Reversible disorder-order transitions in atomic crystal nucleation

被引：196

作者：

Jeon, Sungho ^{[1
]}

Heo, Taeyeong ^{[1
]}

Hwang, Sang-Yeon ^{[2
,13
]}

Ciston, Jim ^{[3
]}

Bustillo, Karen C. ^{[3
]}

Reed, Bryan W. ^{[4
]}

Ham, Jimin ^{[1
]}

Kang, Sungsu ^{[5
,6
,7
]}

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

Lim, Joowon ^{[1
]}

Lim, Kitaek ^{[1
]}

Kim, Ji Soo ^{[5
,6
,7
]}

Kang, Min-Ho ^{[5
,6
,7
]}

Bloom, Ruth S. ^{[4
]}

Hong, Sukjoon ^{[1
]}

Kim, Kwanpyo ^{[8
,9
]}

Zettl, Alex ^{[10
,11
,12
]}

Kim, Woo Youn ^{[2
]}

Ercius, Peter ^{[3
]}

Park, Jungwon ^{[5
,6
,7
]}

Lee, Won Chul ^{[1
]}

机构：

[1] Hanyang Univ, BK21 FOUR ERICA ACE Ctr, Dept Mech Engn, Ansan 15588, Gyeonggi, South Korea

[2] Korea Adv Inst Sci & Technol KAIST, Dept Chem, Daejeon 34141, South Korea

[3] Lawrence Berkeley Natl Lab LBNL, Natl Ctr Electron Microscopy, Mol Foundry, Berkeley, CA 94720 USA

[4] Integrated Dynam Electron Solut Inc, Pleasanton, CA 94588 USA

[5] Seoul Natl Univ, Sch Chem & Biol Engn, Seoul 08826, South Korea

[6] Seoul Natl Univ, Inst Chem Proc, Seoul 08826, South Korea

[7] Inst Basic Sci IBS, Ctr Nanoparticle Res, Seoul 08826, South Korea

[8] Yonsei Univ, Dept Phys, Seoul 03722, South Korea

[9] Inst for Basic Sci Korea, Ctr Nanomed, Seoul 03722, South Korea

[10] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA

[11] LBNL, Mat Sci Div, Berkeley, CA 94720 USA

[12] Kavli Energy NanoSci Inst, Berkeley, CA 94720 USA

[13] Samsung Elect, Samsung Adv Inst Technol SAIT, Suwon 16678, South Korea

来源：

SCIENCE | 2021年 / 371卷 / 6528期

基金：

新加坡国家研究基金会; 美国国家科学基金会;

关键词：

GOLD NANOPARTICLES; PARTICLE-SIZE; ELECTRON; GROWTH; CRYSTALLIZATION; NANOCRYSTALS; MECHANISM; CLUSTERS; TEM;

D O I：

10.1126/science.aaz7555

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：

Nucleation in atomic crystallization remains poorly understood, despite advances in classical nucleation theory. The nucleation process has been described to involve a nonclassical mechanism that includes a spontaneous transition from disordered to crystalline states, but a detailed understanding of dynamics requires further investigation. In situ electron microscopy of heterogeneous nucleation of individual gold nanocrystals with millisecond temporal resolution shows that the early stage of atomic crystallization proceeds through dynamic structural fluctuations between disordered and crystalline states, rather than through a single irreversible transition. Our experimental and theoretical analyses support the idea that structural fluctuations originate from size-dependent thermodynamic stability of the two states in atomic dusters. These findings, based on dynamics in a real atomic system, reshape and improve our understanding of nucleation mechanisms in atomic crystallization.

引用

页码：498 / +

页数：75

共 65 条

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