Development of a “First-Principles” Water Potential with Flexible Monomers. III. Liquid Phase Properties

Medders, Gregory R.; Babin, Volodymyr; Paesani, Francesco

doi:10.1021/ct5004115

Cited by 396 publications

(600 citation statements)

References 63 publications

(98 reference statements)

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“…17 In 2015, two new heterodyne-detected experiments with a more careful consideration of the reference used to determine the phase were performed by Yamaguchi, and Tahara and co-workers, which showed, in fact, that for neat H 2 O the low-frequency positive feature was absent 19,20 21 which does essentially confirm the result that there is no positive feature at low frequencies. We note that Nagata and co-workers have recently calculated sum-frequency spectra with ab initio MD simulations, 22 and Medders and Paesani have done the same 23 using their MB-pol model, 24 and the results of both groups are in good agreement with these new experiments.…”

supporting

confidence: 65%

Communication: Vibrational sum-frequency spectrum of the air-water interface, revisited

Skinner

2016

The Journal of Chemical Physics

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supporting

confidence: 65%

Communication: Vibrational sum-frequency spectrum of the air-water interface, revisited

Skinner

2016

The Journal of Chemical Physics

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“…8(b)). It will be very interesting to see how more involved, ab-initio based water models, such as MB-pol, 57 behave in this regard. Another possible extension of this work concerns the possibility that the so-called dynamical transition in proteins is correlated with a crossing of the Widom-line, i.e., that HDL or LDL water affects the dynamics of a protein differently.…”

Section: Discussionmentioning

confidence: 99%

Markov state model of the two-state behaviour of water

Hamm

2016

The Journal of Chemical Physics

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With the help of a Markov State Model (MSM), two-state behaviour is resolved for two computer models of water in a temperature range from 255 K to room temperature (295 K). The method is first validated for ST2 water, for which the so far strongest evidence for a liquid-liquid phase transition exists. In that case, the results from the MSM can be cross-checked against the radial distribution function g(5)(r) of the 5th-closest water molecule around a given reference water molecule. The latter is a commonly used local order parameter, which exhibits a bimodal distribution just above the liquidliquid critical point that represents the low-density form of the liquid (LDL) and the high density liquid. The correlation times and correlation lengths of the corresponding spatial domains are calculated and it is shown that they are connected via a simple diffusion model. Once the approach is established, TIP4P/2005 will be considered, which is the much more realistic representation of real water. The MSM can resolve two-state behavior also in that case, albeit with significantly smaller correlation times and lengths. The population of LDL-like water increases with decreasing temperature, thereby explaining the density maximum at 4 degrees C along the lines of the two-state model of water. Published by AIP Publishing. With the help of a Markov State Model (MSM), two-state behaviour is resolved for two computer models of water in a temperature range from 255 K to room temperature (295 K). The method is first validated for ST2 water, for which the so far strongest evidence for a liquid-liquid phase transition exists. In that case, the results from the MSM can be cross-checked against the radial distribution function g 5 (r) of the 5th-closest water molecule around a given reference water molecule. The latter is a commonly used local order parameter, which exhibits a bimodal distribution just above the liquid-liquid critical point that represents the low-density form of the liquid (LDL) and the high density liquid. The correlation times and correlation lengths of the corresponding spatial domains are calculated and it is shown that they are connected via a simple diffusion model. Once the approach is established, TIP4P/2005 will be considered, which is the much more realistic representation of real water. The MSM can resolve two-state behavior also in that case, albeit with significantly smaller correlation times and lengths. The population of LDL-like water increases with decreasing temperature, thereby explaining the density maximum at 4• C along the lines of the two-state model of water. Published by AIP Publishing. [http://dx

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“…It will be evident already from the discussions in Sec. 3 that these techniques have found widespread use; mainly this is due to the combination of effective algorithms that have reduced their computational cost combined with increases in computational 27 power. In Sec.…”

Section: Methods To Simulate Nuclear Quantum Effectsmentioning

confidence: 99%

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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Development of a “First-Principles” Water Potential with Flexible Monomers. III. Liquid Phase Properties

Cited by 396 publications

References 63 publications

Communication: Vibrational sum-frequency spectrum of the air-water interface, revisited

Communication: Vibrational sum-frequency spectrum of the air-water interface, revisited

Markov state model of the two-state behaviour of water

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

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