Structure and Single Proton Dynamics of Bulk Supercooled Water

Botti, A.; Bruni, Fabio; Ricci, Maria Antonietta; Pietropaolo, A.; Senesi, R.

doi:10.1016/j.molliq.2007.08.017

Cited by 4 publications

(7 citation statements)

References 20 publications

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“…Ring polymer molecular dynamics (RPMD) simply evolves the ring 36 polymer according to the discretized path integral Hamiltonian (9,(219)(220)(221), while centroid molecular dynamics (CMD) approximates the centroid-density dynamics by evolving the center of mass of the ring polymer over the potential of mean force obtained by averaging over the internal fluctuations of the ring polymer(222-224). Both techniques can be shown to yield exact quantum dynamics in some simple limiting cases, and some progress has been made towards giving formal justification to their use (217,225,226).…”

Section: Simulating Quantum Dynamical Propertiesmentioning

confidence: 99%

“…These algorithmic advances have allowed simulations of liquid water with NQEs to be performed where the molecular interactions are computed using on-the-fly electronic structure calculations (5,(17)(18)(19)(20)(21)(22) and on potential energy surfaces fit to high-level ab initio calculations (23)(24)(25)(26)(27). In addition, experimental techniques such as deep inelastic neutron scattering (DINS) are now able to probe the proton and oxygen momentum distributions and quantum kinetic energies, providing intriguing new observations of these quantum properties of the nuclei at thermodynamic conditions ranging from supercooled to supercritical water, and environments ranging from the bulk to hydrophobic confinement (26,(28)(29)(30)(31)(32)(33)(34)(35)(36)(37)(38)(39)(40)(41)(42).…”

Section: Introductionmentioning

confidence: 99%

“…This theoretical picture has been coupled with new algorithms that have greatly reduced the cost of performing simulations that include NQEs, in some cases yielding schemes with costs comparable to those of the corresponding classical simulations. − These algorithmic advances have allowed simulations of liquid water with NQEs to be performed where the molecular interactions are computed using on-the-fly electronic structure calculations ,− and on potential energy surfaces fitted to high-level ab initio calculations. − In addition, experimental techniques such as deep inelastic neutron scattering (DINS) are now able to probe the proton and oxygen momentum distributions and quantum kinetic energies, providing intriguing new observations of these quantum properties of the nuclei under thermodynamic conditions ranging from supercooled to supercritical water and environments ranging from the bulk to hydrophobic confinement. ,− …”

Section: Introductionmentioning

confidence: 99%

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Nuclear Quantum Effects in Water and Aqueous Systems: Experiment, Theory, and Current Challenges

et al. 2016

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Nuclear quantum effects influence the structure and dynamics of hydrogen bonded systems, such as water, which impacts their observed properties with widely varying magnitudes. This review highlights the recent significant developments in the experiment, theory and simulation of nuclear quantum effects in water. Novel experimental techniques, such as deep inelastic neutron scattering, now provide a detailed view of the role of nuclear quantum effects in water's 2 properties. These have been combined with theoretical developments such as the introduction of the competing quantum effects principle that allows the subtle interplay of water's quantum effects and their manifestation in experimental observables to be explained. We discuss how this principle has recently been used to explain the apparent dichotomy in water's isotope effects, which can range from very large to almost nonexistent depending on the property and conditions. We then review the latest major developments in simulation algorithms and theory that have enabled the efficient inclusion of nuclear quantum effects in molecular simulations, permitting their combination with on-the-fly evaluation of the potential energy surface using electronic structure theory. Finally, we identify current challenges and future opportunities in the area.3

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Section: Simulating Quantum Dynamical Propertiesmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Nuclear Quantum Effects in Water and Aqueous Systems: Experiment, Theory, and Current Challenges

et al. 2016

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“…As a consequence of their directionality, the hydrogen bonds induce a rearrangement of the molecules in an open network (tetrahedral in 3D), in contrast with the more dense arrangement that can be observed at higher T or higher P [37]. This effect can be included in the model by associating a small volume contribution v HB , due to the formation of each bond, to the total volume of the system…”

Section: General Definition Of the Modelmentioning

confidence: 99%

Dynamically Slow Processes in Supercooled Water Confined Between Hydrophobic Plates

Franzese,

Santos

2009

Preprint

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We study the dynamics of water confined between hydrophobic flat surfaces at low temperature. At different pressures, we observe different behaviors that we understand in terms of the hydrogen bonds dynamics. At high pressure, the formation of the open structure of the hydrogen bond network is inhibited and the surfaces can be rapidly dehydrated by decreasing the temperature. At lower pressure the rapid ordering of the hydrogen bonds generates heterogeneities that are responsible for strong non-exponential behavior of the correlation function, but with no strong increase of the correlation time. At very low pressures, the gradual formation of the hydrogen bond network is responsible for the large increase of the correlation time and, eventually, the dynamical arrest of the system and of the dehydration process.

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“…There is currently great interest in probing the structure and dynamics of water, [1][2][3][4][5][6][7][8] largely motivated by the wide range of technological applications and biological importance of this fluid. Most recently particular attention has been devoted to theoretical [9][10][11][12][13] and experimental studies of the structure and dynamics of water confined in nanopores.…”

Section: Introductionmentioning

confidence: 99%

Interaction of single water molecules with silanols in mesoporous silica

Pantalei

Senesi

Sozzani

et al. 2011

Phys. Chem. Chem. Phys.

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Deep Inelastic Neutron Scattering measurements of water confined in mesoporous silica have been carried out. The experiment has been performed at room temperature on dry and on hydrated samples in order to investigate the interaction between the protons and the silanol groups of the confining surface. With this aim we could control the hydration of the pores in such a way as to adsorb 3.0 water molecules per nm(2), corresponding to a 1 to 1 ratio with the silanol groups of the surface. DINS measurements directly measure the mean kinetic energy and the momentum distribution of the protons. A detailed analysis of the hydrated sample has been performed in order to separate the contributions of the protons in the system, allowing us to determine the arrangement of water molecules on the silanol groups. We find that the hydrogen bond of the water proton with the oxygen of the silanol group is much stronger than the hydrogen bonds of bulk water.

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Structure and Single Proton Dynamics of Bulk Supercooled Water

Cited by 4 publications

References 20 publications

Nuclear Quantum Effects in Water and Aqueous Systems: Experiment, Theory, and Current Challenges

Nuclear Quantum Effects in Water and Aqueous Systems: Experiment, Theory, and Current Challenges

Dynamically Slow Processes in Supercooled Water Confined Between Hydrophobic Plates

Interaction of single water molecules with silanols in mesoporous silica

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