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Photoinduced electronic ferroelectric phase in a metal-organic framework

Takahisa Kato, Shu Ohmura, and Akira Takahashi*

  • *Contact author: takahashi.akira@nitech.ac.jp
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Phys. Rev. B 113, 165148 – Published 27 April, 2026

DOI: https://doi.org/10.1103/8vq8-nj6c

Abstract

We investigate the physical properties and lattice relaxation of important photoexcited states in a charge-transfer-type metal-organic framework (NPr4)2[Fe2(Cl2An)3]. We construct the one-dimensional spinless fermion model for the material and numerically calculate the photoexcited states and the lattice-relaxed states from them. The ground state is a charge-ordered (CO) state with a uniform lattice. The dominant peak in the light absorption spectrum corresponds to an optically allowed bond order wave (BOW) state with charge disproportionation (CD). This Franck-Condon BOW state forms as a linear combination of two degenerate inversion-symmetry-broken BOW states, which have different phases of bond order alternation, combined with the CD, and the inversion symmetry is restored in the state. The Franck-Condon BOW state is strongly coupled to the lattice deformation of bond length alternation, and lattice relaxation can occur even in this rigid material. The lattice-relaxed state originating from the Franck-Condon state is a BOW state with CD, where inversion symmetry is broken due to bond length alternation, making it an electronic ferroelectric state. The largest peak in the induced light absorption spectrum from this lattice-relaxed BOW state results from excitation to another BOW state with CD, which has the opposite phase of bond order alternation. This state is also an electronic ferroelectric, with its polarization opposite to that of the lattice-relaxed BOW state from the Franck-Condon state. This shows that polarization can be reversed instantly through resonant photoexcitation from the lattice-relaxed state.

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Phys. Rev. B 113, 165148– Published 27 April, 2026
  • Received 29 October 2025
  • Revised 18 February 2026
  • Accepted 11 March 2026
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