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    Structural Contribution to Light-Induced Gap Suppression in Ta2NiSe5

    Zijing Chen1,2,3,*, Chenhang Xu4,5,*, Chendi Xie6,*, Weichen Tang7,8, Qiaomei Liu9, Dong Wu10, Qing Xu1,2,3, Tao Jiang1,2,3, Pengfei Zhu1,2,3,11 et al.

    Xiao Zou1,2,3, Jun Li12, Zhiwei Wang13,14,15, Nanlin Wang9,10, Dong Qian11,16,17,†, Alfred Zong4,5,‡, and Dao Xiang1,2,3,11,§

    • *These authors contributed equally to this work.
    • †Contact author: dqian@sjtu.edu.cn
    • ‡Contact author: alfredz@stanford.edu
    • §Contact author: dxiang@sjtu.edu.cn

    Phys. Rev. Lett. 135, 096901 – Published 26 August, 2025

    DOI: https://doi.org/10.1103/1kzk-sz7g

    Abstract

    An excitonic insulator is a material that hosts an exotic ground state, where an energy gap opens due to spontaneous condensation of bound electron-hole pairs. Ta2NiSe5 is a promising candidate for this type of material, but the coexistence of a structural phase transition with the gap opening has led to a long-standing debate regarding the origin of the insulating gap. Here we employ MeV ultrafast electron diffraction to obtain quantitative insights into the atomic displacements in Ta2NiSe5 following photoexcitation, which has been overlooked in previous time-resolved spectroscopy studies. In conjunction with first-principles calculations using the measured atomic displacements, we find that the structural change can largely account for the photoinduced reduction in the energy gap without considering excitonic effects. Our Letter illustrates the importance of a quantitative reconstruction of individual atomic pathways during nonequilibrium phase transitions, paving the way for a mechanistic understanding of a diverse array of phase transitions in correlated materials where lattice dynamics can play a pivotal role.

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