Properties of water have been well elucidated for temperatures above ∼230 K and yet mysteries remain in the deeply supercooled region. By performing extensive molecular dynamics simulations on this supercooled region, we find that structural and dynamical instabilities are hidden in the experimentally inaccessible region between 235 K and 150 K. We find a hitherto undiscovered fragmentation from 220 K to 190 K, which is the breakup of large clusters consisting of molecules with a locally distorted tetrahedral structure into small pieces with one or two isolated defects. The fragmentation leads to considerable changes in the relaxation dynamics of water. We reveal a crucial role of specific three-coordinated defects in slow but persistent structural relaxation. The presence of relaxation due to these specific defects makes the water glass transition temperature Tg (=136 K) extremely low and explains why the Tg of water is ∼1/2 of the melting temperature Tm, much lower than the commonly obeyed 2/3 rule of Tg/Tm.
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28 September 2018
Research Article|
September 25 2018
Crucial role of fragmented and isolated defects in persistent relaxation of deeply supercooled water
Shinji Saito
;
Shinji Saito
a)
1
Institute for Molecular Science
, Myodaiji, Okazaki, Aichi 444-8585, Japan
and The Graduate University for Advanced Studies
, Myodaiji, Okazaki, Aichi 444-8585, Japan
a)Authors to whom correspondence should be addressed: shinji@ims.ac.jp; profbiman@gmail.com; and ohmine@ims.ac.jp
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Biman Bagchi
;
Biman Bagchi
a)
2
Indian Institute of Science
, Bangalore 560012, India
a)Authors to whom correspondence should be addressed: shinji@ims.ac.jp; profbiman@gmail.com; and ohmine@ims.ac.jp
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Iwao Ohmine
Iwao Ohmine
a)
1
Institute for Molecular Science
, Myodaiji, Okazaki, Aichi 444-8585, Japan
and The Graduate University for Advanced Studies
, Myodaiji, Okazaki, Aichi 444-8585, Japan
a)Authors to whom correspondence should be addressed: shinji@ims.ac.jp; profbiman@gmail.com; and ohmine@ims.ac.jp
Search for other works by this author on:
a)Authors to whom correspondence should be addressed: shinji@ims.ac.jp; profbiman@gmail.com; and ohmine@ims.ac.jp
J. Chem. Phys. 149, 124504 (2018)
Article history
Received:
June 13 2018
Accepted:
September 10 2018
Citation
Shinji Saito, Biman Bagchi, Iwao Ohmine; Crucial role of fragmented and isolated defects in persistent relaxation of deeply supercooled water. J. Chem. Phys. 28 September 2018; 149 (12): 124504. https://doi.org/10.1063/1.5044458
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