Ultrafast atomic dimerization of Peierls distortion in semimetal molybdenum ditelluride

TL;DR

This study reveals ultrafast atomic dimerization in 1T'-MoTe2 driven by photoexcitation, combining experimental ultrafast electron diffraction and DFT calculations to uncover the rapid structural changes and electronic mechanisms involved.

Contribution

It provides new insights into the ultrafast lattice dynamics and Peierls distortion mechanisms in 1T'-MoTe2 using combined experimental and theoretical approaches.

Findings

Shear displacement and Mo-Mo bond shortening occur within a few picoseconds.

Metastable structure persists for nanoseconds after photoexcitation.

Photodoped electrons induce changes in antibonding states leading to dimerization.

Abstract

Semimetal molybdenum ditelluride (1T'-MoTe$_2$) possess 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'-MoTe$_2$ 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, basing on the analyses of structure factor and pair distribution function. The DFT calculations reveal that, the photodoped electrons induced population change of the antibonding states close to Fermi level, lead to the shear displacement and the dimerization of Mo pairs. Our findings present new insights for elucidating the picture of Peierls distortion in 1T'-MoTe$_2$.