Physics – Condensed Matter – Strongly Correlated Electrons
Scientific paper
2004-08-13
J. Phys. Soc. Jpn. 73, 2868 (2004)
Physics
Condensed Matter
Strongly Correlated Electrons
24 pages, 11 figures
Scientific paper
10.1143/JPSJ.73.2868
Photoinduced dynamics of charge density and lattice displacements is calculated by solving the time-dependent Schr\"odinger equation for a one-dimensional extended Peierls-Hubbard model with alternating potentials for the mixed-stack organic charge-transfer complex, TTF-CA. A pulse of oscillating electric field is incorporated into the Peierls phase of the transfer integral. The frequency, the amplitude, and the duration of the pulse are varied to study the nonlinear and cooperative character of the photoinduced transition. When the dimerized ionic phase is photoexcited, the threshold behavior is clearly observed by plotting the final ionicity as a function of the increment of the total energy. Above the threshold photoexcitation, the electronic state reaches the neutral one with equidistant molecules after the electric field is turned off. The transition is initiated by nucleation of a metastable neutral domain, for which an electric field with frequency below the linear absorption peak is more effective than that at the peak. When the pulse is strong and short, the charge transfer takes place on the same time scale with the disappearance of dimerization. As the pulse becomes weak and long, the dimerization-induced polarization is disordered to restore the inversion symmetry on average before the charge transfer takes place to bring the system neutral. Thus, a paraelectric ionic phase is transiently realized by a weak electric field. It is shown that infrared light also induces the ionic-to-neutral transition, which is characterized by the threshold behavior.
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