气候变化领域集成服务门户(CCPortal): Structural relaxation and crystallization in supercooled water from 170 to 260 K

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DOI	10.1073/pnas.2022884118
	Structural relaxation and crystallization in supercooled water from 170 to 260 K
	Kringle L.; Thornley W.A.; Kay B.D.; Kimmel G.A.
发表日期	2021
ISSN	00278424
卷号	118 期号:14
英文摘要	The origin of water's anomalous properties has been debated for decades. Resolution of the problem is hindered by a lack of experimental data in a crucial region of temperatures, T, and pressures where supercooled water rapidly crystallizes-a region often referred to as "no man's land." A recently developed technique where water is heated and cooled at rates greater than 109 K/s now enables experiments in this region. Here, it is used to investigate the structural relaxation and crystallization of deeply supercooled water for 170 K < T < 260 K. Water's relaxation toward a new equilibrium structure depends on its initial structure with hyperquenched glassy water (HQW) typically relaxing more quickly than low-density amorphous solid water (LDA). For HQW and T > 230 K, simple exponential relaxation kinetics is observed. For HQW at lower temperatures, increasingly nonexponential relaxation is observed, which is consistent with the dynamics expected on a rough potential energy landscape. For LDA, approximately exponential relaxation is observed for T > 230 K and T < 200 K, with nonexponential relaxation only at intermediate temperatures. At all temperatures, water's structure can be reproduced by a linear combination of two, local structural motifs, and we show that a simple model accounts for the complex kinetics within this context. The relaxation time, τrel, is always shorter than the crystallization time, τxtal. For HQW, the ratio, τxtal/τrel, goes through a minimum at ∼198 K where the ratio is about 60. © 2021 National Academy of Sciences. All rights reserved.
英文关键词	Metastable states; Nonexponentialkinetics; Supercooled water
语种	英语
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/179985
作者单位	Physical Sciences Division, Pacific Northwest National Laboratory, Richland, WA 99352, United States
推荐引用方式 GB/T 7714	Kringle L.,Thornley W.A.,Kay B.D.,et al. Structural relaxation and crystallization in supercooled water from 170 to 260 K[J],2021,118(14).
APA	Kringle L.,Thornley W.A.,Kay B.D.,&Kimmel G.A..(2021).Structural relaxation and crystallization in supercooled water from 170 to 260 K.Proceedings of the National Academy of Sciences of the United States of America,118(14).
MLA	Kringle L.,et al."Structural relaxation and crystallization in supercooled water from 170 to 260 K".Proceedings of the National Academy of Sciences of the United States of America 118.14(2021).