendencies for antiferromagnetic and ferromagnetic Kitaev couplings, respectively, together with finite-size Majorana edge correlations suggestive of topological superconductivity. In the full Kitaev-Heisenberg chain, cooperative J - and K exchanges broadly stabilize superconductivity, while competition between J and K induces a strong filling dependence and enables superconductivity even when both J and K are weak. At quarter filling, this competition produces a Mott insulator with spontaneous hopping dimerization. These results identify magnetic frustration as a common mechanism underlying superconducting and interaction-driven insulating phases in doped Kitaev systems.
In the past few decades, tremendous efforts have been made toward understanding the exotic physics emerging from competition between various ordering tendencies in strongly correlated systems. Employing state-of-the-art quantum Monte Carlo simulation, we investigate an interacting SU(N) fermionic model with varying interaction strength and value of N, and we unveil the ground-state phase diagram of the model exhibiting a plethora of exotic phases. For small values of N-namely, N=2, 3-the ground state is an antiferromagnetic (AFM) phase, whereas in the large-N limit, a staggered valence bond solid (VBS) order is dominant. For intermediate values of N such as N=4, 5, remarkably, our study reveals that distinct VBS orders appear in the weak and strong coupling regimes. More fantastically, the competition between staggered and columnar VBS ordering tendencies gives rise to a Mott insulating phase without spontaneous symmetry breaking (SSB), existing in a large interacting parameter regime, which is consistent with a gapped quantum spin liquid. Our study not only provides a platform to investigate the fundamental physics of quantum many-body systems-it also offers a novel route toward searching for exotic states of matter such as quantum spin liquid in realistic quantum materials.