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We investigate the charge and lattice states in a quasi-one-dimensionalorganic ferroelectric material, TTF-QCl$_{4}$, under pressures of up to 35 kbarby nuclear quadrupole resonance experiments. The results reveal a globalpressure-temperature phase diagram, which spans the electronic and ionicregimes of ferroelectric transitions, which have so far been studiedseparately, in a single material. The revealed phase diagram clearly shows thatthe charge-transfer instability and the lattice symmetry breaking, whichcoincide in the electronic ferroelectric regime at low pressures, bifurcate ata certain pressure, leading to the conventional ferroelectric regime. Thepresent results reveal that the crossover from electronic to ionicferroelectricity occurs through the separation of charge and latticeinstabilities.

Separation of Charge Instability and Lattice Symmetry Breaking in an Organic Ferroelectric