Inducing thermodynamically blocked atomic ordering via strongly driven nonequilibrium kinetics
Date
2021-12-22
Authors
Jung, Chulho
Ihm, Yungok
Cho, Do Hyung
Lee, Heemin
Nam, Daewoong
Kim, Sangsoo
Eom, In-Tae
Park, Jaehyun
Kim, Chan
Kim, Yoonhee
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Iowa State University Digital Repository, Ames IA (United States)
Abstract
Ultrafast light-matter interactions enable inducing exotic material phases by promoting access to kinetic processes blocked in equilibrium. Despite potential opportunities, actively using nonequilibrium kinetics for material discovery is limited by the poor understanding on intermediate states of driven systems. Here, using single-pulse time-resolved imaging with x-ray free-electron lasers, we found intermediate states of photoexcited bismuth nanoparticles that showed kinetically reversed surface ordering during ultrafast melting. This entropy-lowering reaction was further investigated by molecular dynamics simulations to reveal that observed kinetics were thermodynamically buried in equilibrium, which emphasized the critical role of electron-mediated ultrafast free-energy modification in inducing exotic material phases. This study demonstrated that ultrafast photoexcitations of electrons provide an efficient strategy to induce hidden material phases by overcoming thermodynamic barriers via nonequilibrium reaction pathways.
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IS-J 10678
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article
Comments
This article is published as Jung, Chulho, Yungok Ihm, Do Hyung Cho, Heemin Lee, Daewoong Nam, Sangsoo Kim, In-Tae Eom et al. "Inducing thermodynamically blocked atomic ordering via strongly driven nonequilibrium kinetics." Science Advances 7, no. 52 (2021): eabj8552.
DOI: 10.1126/sciadv.abj8552.
Copyright 2021 The Authors.
Attribution 4.0 International (CC BY 4.0).
DOE Contract Number(s): AC05-00OR22725; AC02-07CH11358.
Posted with permission.