Abstract
Using extensive molecular dynamics simulations combined with a novel approach to analyze the molecular displacements we analyzed the change in the dynamics above and below the crossover temperature Tx for supercooled water. Our findings suggest that the crossover from fragile to strong glass former occurring at Tx is related with a change in the diffusion mechanism evidencing the presence of jump-like diffusion at lower temperatures. Also we observe that fluctuations of the local environments are intimately connected with fluctuations in the size and the amount of cooperative cluster of mobile molecules, and in particular we find a highly cooperative nature of the motion at low temperatures.
References
55
Referenced
11
10.1038/24540
/ Nature (London) (1998)10.1146/annurev.pc.34.100183.003113
/ Annu. Rev. Phys. Chem. (1983)10.1063/1.433153
/ J. Chem. Phys. (1976)10.1088/0953-8984/15/45/R01
/ J. Phys.: Condens. Matter (2003)10.1073/pnas.1015340107
/ Proc. Natl. Acad. Sci. U.S.A. (2010)10.1063/1.1832595
/ J. Chem. Phys. (2004)10.1063/1.2193159
/ J. Chem. Phys. (2006)10.1103/PhysRevLett.95.117802
/ Phys. Rev. Lett. (2005)10.1126/science.267.5206.1924
/ Science (1995)10.1021/cr000689q
/ Chem. Rev. (2002)10.1016/S0140-7007(00)00027-X
/ Int. J. Refrig. (2001)10.1088/0953-8984/21/50/504102
/ J. Phys.: Condens. Matter (2009)10.1140/epje/i2011-11094-7
/ Eur. Phys. J. E (2011)10.1063/1.4795539
/ J. Chem. Phys. (2013)10.1073/pnas.0507870102
/ Proc. Natl. Acad. Sci. U.S.A. (2005)10.1063/1.3229892
/ J. Chem. Phys. (2009)10.1063/1.3506860
/ J. Chem. Phys. (2010)10.1063/1.3585676
/ J. Chem. Phys. (2011)10.1088/0953-8984/24/6/064109
/ J. Phys.: Condens. Matter (2012)10.1021/jz9003125
/ J. Phys. Chem. Lett. (2010)10.1073/pnas.0702608104
/ Proc. Natl. Acad. Sci. U.S.A. (2007)10.1063/1.4759262
/ J. Chem. Phys. (2012)10.1038/416409a
/ Nature (London) (2002)10.1021/ja0211252
/ J. Am. Chem. Soc. (2003)10.1073/pnas.1221805110
/ Proc. Natl. Acad. Sci. U.S.A. (2013)10.1063/1.3697841
/ J. Chem. Phys. (2012)10.1063/1.3690497
/ J. Chem. Phys. (2012)10.1063/1.3643333
/ J. Chem. Phys. (2011)10.1063/1.4737907
/ J. Chem. Phys. (2012)10.1103/PhysRevA.31.1913
/ Phys. Rev. A (1985)10.1021/jp984075p
/ J. Phys. Chem. B (1999)10.1063/1.3578472
/ J. Chem. Phys. (2011)10.1063/1.1652434
/ J. Chem. Phys. (2004)10.1146/annurev.physchem.51.1.99
/ Ann. Rev. Phys. Chem. (2000)10.1002/jcc.20291
/ J. Comput. Chem. (2005)10.1063/1.2183308
/ J. Chem. Phys. (2006)10.1016/j.cplett.2012.04.022
/ Chem. Phys. Lett. (2012)10.1063/1.1683075
/ J. Chem. Phys. (2004)10.1039/c1cp22168j
/ Phys. Chem. Chem. Phys. (2011)10.1080/00268970500243796
/ Mol. Phys. (2005)10.1063/1.4812928
/ J. Chem. Phys. (2013)10.1016/S0301-0104(02)00667-5
/ Chem. Phys. (2002)10.1103/PhysRevLett.80.4915
/ Phys. Rev. Lett. (1998)10.1103/PhysRevLett.76.2730
/ Phys. Rev. Lett. (1996)10.1103/PhysRevE.62.579
/ Phys. Rev. E (2000)10.1038/379055a0
/ Nature (London) (1996)10.1103/PhysRevLett.80.2338
/ Phys. Rev. Lett. (1998)10.1002/j.1538-7305.1948.tb01338.x
/ Bell Syst. Tech. J. (1948)10.1523/JNEUROSCI.4714-06.2007
/ J. Neurosci. (2007)10.1063/1.1696442
/ J. Chem. Phys. (1965)10.1103/PhysRevE.60.3107
/ Phys. Rev. E (1999)10.1209/0295-5075/88/16003
/ Europhys. Lett. (2009)10.1088/0034-4885/55/3/001
/ Rep. Prog. Phys. (1992)10.1088/0953-8984/21/50/504101
/ J. Phys.: Condens. Matter (2009)10.1103/PhysRevE.78.041501
/ Phys. Rev. E (2008)
Dates
Type | When |
---|---|
Created | 12 years ago (July 30, 2013, 6:25 p.m.) |
Deposited | 2 years, 2 months ago (June 19, 2023, 1:33 p.m.) |
Indexed | 3 weeks, 5 days ago (July 30, 2025, 7:01 a.m.) |
Issued | 12 years ago (July 28, 2013) |
Published | 12 years ago (July 28, 2013) |
Published Online | 12 years ago (July 30, 2013) |
Published Print | 12 years ago (July 28, 2013) |
@article{Picasso_2013, title={Cooperative dynamic and diffusion behavior above and below the dynamical crossover of supercooled water}, volume={139}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.4816523}, DOI={10.1063/1.4816523}, number={4}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Picasso, Germán C. and Malaspina, David C. and Carignano, Marcelo A. and Szleifer, Igal}, year={2013}, month=jul }