The puzzling unsolved mysteries of liquid water: Some recent progress

Stanley, H. Eugene; Kumar, Pradeep; Xu, Limei; Yan, Zhen; Mazza, Marco G.; Buldyrev, Sergey V.; Chen, S.-H.; Mallamace, Francesco

doi:10.1016/j.physa.2007.07.044

Cited by 75 publications

(58 citation statements)

References 96 publications

Supporting

Mentioning

Contrasting

Unclassified

Order By: Relevance

“…A complete knowledge of the behavior of water at interfaces and under nanoconfinement is expected to open new roads of both academic and technological relevance in fields ranging from biology to materials science A c c e p t e d M a n u s c r i p t [1,2,3,4,5,6,7,8,9,10,11,12]. Both in biological organization and in the supramolecular self-assembly of materials, the nanoconfinement that arises upon the interaction of the different assembling units affects the thermodynamic properties of the hydration water, which usually must be removed for the process to take place [7].…”

Section: Introductionmentioning

confidence: 99%

Hydrophobicity and geometry: Water at curved graphitic-like surfaces and within model pores in self-assembled monolayers

Alarcón

Accordino

et al. 2014

Fluid Phase Equilibria

View full text Add to dashboard Cite

Section: Introductionmentioning

confidence: 99%

Hydrophobicity and geometry: Water at curved graphitic-like surfaces and within model pores in self-assembled monolayers

Alarcón

Accordino

et al. 2014

Fluid Phase Equilibria

View full text Add to dashboard Cite

“…4 in Ref. [26]), the exact boundary location between LDL and HDL is not well-defined as well as the smoothed LDL/HDL transformations range are still undetected. So, the problem associated with the structural transformation and its influence on microscopic dynamics of liquid water (even at the room temperature) requires the additional studies [15].…”

Section: Introductionmentioning

confidence: 99%

Vibrational features of water at the low-density/high-density liquid structural transformations

Khusnutdinoff

Мокшин

2012

Physica A: Statistical Mechanics and its Applications

View full text Add to dashboard Cite

A structural transformation in water upon compression was recently observed at the temperature T = 277 K in the vicinity of the pressure p ≈ 2 000 Atm [R.M. Khusnutdinoff, A.V. Mokshin, J. Non-Cryst. Solids 357, 1677 (2011)]. It was found that the transformations are related with the principal structural changes within the first two coordination shells as well as the deformation of the hydrogen-bond network. In this work we study in details the influence of these structural transformations on the vibrational molecular dynamics of water by means of molecular dynamics simulations on the basis of the model Amoeba potential (T = 290 K, p = 1.0 ÷ 10 000 Atm). The equation of state and the isothermal compressibility are found for the considered (p,T )-range. The vibrational density of states extracted for T Hz-frequency range manifests the two distinct modes, where the high-frequency mode is independent on pressure whereas the low-frequency one has the strong, non-monotonic pressure-dependence and exhibits a step-like behavior at the pressure p ≈ 2000 Atm. The extended analysis of the local structural and vibrational properties discovers that there is a strong correlation between the primary structural and vibrational aspects of the liquid-liquid structural transformation related with the molecular rearrangement within the range of the second coordination shell.

show abstract

“…The theory also requires the liquid state counterparts of HDA and LDA ice (46)(47)(48). Based on the LL critical theory, the observed protein dynamical transition at cryogenic temperatures might be related to the two proposed liquid forms of water (highdensity liquid and low-density liquid) existing well below the homogeneous nucleation temperature of water (35,(46)(47)(48)(49). It remains to be seen how the cryogenic protein dynamical transition is related to the conventional protein dynamical transition at around 200 K, which is thought to be a precondition for a biologically active state of proteins.…”

Section: Discussionmentioning

confidence: 99%

Protein dynamical transition at 110 K

Kim

Täte

Grüner

2011

Proc. Natl. Acad. Sci. U.S.A.

View full text Add to dashboard Cite

Proteins are known to undergo a dynamical transition at around 200 K but the underlying mechanism, physical origin, and relationship to water are controversial. Here we report an observation of a protein dynamical transition as low as 110 K. This unexpected protein dynamical transition precisely correlated with the cryogenic phase transition of water from a high-density amorphous to a low-density amorphous state. The results suggest that the cryogenic protein dynamical transition might be directly related to the two liquid forms of water proposed at cryogenic temperatures.conformation fluctuations | water phase transition | high-pressure cryocooling | X-ray crystallography I t is known that a hydrated protein undergoes a dynamical transition at around 200 K (1). Proteins below the transition temperature are in a glassy state with little conformational flexibility and no appreciable biological function; above the transition temperature flexibility is restored and the protein becomes biologically active (2-4). This protein dynamical transition has been extensively studied by measuring the mean square atomic displacement, hx 2 i, of protein atoms as a function of temperature with various methods, including Mössbauer and terahertz time domain spectroscopies (5-7), X-ray crystallography (4, 8-11), neutron scattering (2,(12)(13)(14)(15)(16)(17)(18)(19), and molecular dynamics simulations (20)(21)(22)(23)(24)(25).It is believed that the protein dynamical transition involves a strong coupling to the hydration water (10,26,27), as a protein dehydrated below a critical level (water/protein mass ratio of ∼0.2) does not show the dynamical transition (13,14,28). Several mechanisms have been proposed to explain the microscopic origin of protein dynamical transition, including α and β fluctuations in the bulk solvent and the hydration shell (29, 30), liquid-glass transition of hydration water (31), a frequency window scenario (32, 33), and a fragile to strong transition of the hydration water (15,20).In this work, we studied a protein dynamical transition inside protein crystals using a high-pressure cryocooling method (34) and temperature-dependent X-ray diffraction (8,35,36). Protein crystals contain large amounts of water in solvent channels between the proteins in the crystal lattice; water fractions of greater than 50% are very common. It has been reported that this intracrystalline water can be cryocooled under high pressure into a high-density amorphous (HDA) state that subsequently transforms upon heating to the low-density amorphous (LDA) (36) water typical of ambient-pressure flash-cooling [in bulk water the respective densities of HDA and LDA are 1.17 and 0.94 g cm −3 at 77 K and 0.1 MPa. (37, 38)]. In this study, the temperature of the HDA-LDA transition was adjusted by controlling solvent conditions inside the protein crystals. X-ray diffraction data from five thaumatin crystals were used for this study, including four high-pressure cryocooled crystals (Thau-0M-1, Thau-0M-2, Thau-0.45M, Thau-0.9M; 0.9M indicates w...

show abstract

The puzzling unsolved mysteries of liquid water: Some recent progress

Cited by 75 publications

References 96 publications

Hydrophobicity and geometry: Water at curved graphitic-like surfaces and within model pores in self-assembled monolayers

Hydrophobicity and geometry: Water at curved graphitic-like surfaces and within model pores in self-assembled monolayers

Vibrational features of water at the low-density/high-density liquid structural transformations

Protein dynamical transition at 110 K

Contact Info

Product

Resources

About