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Unifying the order and disorder dynamics in photoexcited VO(2)
Photoinduced phase transition (PIPT) is always treated as a coherent process, but ultrafast disordering in PIPT is observed in recent experiments. Utilizing the real-time time-dependent density functional theory method, here we track the motion of individual vanadium (V) ions during PIPT in VO(2) an...
Autores principales: | , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
National Academy of Sciences
2022
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9282394/ https://www.ncbi.nlm.nih.gov/pubmed/35867737 http://dx.doi.org/10.1073/pnas.2122534119 |
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author | Liu, Hao-Wen Liu, Wen-Hao Suo, Zhao-Jun Wang, Zhi Luo, Jun-Wei Li, Shu-Shen Wang, Lin-Wang |
author_facet | Liu, Hao-Wen Liu, Wen-Hao Suo, Zhao-Jun Wang, Zhi Luo, Jun-Wei Li, Shu-Shen Wang, Lin-Wang |
author_sort | Liu, Hao-Wen |
collection | PubMed |
description | Photoinduced phase transition (PIPT) is always treated as a coherent process, but ultrafast disordering in PIPT is observed in recent experiments. Utilizing the real-time time-dependent density functional theory method, here we track the motion of individual vanadium (V) ions during PIPT in VO(2) and uncover that their coherent or disordered dynamics can be manipulated by tuning the laser fluence. We find that the photoexcited holes generate a force on each V–V dimer to drive their collective coherent motion, in competing with the thermal-induced vibrations. If the laser fluence is so weak that the photoexcited hole density is too low to drive the phase transition alone, the PIPT is a disordered process due to the interference of thermal phonons. We also reveal that the photoexcited holes populated by the V–V dimerized bonding states will become saturated if the laser fluence is too strong, limiting the timescale of photoinduced phase transition. |
format | Online Article Text |
id | pubmed-9282394 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | National Academy of Sciences |
record_format | MEDLINE/PubMed |
spelling | pubmed-92823942023-01-06 Unifying the order and disorder dynamics in photoexcited VO(2) Liu, Hao-Wen Liu, Wen-Hao Suo, Zhao-Jun Wang, Zhi Luo, Jun-Wei Li, Shu-Shen Wang, Lin-Wang Proc Natl Acad Sci U S A Physical Sciences Photoinduced phase transition (PIPT) is always treated as a coherent process, but ultrafast disordering in PIPT is observed in recent experiments. Utilizing the real-time time-dependent density functional theory method, here we track the motion of individual vanadium (V) ions during PIPT in VO(2) and uncover that their coherent or disordered dynamics can be manipulated by tuning the laser fluence. We find that the photoexcited holes generate a force on each V–V dimer to drive their collective coherent motion, in competing with the thermal-induced vibrations. If the laser fluence is so weak that the photoexcited hole density is too low to drive the phase transition alone, the PIPT is a disordered process due to the interference of thermal phonons. We also reveal that the photoexcited holes populated by the V–V dimerized bonding states will become saturated if the laser fluence is too strong, limiting the timescale of photoinduced phase transition. National Academy of Sciences 2022-07-06 2022-07-12 /pmc/articles/PMC9282394/ /pubmed/35867737 http://dx.doi.org/10.1073/pnas.2122534119 Text en Copyright © 2022 the Author(s). Published by PNAS. https://creativecommons.org/licenses/by-nc-nd/4.0/This article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND) (https://creativecommons.org/licenses/by-nc-nd/4.0/) . |
spellingShingle | Physical Sciences Liu, Hao-Wen Liu, Wen-Hao Suo, Zhao-Jun Wang, Zhi Luo, Jun-Wei Li, Shu-Shen Wang, Lin-Wang Unifying the order and disorder dynamics in photoexcited VO(2) |
title | Unifying the order and disorder dynamics in photoexcited VO(2) |
title_full | Unifying the order and disorder dynamics in photoexcited VO(2) |
title_fullStr | Unifying the order and disorder dynamics in photoexcited VO(2) |
title_full_unstemmed | Unifying the order and disorder dynamics in photoexcited VO(2) |
title_short | Unifying the order and disorder dynamics in photoexcited VO(2) |
title_sort | unifying the order and disorder dynamics in photoexcited vo(2) |
topic | Physical Sciences |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9282394/ https://www.ncbi.nlm.nih.gov/pubmed/35867737 http://dx.doi.org/10.1073/pnas.2122534119 |
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