Abstract

The photoexcited state in a correlated electron system with a spin-state degree of freedom is studied. We start from the two-orbital extended Hubbard model where the energy difference between the two orbitals is introduced. The photoexcited metastable state is examined based on the effective model Hamiltonian derived using the two-orbital Hubbard model. Spin-state change is induced by photoirradiation in the low-spin band insulator near the phase boundary, and it is found that a high-spin state is stabilized by creating a ferromagnetic bound state with photodoped hole carriers. An optical absorption occurs between the bonding and antibonding orbitals inside the bound state. The time evolution of photoexcited states is simulated in the time-dependent mean-field scheme. It is found that pair annihilations of photodoped electrons and holes generate the high-spin state in a low-spin band insulator. We propose that this process is directly observed by the time-resolved photoemission experiments.

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