Slow spin dynamics in the hyper-honeycomb Lattice [(C2H5)3NH]2Cu2(C2O4)3 revealed by 1H NMR studies

TL;DR

This study investigates the slow spin dynamics in a 3D hyper-honeycomb lattice compound using 1H NMR, revealing persistent Cu spin moments and thermally-activated spin fluctuation slowing down at low temperatures.

Contribution

First detailed NMR analysis of hyper-honeycomb lattice CCCO showing non-spin-singlet ground state and low-temperature spin dynamics.

Findings

No long-range magnetic order down to 50 mK.

Cu spin moments remain at low temperatures.

Spin fluctuations slow down and become thermally activated below 1 K.

Abstract

We report the results of magnetic susceptibility $\chi$ and $^1$H nuclear magnetic resonance (NMR) measurements on a three-dimensional hyper-honeycomb lattice compound [(C$_2$H$_5$)$_3$NH]$_2$Cu$_2$(C$_2$O$_4$)$_3$ (CCCO). The average value of the antiferromagnetic (AFM) exchange coupling between the Cu$^{2+}$ ($S$ = 1/2) spins was determined to be $J$~$\sim$~50 K from the $\chi$ measurements. No long-range magnetic ordering has been observed down to $T$ = 50 mK, although NMR lines become slightly broader at low temperatures below 1 K. The broadening of the NMR spectrum observed below 1 K reveals that the Cu spin moments remain at this temperature, suggesting a non-spin-singlet ground state. The temperature and magnetic field dependence of 1/$T_1$ at temperatures above 20 K is well explained by paramagnetic thermal spin fluctuations where the fluctuation frequency of Cu$^{2+}$ spins is higher than the NMR frequency of the order of MHz. However, a clear signature of the slowing down of the Cu$^{2+}$ spin fluctuations was observed at low temperatures where 1/$T_1$ shows a thermally-activated behavior. The magnetic field dependence of the magnitude of the spin excitation gap suggests that the magnetic behaviors of CCCO are characterized as an AFM chain at low temperatures.