Gapless spinons and a field-induced soliton gap in the hyper-honeycomb Cu oxalate framework compound [(C$_{2}$H$_{5}$)$_{3}$NH]$_{2}$Cu$_{2}$(C$_{2}$O$_{4}$)$_{3}$

TL;DR

This study investigates the magnetic properties of a hyper-honeycomb Cu oxalate compound, revealing gapless spinons, a field-induced soliton gap, and clarifying its nature as a one-dimensional antiferromagnetic chain rather than a quantum spin liquid.

Contribution

The paper combines experimental measurements and DFT calculations to demonstrate the presence of a field-induced soliton gap and clarify the magnetic interactions, challenging the previous quantum spin liquid interpretation.

Findings

Presence of a linear-in-T specific heat indicating fermionic excitations.

Magnetic field induces a gap in spin excitations proportional to H^{2/3}.

The compound is a one-dimensional spin-1/2 Heisenberg antiferromagnet, not a quantum spin liquid.

Abstract

We report a detailed study of the specific heat and magnetic susceptibility of single crystals of a spin liquid candidate: the hyper-honeycomb Cu oxalate framework compound [(C$_2$H$_5$)$_3$NH]$_2$Cu$_2$(C$_2$O$_4$)$_3$. The specific heat shows no anomaly associated with a magnetic transition at low temperatures down to $T\sim$ 180 mK in zero magnetic field. We observe a large linear-in-$T$ contribution to the specific heat $\gamma T$, $\gamma = 98(1)$ mK/mol K$^{2}$, at low temperatures, indicative of the presence of fermionic excitations despite the Mott insulating state. The low-$T$ specific heat is strongly suppressed by applied magnetic fields $H$, which induce an energy gap, $\Delta (H)$, in the spin-excitation spectrum. We use the four-component relativistic density-functional theory (DFT) to calculate the magnetic interactions, including the Dzyaloshinskii-Moriya antisymmetric exchange, which causes an effective staggered field acting on one copper sublattice. The magnitude and field dependence of the field-induced gap, $\Delta (H) \propto H^{2/3}$, are accurately predicted by the soliton mass calculated from the sine-Gordon model of weakly coupled antiferromagnetic Heisenberg chains with all parameters determined by our DFT calculations. Thus our experiment and calculations are entirely consistent with a model of [(C$_2$H$_5$)$_3$NH]$_2$Cu$_2$(C$_2$O$_4$)$_3$ in which anisotropic magnetic exchange interactions due to Jahn-Teller distortion cause one copper sublattice to dimerize, leaving a second sublattice of weakly coupled antiferromagnetic chains. We also show that this model quantitatively accounts for the measured temperature-dependent magnetic susceptibility. Thus [(C$_2$H$_5$)$_3$NH]$_2$Cu$_2$(C$_2$O$_4$)$_3$ is a canonical example of a one-dimensional spin-1/2 Heisenberg antiferromagnet and not a resonating-valence-bond quantum spin liquid, as previously proposed.