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Traversing Double-Well Potential Energy Surfaces: Photoinduced Concurrent Intralayer and Interlayer Structural Transitions in XTe2 (X = Mo, W)

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Qi,  Yingpeng
Physical Chemistry, Fritz Haber Institute, Max Planck Society;
Center for Ultrafast Science and Technology, School of Physics and Astronomy, Shanghai Jiao Tong University;

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Zahn,  Daniela
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Vasileiadis,  Thomas
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Seiler,  Helene
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Windsor,  Yoav William
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Ernstorfer,  Ralph
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Citation

Qi, Y., Guan, M., Zahn, D., Vasileiadis, T., Seiler, H., Windsor, Y. W., et al. (2022). Traversing Double-Well Potential Energy Surfaces: Photoinduced Concurrent Intralayer and Interlayer Structural Transitions in XTe2 (X = Mo, W). ACS Nano, 16(7), 11124-11135. doi:/10.1021/acsnano.2c03809.


Cite as: https://hdl.handle.net/21.11116/0000-000A-C254-C
Abstract
The microscopic arrangement of atoms and molecules is the determining factor in how materials behave and perform; i.e., the structure determines the property, a traditional paradigm in materials science. Photoexcitation-driven manipulation of the crystal structure and associated electronic properties in quantum materials provides opportunities for the exploration of exotic physics and practical applications; however, a generalized mechanism for such symmetry engineering is absent. Here, by ultrafast electron diffraction, structure factor calculation, and TDDFT-MD simulations, we report the photoinduced concurrent intralayer and interlayer structural transitions in the Td and 1T′ phases of XTe2 (X = Mo, W). We discuss the modification of multiple quantum electronic states associated with the intralayer and interlayer structural transitions, such as the topological band inversion and the higher-order topological state. The twin structures and the stacking faults in XTe2 are also identified by ultrafast structural responses. The comprehensive study of the ultrafast structural response in XTe2 suggests the traversal of all double-well potential energy surfaces (DWPES) by laser excitation, which is expected to be an intrinsic mechanism in the field of photoexcitation-driven global/local symmetry engineering and also a critical ingredient inducing the exotic properties in the non-equilibrium state in a large number of material systems.