期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 13, 期 43, 页码 10230-10236出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.2c02448
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资金
- Computational Materials Sciences Program - U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0014607]
- National Science Foundation [OAC 2118061]
Nonadiabatic quantum molecular dynamics is used to investigate the evolution of photoexcited states in GeTe. Results reveal a nonthermal path for the loss of long-range order induced by photoexcitation, which triggers local disorder and promotes the formation of wrong bonds. These findings provide an electronic-structure basis for understanding the ultrafast changes in the structure and properties of GeTe and other phase-change materials induced by photoexcitation.
Nonadiabatic quantum molecular dynamics is used to investigate the evolution of GeTe photoexcited states. Results reveal a photoexcitation-induced picosecond nonthermal path for the loss of long-range order. A valence electron excitation threshold of 4% is found to trigger local disorder by switching Ge atoms from octahedral to tetrahedral sites and promoting Ge-Ge bonding. The resulting loss of long-range order for a higher valence electron excitation fraction is achieved without fulfilling the Lindemann criterion for melting, therefore utilizing a nonthermal path. The photoexcitation-induced structural disorder is accompanied by charge transfer from Te to Ge, Ge-Te bonding-to-antibonding, and Ge-Ge antibonding-to-bonding change, triggering Ge-Te bond breaking and promoting the formation of Ge-Ge wrong bonds. These results provide an electronic-structure basis to understand the photoexcitation-induced ultrafast changes in the structure and properties of GeTe and other phase-change materials.
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