The magnetic Hamiltonian and phase diagram of the quantum spin liquid Ca10Cr7O28

TL;DR

This paper characterizes the magnetic Hamiltonian and phase diagram of Ca10Cr7O28, revealing a complex, frustrated system with a novel Hamiltonian that supports quantum spin liquid behavior, expanding understanding beyond known models.

Contribution

It provides the first detailed determination of the Hamiltonian of Ca10Cr7O28 using inelastic neutron scattering and explores its phase diagram, revealing unique interactions not fitting existing spin liquid models.

Findings

Ca10Cr7O28 has a complex Hamiltonian with competing ferromagnetic and antiferromagnetic interactions.

The material exhibits a quantum spin liquid state with dynamic spins and broad excitation spectrum.

Unexpectedly, ferromagnetic interactions are stronger than antiferromagnetic ones in this system.

Abstract

A spin liquid is a new state of matter with topological order where the spin moments continue to fluctuate coherently down to the lowest temperatures rather than develop static long-range magnetic order as found in conventional magnets. For spin liquid behavior to arise in a material the magnetic Hamiltonian must be "frustrated" where the combination of lattice geometry, interactions and anisotropies gives rise to competing spin arrangements in the ground state. Theoretical Hamiltonians which produce spin liquids are spin ice, the Kitaev honeycomb model and the Heisenberg kagome antiferromagnet. Spin liquid behavior however in real materials is rare because they can only approximate these Hamiltonians and often have weak higher order terms that destroy the spin liquid state. Ca10Cr7O28 is a new quantum spin liquid with magnetic Cr5+ ions that possess quantum spin number S=1/2. The spins are entirely dynamic in the ground state and the excitation spectrum is broad and diffuse as is typical of spinons which are the excitations of a spin liquid. In this paper we determine the Hamiltonian of Ca10Cr7O28 using inelastic neutron scattering under high magnetic field to induce a ferromagnetic ground state and spin-wave excitations that can be fitted to extract the interactions. We further explore the phase diagram by using inelastic neutron scattering and heat capacity measurements and establish the boundaries of the spin liquid phase as a function of magnetic field and temperature. Our results show that Ca10Cr7O28 consists of distorted kagome bilayers with several isotropic ferromagnetic and antiferromagnetic interactions where unexpectedly the ferromagnetic interactions are stronger than the antiferromagnetic ones. This complex Hamiltonian does not correspond to any known spin liquid model and points to new directions in the search for quantum spin liquid behavior.