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The Phase Behavior of Deeply Supercooled Water: a Computational Perspective

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The physical properties of supercooled water have been a source of continued interest since the pioneering work of Speedy and Angell, who reported sharp increases in the response functions upon isobaric cooling [1]. One intriguing hypothesis that has been formulated to explain this behavior is the existence of a metastable liquid-liquid transition at deeply supercooled conditions [2]. The preponderance of experimental evidence is consistent with this hypothesis (e.g., [3], [4]), although no definitive proof exists to date. Computational studies have played an important role in this area [2], [5]-[13]. State-of-the-art free energy techniques provide clear evidence of a liquid-liquid transition in the ST2 model [14] of water [15], including the identification of three phases at the same, deeply supercooled thermodynamic conditions: two metastable liquids in equilibrium, and a stable crystal [15]. Recent calculations on tunable tetrahedral models support this key conclusion of the free energy results [16], [17]. A necessary condition for the existence of a phase transition between two supercooled phases is a wide separation of time scales between nucleation and structural relaxation. Understanding what aspects of intermolecular force fields give rise to this separation of time scales is an important open question.

References [1] Speedy, R.J., Angell, C.A. J. Chem. Phys., 65, 851 (1976). [2] Poole, P.H., Sciortino, F., Essmann, U., Stanley, H.E. Nature, 360, 324 (1992). [3] Mishima, O., Stanley, H.E. Nature, 392, 164 (1998). [4] Amann-Winkel, K., Gainaru, C., Handler, P.H., Seidl, M., Nelson, H., Böhmer, R., Loerting, T. PNAS , 110, 17720 (2013). [5] Liu, Y., Panagiotopoulos, A.Z., Debenedetti, P.G. J. Chem. Phys., 131, 104508 (2009). [6] Moore, E.B., Molinero, V. Nature, 479, 506 (2011). [7] Limmer, D.T., Chandler, D. J. Chem. Phys., 135, 134503 (2011). [8] Liu, Y., Palmer, J.C., Panagiotopoulos, A.Z., Debenedetti, P.G., J. Chem. Phys., 137, 214505 (2012). [9] Poole, P.H., Bowles, R.K., Saika-Voivod, I., Sciortino, F. J. Chem. Phys., 138, 034505 (2013). [10] Overduin, S.D., Patey, G.N. J. Chem. Phys., 138, 184502 (2013). [11] Limmer, D.T., Chandler, D. J. Chem. Phys., 138, 214504 (2013). [12] Kesselring, T.A., Lascaris, E., Franzese, G., Buldyrev, S.V., Stanley, H.E. J. Chem. Phys., 138, 244506 (2013). [13] Li, Y.P., Li, J.C., Wang, F. PNAS , 110, 12209 (2013). [14] Stillinger, F.H., Rahman, A. J. Chem. Phys., 60, 1545 (1974). [15] Palmer, J.C., Martelli, F., Liu, Y., Car, R., Panagiotopoulos, A.Z., Debenedetti, P.G. Nature, 510, 385 (2014). [16] Smallenburg, F., Fillon, L., Sciortino, F. Nature Phys., 10, 653 (2014). [17] Smallenburg, F., Sciortino, F. Phys. Rev. Lett., 115, 015701 (2015).

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