Inducing thermodynamically blocked atomic ordering via strongly driven nonequilibrium kinetics

被引：75

作者：

Jung, Chulho ^{[1
,2
]}

Ihm, Yungok ^{[2
,3
]}

Cho, Do Hyung ^{[1
,2
]}

Lee, Heemin ^{[1
,2
]}

Nam, Daewoong ^{[2
,4
]}

Kim, Sangsoo ^{[4
]}

Eom, In-Tae ^{[2
,4
]}

Park, Jaehyun ^{[3
]}

Kim, Chan ^{[5
,6
,7
]}

Kim, Yoonhee ^{[5
,6
,7
]}

Fan, Jiadong ^{[8
]}

Ji, Nianjing ^{[8
]}

Morris, James R. ^{[9
,10
]}

Owada, Shigeki ^{[11
]}

Tono, Kensuke ^{[12
]}

Shim, Ji Hoon ^{[2
,3
]}

Jiang, Huaidong ^{[8
]}

Yabashi, Makina ^{[11
,12
]}

Ishikawa, Tetsuya ^{[11
]}

Noh, Do Young ^{[5
,6
,13
]}

Song, Changyong ^{[1
,2
,14
]}

机构：

[1] POSTECH, Dept Phys, Pohang 37673, South Korea

[2] POSTECH, Photon Sci Ctr, Pohang 37673, South Korea

[3] POSTECH, Dept Chem, Pohang 37673, South Korea

[4] Pohang Accelerator Lab, Pohang 37673, South Korea

[5] Gwangju Inst Sci & Technol, Dept Phys & Photon Sci, Gwangju 61005, South Korea

[6] Gwangju Inst Sci & Technol, Sch Mat Sci & Engn, Gwangju 61005, South Korea

[7] European XFEL GmbH, D-22869 Schenefeld, Germany

[8] ShanghaiTech Univ, Sch Phys Sci, Shanghai, Peoples R China

[9] Oak Ridge Natl Lab, Mat Sci Div, Oak Ridge, TN 37831 USA

[10] Iowa State Univ, Ames Lab, Ames, IA 50011 USA

[11] RIKEN SPring 8 Ctr, 1-1-1 Kouto, Sayo, Hyogo 6795148, Japan

[12] Japan Synchrotron Radiat Res Inst, 1-1-1 Kouto, Sayo, Hyogo 6795198, Japan

[13] Inst Basic Sci IBS, Daejeon 34126, South Korea

[14] POSTECH, Asia Pacific Ctr Theoret Phys, Pohang 37673, South Korea

来源：

SCIENCE ADVANCES | 2021年 / 7卷 / 52期

基金：

中国国家自然科学基金; 新加坡国家研究基金会;

关键词：

SURFACE-INDUCED CRYSTALLIZATION; FREE-ELECTRON LASER; BISMUTH; SHAPE; FEMTOSECOND; DYNAMICS; VISUALIZATION; DISSOLUTION; NUCLEATION; DIFFUSION;

D O I：

10.1126/sciadv.abj8552

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

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.

引用

页数：10

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