Spin Induced Optical Conductivity in the Spin Liquid Candidate Herbertsmithite

TL;DR

This study uses terahertz spectroscopy on Herbertsmithite to reveal optical conductivity features indicative of a quantum spin liquid state, showing unconventional frequency and temperature dependence.

Contribution

First experimental observation of spin-induced optical conductivity in Herbertsmithite supporting its quantum spin liquid nature.

Findings

Power-law frequency dependence with exponent ~1.4 in optical conductivity

Increase in absorption as temperature decreases

Evidence consistent with charge-spin interactions in a QSL

Abstract

A quantum spin liquid (QSL) is a state of matter in which magnetic spins interact strongly, but quantum fluctuations inhibit long-range magnetic order even at zero temperature. A QSL has been predicted to have a host of exotic properties, including fractionalized excitations and long-range quantum entanglement. Despite the numerous theoretical studies, experimental realization of a QSL has proved to be challenging due to the lack of candidate materials. The triangular organic salts EtMe3Sb[Pd(dmit)2]2 and {\kappa}-(BEDT-TTF)2Cu2(CN)3, and kagome ZnCu3(OH)6Cl2 (Herbertsmithite) have recently emerged as promising candidates of exhibiting a QSL state, but the nature of their ground states is still elusive. Here we studied a large-area high-quality single crystal of Herbertsmithite by means of time-domain terahertz (THz) spectroscopy. We observed in the low-frequency (0.6-2.2 THz) optical conductivity evidence for the nature of the spin system. In particular, the in-plane absorption spectrum exhibits a unique frequency dependence that can be described by a power-law with an exponent of approximately 1.4, in sharp contrast with the {\omega}^4 dependence expected for an ordered Mott insulator. The absorption is also found to increase as the temperature decreases, a behavior unexpected for conventional insulators. Such features are consistent with recent theory based on the interactions between the charge and spin degrees of freedom in a QSL system.