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Emergence of a real-space symmetry axis in the magnetoresistance of the one-dimensional conductor Li_0.9Mo₆O₁₇.

ABSTRACT: We report on an emerging symmetry axis in the magnetoresistance of bulk single crystals of quasi-one-dimensional Li_0.9Mo₆O₁₇ below T _min = 25 K, the temperature at which the electrical resistivity experiences a minimum. Detailed angle-dependent magnetoresistance sweeps reveal that this symmetry axis is induced by the development of a negative magnetoresistance, which is suppressed only for magnetic fields oriented along the poles of the MoO₆ octahedra that form the conducting chains. We show that this unusual negative magnetoresistance is consistent with the melting of dark excitons, composed of previously omitted orbitals within the t _2g manifold that order below T _min. The unveiled symmetry axis in directional magnetic fields not only provides evidence for the crystallization of these dark excitons but also sheds new light on the long-standing mystery of the metal-insulator transition in Li_0.9Mo₆O₁₇.

SUBMITTER: Lu J

PROVIDER: S-EPMC6611691 | biostudies-literature | 2019 Jul

REPOSITORIES: biostudies-literature

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Publications

Emergence of a real-space symmetry axis in the magnetoresistance of the one-dimensional conductor Li0.9Mo6O17.

Lu Jianming J Xu Xiaofeng X Greenblatt M M Jin R R Tinnemans P P Licciardello S S van Delft M R MR Buhot J J Chudzinski P P Hussey N E NE

Science advances 20190705 7

We report on an emerging symmetry axis in the magnetoresistance of bulk single crystals of quasi-one-dimensional Li0.9Mo6O17 below T min = 25 K, the temperature at which the electrical resistivity experiences a minimum. Detailed angle-dependent magnetoresistance sweeps reveal that this symmetry axis is induced by the development of a negative magnetoresistance, which is suppressed only for magnetic fields oriented along the poles of the MoO ...[more]

PMID: 31281877

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Project description:The development of fast Li ion-conducting materials for use as solid electrolytes that provide sufficient electrochemical stability against electrode materials is paramount for the future of all-solid-state batteries. Advances on these fast ionic materials are dependent on building structure-ionic mobility-function relationships. Here, we exploit a series of multinuclear and multidimensional nuclear magnetic resonance (NMR) approaches, including 6Li and 31P magic angle spinning (MAS), in conjunction with density functional theory (DFT) to provide a detailed understanding of the local structure of the ultraphosphate Li3P5O14, a promising candidate for an oxide-based Li ion conductor that has been shown to be a highly conductive, energetically favorable, and electrochemically stable potential solid electrolyte. We have reported a comprehensive assignment of the ultraphosphate layer and layered Li6O16 26- chains through 31P and 6Li MAS NMR, respectively, in conjunction with DFT. The chemical shift anisotropy of the eight resonances with the lowest 31P chemical shift is significantly lower than that of the 12 remaining resonances, suggesting the phosphate bonding nature of these P sites being one that bridges to three other phosphate groups. We employed a number of complementary 6,7Li NMR techniques, including MAS variable-temperature line narrowing spectra, spin-alignment echo (SAE) NMR, and relaxometry, to quantify the lithium ion dynamics in Li3P5O14. Detailed analysis of the diffusion-induced spin-lattice relaxation data allowed for experimental verification of the three-dimensional Li diffusion previously proposed computationally. The 6Li NMR relaxation rates suggest sites Li1 and Li5 (the only five-coordinate Li site) are the most mobile and are adjacent to one another, both in the a-b plane (intralayer) and on the c-axis (interlayer). As shown in the 6Li-6Li exchange spectroscopy NMR spectra, sites Li1 and Li5 likely exchange with one another both between adjacent layered Li6O16 26- chains and through the center of the P12O36 12- rings forming the three-dimensional pathway. The understanding of the Li ion mobility pathways in high-performing solid electrolytes outlines a route for further development of such materials to improve their performance.

Dataset Information

Emergence of a real-space symmetry axis in the magnetoresistance of the one-dimensional conductor Li_0.9Mo₆O₁₇.

Publications

Emergence of a real-space symmetry axis in the magnetoresistance of the one-dimensional conductor Li<sub>0.9</sub>Mo<sub>6</sub>O<sub>17</sub>.

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