Abstract

A two-step neutral-ionic transition has been discovered in a 1:1 mixed-stack charge-transfer crystal, (3,3',5,5') tetramethylbenzidine-(7,7,8,8) tetracyanoquinodimethane (TMB-TCNQ) under pressure. The fraction of ionized molecules changes discontinuously at two critical pressures, P 1 ∼6 and P 2 ∼20 kbar, demonstrating a characteristic feature of a staging phenomena. This result is interpreted in terms of a frustration effect of Coulomb interactions in the crystal, as predicted theoretically by Hubbard and Torrance

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