title: Direct photoexcitation of appreciable size of domains without lattice motion in neutral-ionic transition systems.
abstract: In a recent ultrafast pump-probe experiment on a typical neutral-(N-)ionic (I) transition material, tetrathiafulvalene-p-chloranil [S. Iwai, Phys. Rev. Lett. 96, 057403 (2006)10.1103/PhysRevLett.96.057403], it was claimed that an I-phase domain in the N-phase background was very quickly formed even before the lattice started to move. This study proves this idea in terms of an extended Hubbard model that has site-potential alternation and has been frequently used so far. Our focus is on the photoexcited states of the N phase and the optical conductivity spectrum. As a result of accurate spectrum calculation based on a dynamical density-matrix renormalization group technique, we clearly observe photoexcited ionic domains accompanied by no lattice dimerization. Their contribution almost dominates the spectrum near the N-I phase boundary, and we relate this property to the long-tailed spectrum observed in experiments.
authors.affiliation: Graduate University for Advanced Studies, Institute of Materials Structure Science, High Energy Accelerator Research Organization, 1-1 Oho, Tsukuba 305-0801, Japan.
authors.forename: Kaoru
authors.initials: K
authors.lastname: Iwano