Traversing Double-Well Potential Energy Surfaces: Photoinduced Concurrent Intralayer and Interlayer Structural...

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.