Ultrafast atomic dimerization of Peierls distortion in semimetal molybdenum ditelluride

Semimetal molybdenum ditelluride (1T′-MoTe2) possesses diverse phase transitions, enriching its application prospects. The structural response during these transitions is crucial to understanding the underlying mechanisms, but the desired details of pathway and time span are still insufficient. Here, we investigate the lattice evolution in few-layer 1T′-MoTe2 after photoexcitation, using ultrafast electron diffraction and density functional theory (DFT) calculations. The observed complex lattice responses with unintuitively evolving Bragg peak intensity and interplanar spacing are best interpreted as the combination of shear displacement and Mo–Mo bond shortening in a few picoseconds, and a metastable structure in nanoseconds, based on the analyses of structure factor and pair distribution function. The DFT calculations reveal that photodoped electrons induce population change of the antibonding states close to the Fermi level, leading to shear displacement and dimerization of Mo pairs. Our findings present valuable insights for elucidating the picture of Peierls distortion in 1T′-MoTe2.