Author(s): Liu, Wen-Hao; Luo, Jun-Wei; Li, Shu-Shen; Wang, Lin-Wang

Source: NPJ COMPUTATIONAL MATERIALS Volume: 7 Issue: 1 Article Number: 117 DOI: 10.1038/s41524-021-00582-w Published: JUL 22 2021

Abstract: The hot carrier cooling occurs in most photoexcitation-induced phase transitions (PIPTs), but its role has often been neglected in many theoretical simulations as well as in proposed mechanisms. Here, by including the previously ignored hot carrier cooling in real-time time-dependent density functional theory (rt-TDDFT) simulations, we investigated the role of hot carrier cooling in PIPTs. Taking IrTe2 as an example, we reveal that the cooling of hot electrons from the higher energy levels of spatially extended states to the lower energy levels of the localized Ir-Ir dimer antibonding states strengthens remarkably the atomic driving forces and enhances atomic kinetic energy. These two factors combine to dissolute the Ir-Ir dimers on a timescale near the limit of atomic motions, thus initiating a deterministic kinetic phase transition. We further demonstrate that the subsequent cooling induces nonradiative recombination of photoexcited electrons and holes, leading to the ultrafast recovery of the Ir-Ir dimers observed experimentally. These findings provide a complete picture of the atomic dynamics in optically excited structural phase transitions.

Accession Number: WOS:000680857700002

eISSN: 2057-3960

Full Text: https://www.nature.com/articles/s41524-021-00582-w