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Magnetic and non-magnetic phases of a quantum spin liquid

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Abstract

A quantum spin-liquid phase is an intriguing possibility for a system of strongly interacting magnetic units in which the usual magnetically ordered ground state is avoided owing to strong quantum fluctuations. It was first predicted theoretically for a triangular-lattice model with antiferromagnetically coupled S = 1/2 spins1. Recently, materials have become available showing persuasive experimental evidence for such a state2. Although many studies show that the ideal triangular lattice of S = 1/2 Heisenberg spins actually orders magnetically into a three-sublattice, non-collinear 120° arrangement, quantum fluctuations significantly reduce the size of the ordered moment3. This residual ordering can be completely suppressed when higher-order ring-exchange magnetic interactions are significant, as found in nearly metallic Mott insulators4. The layered molecular system κ-(BEDT-TTF)2Cu2(CN)3 is a Mott insulator with an almost isotropic, triangular magnetic lattice of spin-1/2 BEDT-TTF dimers5 that provides a prime example of a spin liquid formed in this way6,7,8,9,10,11. Despite a high-temperature exchange coupling, J, of 250 K (ref. 6), no obvious signature of conventional magnetic ordering is seen down to 20 mK (refs 7, 8). Here we show, using muon spin rotation, that applying a small magnetic field to this system produces a quantum phase transition between the spin-liquid phase and an antiferromagnetic phase with a strongly suppressed moment. This can be described as Bose–Einstein condensation of spin excitations with an extremely small spin gap. At higher fields, a second transition is found that suggests a threshold for deconfinement of the spin excitations. Our studies reveal the low-temperature magnetic phase diagram and enable us to measure characteristic critical properties. We compare our results closely with current theoretical models, and this gives some further insight into the nature of the spin-liquid phase.

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Figure 1: Phase diagram for κ-(BEDT-TTF)2Cu2(CN)3.
Figure 2: Low-field QPT and phase boundary.
Figure 3: Electronic spin fluctuation rate.
Figure 4: High-field QPT and critical exponents.

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Acknowledgements

We acknowledge discussions with S. Sachdev, J. Schmalian and T. Senthil. Part of this work was performed at the Swiss Muon Source, Paul Scherrer Institute, Villigen, Switzerland. This work is supported by EPSRC (UK).

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Contributions

F.L.P. and S.O.-K. planned the experiments. F.L.P., P.J.B., S.J.B., T.L., S.O.-K., C.B. and I.W. contributed to the measurements. Y.S., G.S. and K.K. supplied the sample material and supporting NMR measurements. F.L.P. analysed the data and wrote the paper. All authors critically reviewed the paper.

Corresponding author

Correspondence to F. L. Pratt.

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The authors declare no competing financial interests.

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Supplementary Information

The file contains Supplementary Methods, Supplementary Figures 1-4 with legends, Supplementary Notes on Models and Critical Exponents, Supplementary Table 1 and additional references. (PDF 816 kb)

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Pratt, F., Baker, P., Blundell, S. et al. Magnetic and non-magnetic phases of a quantum spin liquid. Nature 471, 612–616 (2011). https://doi.org/10.1038/nature09910

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