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The pressure-induced phase transition from a neutral regular stack to an ionic dimerized stack (NR-ID) in the tetrathiafulvalene chloranil charge-transfer crystal has been studied by Raman spectroscopy. An accurate estimate of the change of ionicity during the phase transition is obtained from calculations of mode frequencies which are based on the trimer (NR phase) and dimer (ID phase) models of the electron--molecular-vibration interaction. The possibility of the formation of ionic dimers embedded in neutral chains as precursors of the phase change is discussed.
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Hanfland et al. (1988) studied this question.
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