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- Title
Chasing the spin gap through the phase diagram of a frustrated Mott insulator.
- Authors
Pustogow, A.; Kawasugi, Y.; Sakurakoji, H.; Tajima, N.
- Abstract
The quest for entangled spin excitations has stimulated intense research on frustrated magnetic systems. For almost two decades, the triangular-lattice Mott insulator κ-(BEDT-TTF)2Cu2(CN)3 has been one of the hottest candidates for a gapless quantum spin liquid with itinerant spinons. Very recently, however, this scenario was overturned as electron-spin-resonance (ESR) studies unveiled a spin gap, calling for reevaluation of the magnetic ground state. Here we achieve a precise mapping of this spin-gapped phase through the Mott transition by ultrahigh-resolution strain tuning. Our transport experiments reveal a reentrance of charge localization below T⋆ = 6 K associated with a gap size of 30–50 K. The negative slope of the insulator-metal boundary, dT⋆/dp < 0, evidences the low-entropy nature of the spin-singlet ground state. By tuning the enigmatic '6K anomaly' through the phase diagram of κ-(BEDT-TTF)2Cu2(CN)3, we identify it as the transition to a valence-bond-solid phase, in agreement with previous thermal expansion and magnetic resonance studies. This spin-gapped insulating state persists at T → 0 until unconventional superconductivity and metallic transport proliferate. The Mott insulator κ-(BEDT-TTF)2Cu2(CN)3 has been a strong candidate for a gapless quantum spin liquid, but recent experiments suggested a spin-gapped phase below 6 K. Pustogow et al. study the entropy of this phase by driving the system through the metal-insulator transition with a strain engineering approach.
- Subjects
PHASE diagrams; QUANTUM spin liquid; SPIN excitations; PHASE transitions; THERMAL expansion; METAL-insulator transitions
- Publication
Nature Communications, 2023, Vol 14, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-023-37491-z