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Supercooled Jahn-Teller ice
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DOI：10.1103/PhysRevResearch.4.033157.png)
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When the spins on the frustrated pyrochlore lattice obey the celebrated 2-in-2-out ice rule, they stay in a correlated disordered phase and break the third law of thermodynamics. Similarly, if the atomic ions on the pyrochlore lattice move in and outward of the tetrahedra, they may obey a constraint resembling the ice rule. We discover that a model for pyrochlore molybdates A(2)Mo(2)O(7) (A = Y, Dy, Tb) exhibits a supercooled ice state of the displacement degrees of freedom of Mo4+ ions, when we take account of the Jahn-Teller (JT) effect. The JT effect occurs when the lattice distortions reduce the symmetry of the local crystal field, resulting in the orbital-energy splitting that causes the local energy gain. Unlike the standard JT effect that leads to periodic long-range ordering, the displacements of Mo4+ ions are disordered following the icelike rule. We microscopically derive a model that describes this situation by having the 2nd-and 3rd-neighbor interactions between in-out lattice displacements comparably as strong as the nearest-neighbor interactions of standard ice. There, the well-known nearly flat energy landscape of the ice state is altered to a metastable highly quasidegenerate icelike liquid state coexisting with a crystalline-like ground state. Our Monte Carlo simulations show that this liquid remains remarkably stable down to low temperatures by avoiding the putative first-order transition. The relaxation in the supercooled JT ice state exhibits glassy dynamics with a plateau structure. They fit the feature of a good glass former very often found in molecular liquids but that has never been observed in material solids. The high glass-forming ability of the interacting lattice degrees of freedom will play a key role in the spin-glass transition of the material.
Keyword:
SPIN-GLASS PYROCHLORE
LIQUIDS
ENTROPY
RELAXATION
CRYSTALS
DYNAMICS
FERROMAGNET
TRANSITION
BEHAVIOR
Y2MO2O7
期刊
IF:
4.2
论文数:
7.6K
被引数:
2.7W
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