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Robust spin liquid state against magnetic-dilution in the bi-layer Kagome material Ca$_{10}$Cr$_7$O$_{28}$

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 Added by Yogesh Singh
 Publication date 2020
  fields Physics
and research's language is English




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Recently, the bi-layer Kagome lattice material Ca$_{10}$Cr$_7$O$_{28}$ has been shown to be a quasi-two-dimensional quantum spin liquid (QSL) where the frustration arises from a balance between competing ferromagnetic and antiferromagnetic exchange within a bi-layer. In an attempt to understand what happens when this balance is disturbed, we present a magnetic dilution study. Specifically, we have synthesized Ca$_{10}$(Cr$_{1-x}$V$_x$)$_7$O$_{28}$ (0 $leq$ x $leq$ 0.5) where magnetic Cr$^{5+}$ ($S = 1/2$) is partially replaced by non-magnetic V$^{5+}$ ($S = 0$). We also synthesized the fully non-magnetic isostructural material Ca$_{10}$V$_7$O$_{27.5}$. We report a detailed structural, magnetic and heat capacity study on these materials. A monotonic increase in the unit cell parameters is found for the Ca$_{10}$(Cr$_{1-x}$V$_x$)$_7$O$_{28}$ materials with increasing $x$. An order of magnitude decrease in the Curie-Weiss temperature from $4$ to $0.5$~ K is found for the partial V substituted samples, which indicates a relative increase in antiferromagnetic exchange with increase in V content. However, despite this change in the relative balance in the exchange interactions and the large disorder introduced, no magnetic ordering or spin-glass state is observed down to $2$~K in the V substituted samples. The QSL state of the parent compound thus seems surprisingly robust against these large perturbations.



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Quantum spin liquids are exotic quantum phases of matter that do not order even at zero temperature. While there are several toy models and simple Hamiltonians that could host a quantum spin liquid as their ground state, it is very rare to find actual, realistic materials that exhibits their properties. At the same time, the classical simulation of such instances of strongly correlated systems is intricate and reliable methods are scarce. In this work, we investigate the quantum magnet Ca$_{10}$Cr$_7$O$_{28}$ that has recently been discovered to exhibit properties of a quantum spin liquid in inelastic neutron scattering experiments. This compound has a distorted bilayer Kagome lattice crystal structure consisting of Cr$^{5+}$ ions with spin-$1/2$ moments. Coincidentally, the lattice structure renders a tensor network algorithm in 2D applicable that can be seen as a new variant of a projected entangled simplex state algorithm in the thermodynamic limit. In this first numerical investigation of this material that takes into account genuine quantum correlations, good agreement with the experimental findings is found. We argue that this is one of the very first studies of physical materials in the laboratory with tensor network methods, contributing to uplifting tensor networks from conceptual tools to methods to describe real two-dimensional quantum materials.
Ca$_{10}$Cr$_7$O$_{28}$ is a novel spin-$1/2$ magnet exhibiting spin liquid behaviour which sets it apart from any previously studied model or material. However, understanding Ca$_{10}$Cr$_7$O$_{28}$ presents a significant challenge, because the low symmetry of the crystal structure leads to very complex interactions, with up to seven inequivalent coupling parameters in the unit cell. Here we explore the origin of the spin-liquid behaviour in Ca$_{10}$Cr$_7$O$_{28}$, starting from the simplest microscopic model consistent with experiment - a Heisenberg model on a single bilayer of the breathing-kagome (BBK) lattice. We use a combination of classical Monte Carlo (MC) simulation and (semi-)classical Molecular Dynamics (MD) simulation to explore the thermodynamic and dynamic properties of this model, and compare these with experimental results for Ca$_{10}$Cr$_7$O$_{28}$. We uncover qualitatively different behaviours on different timescales, and argue that the ground state of Ca$_{10}$Cr$_7$O$_{28}$ is born out of a slowly-fluctuating spiral spin liquid, while faster fluctuations echo the U(1) spin liquid found in the kagome antiferromagnet. We also identify key differences between longitudinal and transverse spin excitations in applied magnetic field, and argue that these are a distinguishing feature of the spin liquid in the BBK model.
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