Static and dynamic order of cooperative multi-electron transfer

Abstract

We report on high correlation and ordering of multi-electron transfer at neutral-ionic transformation in quasi–one-dimensional prototype crystal of tetrathiafulvalene-chloranil (TTF-CA). We present experimental evidences that the ordering of lattice-relaxed charge-transfer strings, which are nano-scale objects, occurs under static thermal equilibrium condition and non-equilibrium one achieved by femto-second laser irradiation. We suggest that the transformation is a profound example of self-organized, cooperative electron transfer with tendency for phase separation driven by energetics of inter-chain interaction and ferroelectric ordering.