The experimental quest for a quantum spin-liquid state (QSL) in frustrated magnetic systems addresses fundamental scientific interests, as this intriguing quantum phase provides excellent grounds for discovering exotic collective phenomena. ZnCu3(OH)6Cl2 (herbertsmithite), an S=1/2 kagomé-lattice Heisenberg antiferromagnet, is the most promising candidate for experimentally realizing a QSL. However, despite years of intense research, the nature of its paramagnetic ground state remains highly debated. The root cause of the controversy lies in the difficulty in distinguishing the effects of defects from the intrinsic properties of the kagomé lattice.
In this thesis, we present 17-O nuclear magnetic resonance (NMR) measurements of an isotope-enriched ZnCu3(OH)6Cl2 single crystal. We succeeded in distinguishing the intrinsic magnetic behavior of the kagomé lattice from the defect-induced phenomena down to T~0.01J, where J~200K is the Cu-Cu super-exchange interaction. We identify NMR signals arising from the nearest-neighbor 17-O sites of Cu2+ defects occupying the Zn2+ interlayer sites. From the 17-O Knight shift measurements, we show that these Cu2+ defects induce a large Curie-Weiss contribution to the bulk-averaged susceptibility at low temperatures. Moreover, our 17-O single-crystal lineshapes show no signature of nonmagnetic Zn2+ defects within the kagomé lattice, and therefore, we rule out “anti-site disorder” as a cause of the paramagnetic ground state in ZnCu3(OH)6Cl2. Most importantly, we demonstrate that the intrinsic spin susceptibility of the kagome lattice asymptotically tends to zero below T~0.03J, indicating the presence of a finite gap Δ = 0.03~ 0.07J in the spin excitation spectrum; this gap is completely suppressed under the application of a high magnetic field of ~ 9T. The behavior of low-energy spin fluctuations probed by the 17-O nuclear spin-lattice relaxation rate is consistent with the gap signature observed for the 17-O Knight shift. In short, our 17-O NMR results provide the first experimental evidence for a gapped QSL realized in ZnCu3(OH)6Cl2. / Thesis / Doctor of Philosophy (PhD)
| Identifer | oai:union.ndltd.org:mcmaster.ca/oai:macsphere.mcmaster.ca:11375/18502 |
| Date | 20 November 2015 |
| Creators | Fu, Mingxuan |
| Contributors | Imai, Takashi, Physics and Astronomy |
| Source Sets | McMaster University |
| Language | en_US |
| Detected Language | English |
| Type | Thesis |
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