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For the photoinduced ionic → neutral structural phase transition in the organic charge transfer crystal TTF-CA, we, at first, theoretically show the adiabatic path of this transition, which starts from a single charge transfer (CT) exciton in the ionic phase, but finally results in a macroscopic neutral domain. In the next, using a more simplified model, we theoretically study nonlinear nonequilibrium quantum time-evolution dynamics of the photoinduced phase transition, with a special emphasis on the multistability of the ground state and the “initial condition sensitivity” of the exciton proliferation, both characterize the nonlinearity of this system. [ABSTRACT FROM AUTHOR]