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arXiv:2509.08202 · Physical review. B./Physical review. B

Quantum phase with spontaneous translational symmetry breaking in an extended diamond chain

Hironori Yamaguchi, Shunsuke C. Furuya, Y. Tominaga, Akira Matsuo, Koichi Kindo

Published Aug 21, 2025• 1 citation
arXivHTMLPDF

Abstract

We report the experimental realization of a spin-1/2 extended diamond chain in a verdazyl-Cu complex, where competing interactions and lattice distortions give rise to exotic quantum phases. The magnetic properties exhibit a zero-field energy gap and 1/2 magnetization plateau, which is explained by a dimer-monomer model. Considering the effective interactions between the monomers, three types of dimer-dimer phases are expected to appear as the ground state, depending on the magnitude of the lattice distortions. By mapping to the nonlinear sigma model, three phases are distinguished topologically, and a symmetry-protected topological phase equivalent to the Haldane phase is identified. Furthermore, a nontrivial magnetization is observed above the 1/2 plateau region, suggesting a gapped dimer phase accompanied by a spontaneous breaking of translational symmetry. The discovery of this rare quantum state has broad implications for strongly correlated systems, topological matter, and quantum information science, where symmetry and topology play crucial roles.

DOI
10.1103/hbt8-rxxr

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We report the experimental realization of a spin-1/2 extended diamond chain in a verdazyl-Cu complex, where competing interactions and lattice distortions give rise to exotic quantum phases. The magnetic properties exhibit a zero-field energy gap and 1/2 magnetization plateau, which is explained by a dimer-monomer model. Considering the effective interactions between the monomers, three types of dimer-dimer phases are expected to appear as the ground state, depending on the magnitude of the lattice distortions. By mapping to the nonlinear sigma model, three phases are distinguished topologically, and a symmetry-protected topological phase equivalent to the Haldane phase is identified. Furthermore, a nontrivial magnetization is observed above the 1/2 plateau region, suggesting a gapped dimer phase accompanied by a spontaneous breaking of translational symmetry. The discovery of this rare quantum state has broad implications for strongly correlated systems, topological matter, and quantum information science, where symmetry and topology play crucial roles.
The ground states of two types of distorted mixed diamond chains with spins 1 and 1/2 are investigated using exact diagonalization, DMRG, and mapping onto low-energy effective models. In the undistorted case, the ground state consists of an array of independent spin-1 clusters separated by singlet dimers. The lattice distortion induces an effective interaction between cluster spins. When this effective interaction is antiferromagnetic, several Haldane phases appear with or without spontaneous translational symmetry breakdown (STSB). The transition between the Haldane phase without STSB and that with (n+1)(n+1)(n+1)-fold STSB (nnn = 1, 2, and 3) belongs to the same universality class as the (n+1)(n+1)(n+1)-clock model. In contrast, when the effective interaction is ferromagnetic, the quantized and partial ferrimagnetic phases appear with or without STSB. An effective low-energy theory for the partial ferrimagnetic phase is presented.
The ground states of distorted S=1S=1S=1 diamond chains are investigated for two types of distortion called type A and B [J. Phys. Soc. Jpn. 79 (2010) 114703]. For the type A distortion, Haldane phases with and without spontaneous translational symmetry breakdown are present for large values of parameter λλλ that parametrize the strength of frustration. For small λλλ, the Haldane phase and two quantized ferrimagnetic phases in the undistorted chain remain stable even for strong distortion. In contrast, for the type B distortion, the quantized ferrimagnetic phases with and without spontaneous translational symmetry breakdown are present for large λλλ. The partial ferrimagnetic phases emerge between them. For small λλλ, two quantized ferrimagnetic phases remain and the partial ferrimagnetic phases also emerge between them. The Haldane phase between the two kinds of ferrimagnetic phases turns into a topologically trivial double Haldane phase for strong distortion.
The ground-state phases of alternating-bond spin-1 diamond chains are investigated. Each ground state consists of an array of spin clusters separated by singlet dimers owing to an infinite number of local conservation laws. If no singlet dimers are present, the ground state is equivalent to that of a spin chain with infinite length.For strong frustration, we find a series of quantum phase transitions as in the case of alternating-bond mixed diamond chains with spins 1 and 1/2. For intermediate frustration, we find the nonmagnetic Haldane or dimer phases according to whether the bond alternation is weak or strong. For weak frustration and weak bond alternation, we find the ferrimagnetic states with spontaneous magnetizations m=1/6m=1/6m=1/6 and 1/3 per site. The ferrimagnetic state with m=1/6m=1/6m=1/6 is accompanied by a spontaneous translational symmetry breakdown. This phase vanishes for strong bond alternation.
Topological phases of matter are beyond the paradigm of Landau's symmetry breaking and have challenged our understanding of condensed matter systems. Here we report a new type of symmetry-protected topological phase of matter in the spin-1/2 coupled two-leg ladder antiferromagnet C9H18N2CuBr4, DLCB for short. In this two-sublattice antiferromagnet with a weak easy-axis anisotropy, we find no evidence of a conventional spin-flop transition in the magnetization with the magnetic field applied parallel to the easy axis at T=0.4 K, well below TN=2.0 K. Moreover, the temperature dependence of the gapped transverse excitations across TN indicates that they are not the conventional S=1 magnons associated with explicit symmetry breaking. Instead, the thermal renormalization of the gap energy shows a remarkable agreement with a calculation for the three-dimensional O(3) nonlinear sigma model. Accordingly, the spin gap in DLCB is not due to the spin anisotropy but to the separation between a spin singlet state and a triplet excited state. Since an antiferromagnetic spin-1/2 ladder systems can be mapped onto the spin-1 chain, the notion of the Haldane gap is proposed to explain the opening of the spin gap in DLCB. Therefore, the ground state of DLCB is best described as a quantum superposition of a Haldane phase and a Neel-ordered phase, which resembles the quantum state of a qubit in quantum computing. Our results indicate the presence of a symmetry-protected topological order coexisting with an antiferromagnetic order in this material.
The ground-state phases of anisotropic mixed diamond chains with spins 1 and 1/2 are investigated. Both single-site and exchange anisotropies are considered. We find the phases consisting of an array of uncorrelated spin-1 clusters separated by singlet dimers. Except in the simplest case where the cluster consists of a single S=1S=1S=1 spin, this type of ground state breaks the translational symmetry spontaneously. Although the mechanism leading to this type of ground state is the same as that in the isotropic case, it is nonmagnetic or paramagnetic depending on the competition between two types of anisotropy. We also find the Néel, period-doubled Néel, Haldane, and large-DDD phases, where the ground state is a single spin cluster of infinite size equivalent to the spin-1 Heisenberg chain with alternating anisotropies. The ground-state phase diagrams are determined for typical sets of parameters by numerical analysis. In various limiting cases, the ground-state phase diagrams are determined analytically. The low-temperature behaviors of magnetic susceptibility and entropy are investigated to distinguish each phase by observable quantities. The relationship of the present model with the anisotropic rung-alternating ladder with spin-1/2 is also discussed.
By use of mainly the exact diagonalization and the level spectroscopy method, we investigate the ground-state phase diagrams of the S = 1/2 distorted diamond type quantum spin chain with the monomer-monomer interactions and/or ferromagnetic interactions for the zero magnetic field case, as well as the M = M s /3 case and the M = (2/3) M s case, where M is the total magnetization and M s is the saturation magnetization. The magnetization plateau at M = M s /3 vanishes in the region where the ferromagnetic interaction is rather strong. The monomer-monomer interaction remarkably stabilizes the magnetization plateau at M = (2/3) M s .