Transient dynamics of the phase transition in VO2 revealed by mega-electron-volt ultrafast electron diffraction

Chenhang Xu, Cheng Jin, Zijing Chen, Qi Lu, Yun Cheng, Bo Zhang, Fengfeng Qi, Jiajun Chen, Xunqing Yin, Guohua Wang, Dao Xiang () and Dong Qian ()
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Chenhang Xu: Shanghai Jiao Tong University
Cheng Jin: Shanghai Jiao Tong University
Zijing Chen: Shanghai Jiao Tong University
Qi Lu: Shanghai Jiao Tong University
Yun Cheng: Shanghai Jiao Tong University
Bo Zhang: Shanghai Jiao Tong University
Fengfeng Qi: Shanghai Jiao Tong University
Jiajun Chen: Shanghai Jiao Tong University
Xunqing Yin: Shanghai Jiao Tong University
Guohua Wang: Shanghai Jiao Tong University
Dao Xiang: Shanghai Jiao Tong University
Dong Qian: Shanghai Jiao Tong University

Nature Communications, 2023, vol. 14, issue 1, 1-8

Abstract: Abstract Vanadium dioxide (VO2) exhibits an insulator-to-metal transition accompanied by a structural transition near room temperature. This transition can be triggered by an ultrafast laser pulse. Exotic transient states, such as a metallic state without structural transition, were also proposed. These unique characteristics let VO2 have great potential in thermal switchable devices and photonic applications. Although great efforts have been made, the atomic pathway during the photoinduced phase transition is still not clear. Here, we synthesize freestanding quasi-single-crystal VO2 films and examine their photoinduced structural phase transition with mega-electron-volt ultrafast electron diffraction. Leveraging the high signal-to-noise ratio and high temporal resolution, we observe that the disappearance of vanadium dimers and zigzag chains does not coincide with the transformation of crystal symmetry. After photoexcitation, the initial structure is strongly modified within 200 femtoseconds, resulting in a transient monoclinic structure without vanadium dimers and zigzag chains. Then, it continues to evolve to the final tetragonal structure in approximately 5 picoseconds. In addition, only one laser fluence threshold instead of two thresholds suggested in polycrystalline samples is observed in our quasi-single-crystal samples. Our findings provide essential information for a comprehensive understanding of the photoinduced ultrafast phase transition in VO2.

Date: 2023
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DOI: 10.1038/s41467-023-37000-2

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