The supercooled state of bulk water is largely hidden by unavoidable crystallization, which creates an experimentally inaccessible temperature regime - a 'no man's land'. We address this and circumvent the crystallization problem by systematically studying the supercooled dynamics of hydrogen bonded oligomeric liquids (glycols), where water corresponds to the chain-ends alone. This novel approach permits a 'dilution of water' by altering the hydrogen bond concentration via variations in chain length. We observe a dynamic crossover in the temperature dependence of the structural relaxation time for all glycols, consistent with the common behavior of most supercooled liquids. We find that the crossover becomes more pronounced for increasing hydrogen bond concentrations, which leads to the prediction of a marked dynamic transition for water within 'no man's land' at T~220 K. Interestingly, the predicted transition thus takes place at a temperature where a so called 'strong-fragile' transition has previously been suggested. Our results, however, imply that the dynamic transition of supercooled water is analogous to that commonly observed in supercooled liquids. Moreover, we find support also for the existence of a secondary relaxation of water with behavior analogous to that of the secondary relaxation observed for the glycols.
A direct measure of hydrogen bonding in water under conditions ranging from the normal state to the supercritical regime is derived from the Compton scattering of inelastically-scattered X-rays. First, we show that a measure of the number of electrons $n_e$ involved in hydrogen bonding at varying thermodynamic conditions can be directly obtained from Compton profile differences. Then, we use first-principles simulations to provide a connection between $n_e$ and the number of hydrogen bonds $n_{HB}$. Our study shows that over the broad range studied the relationship between $n_e$ and $n_{HB}$ i…
Dielectric loss spectra covering 13 decades in frequency were collected for 2-ethyl-1-hexanol, a monohydroxy alcohol that exhibits a prominent Debye-like relaxation, typical for several classes of hydrogen-bonded liquids. The thermal variation of the dielectric absorption amplitude agrees well with that of the hydrogen-bond equilibrium population, experimentally mapped out using near infrared (NIR) and nuclear magnetic resonance (NMR) measurements. Despite this agreement, temperature-jump NIR spectroscopy reveals that the hydrogen-bond switching rate does not define the frequency position of t…
Numerical simulations for a number of water models have supported the possibility of a metastable liquid-liquid critical point (LLCP) in the deep super-cooled region. Here we consider a theoretical model for a supercooled liquid water monolayer and its mathematical mapping onto a percolation problem. The mapping allows us to identify the finite-size clusters at any state-point, and the infinite cluster at the critical point, with the regions of correlated hydrogen bonds (HBs). We show that the percolation line coincides with the first-order liquid-liquid phase transition ending at the LLCP. At…
We report a quantitative experimental study of the crystallization kinetics of supercooled quantum liquid mixtures of para-hydrogen (pH$_2$) and ortho-deuterium (oD$_2$) by high spatial resolution Raman spectroscopy of liquid microjets. We show that in a wide range of compositions the crystallization rate of the isotopic mixtures is significantly reduced with respect to that of the pure substances. To clarify this behavior we have performed path-integral simulations of the non-equilibrium pH$_2$-oD$_2$ liquid mixtures, revealing that differences in quantum delocalization between the two isotop…
A square-lattice model for the formation of secondary structures in proteins, the hydrogen-bonding model, extended to include the effects of solvent quality, is examined in the framework of the Bethe approximation.
A two-dimensional square-lattice model for the formation of secondary structures in proteins, the hydrogen-bonding model, is extended to include the effects of solvent quality. This is achieved by allowing configuration-dependent nearest-neighbour interactions. The phase diagram is presented, and found to have a much richer variety of phases than either the pure hydrogen-bonding self-avoiding walk model or the standard $Θ$-point model.
The slow dynamics of glass-forming liquids is generally ascribed to the cage-jump motion. In the cage-jump picture, a molecule remains in a cage formed by neighboring molecules, and after a sufficiently long time, it jumps to escape from the original position by cage-breaking. The clarification of the cage-jump motion is therefore linked to unraveling the fundamental element of the slow dynamics. Here, we develop a cage-jump model for the dynamics of supercooled water. The caged and jumping states of a water molecule are introduced with respect to the hydrogen-bond (H-bond) rearrangement proce…
Hydrogen bonding plays a role in the microphase separation behavior of many block copolymers, such as those used in lithography, where the stronger interactions due to H-bonding can lead to a smaller period for the self-assembled structures, allowing the production of higher resolution templates. However, current statistical thermodynamic models used in descriptions of microphase separation, such as the Flory-Huggins approach, do not take into account some important properties of hydrogen bonding, such as site specificity and cooperativity. In this combined theoretical and experimental study, …
The shear-jamming of dense suspensions can be strongly affected by molecular-scale interactions between particles, e.g. by chemically controlling their propensity for hydrogen bonding. However, hydrogen bonding not only enhances interparticle friction, a critical parameter for shear jamming, but also introduces (reversible) adhesion, whose interplay with friction in shear-jamming systems has so far remained unclear. Here, we present atomic force microscopy studies to assess interparticle adhesion, its relationship to friction, and how these attributes are influenced by urea, a molecule that in…
Hydrogen bonding is a phenomenon of paramount importance in room-temperature ionic liquids. The presence or absence of the hydrogen bond drastically alternates self-diffusion, shear viscosity, phase transition points, and other key properties of a pure substance. For certain applications, the presence of cation-anion hydrogen bonding is undesirable. In the present paper, we investigate perspectives of removing the hydrogen...fluorine interionic attraction in the imidazolium borates, the strongest non-covalent interaction in this type of system. Chemical modification of the tetrafluoroborate an…
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 tim…
Hydrogen bonding liquids, typically water and alcohols, are known to form labile structures (network, chains, etc...), hence the lifetime of such structures is an important microscopic parameter, which can be calculated in computer simulations. Since these cluster entities are mostly statistical in nature, one would expect that, in the short time regime, their lifetime distribution would be a broad Gaussian-like function of time, with a single maximum representing their mean lifetime, and weakly dependent on criteria such as the bonding distance and angle, much similarly to non-hydrogen bondin…
Electric-field control of hydrogen bonding via interfacial charge at atomic resolution
University of Arizona（亚利桑那大学）；City University of Hong Kong（香港城市大学）；Jiangsu University（江苏大学）；Suzhou Laboratory（苏州实验室）；Hong Kong Institute for Clean Energy, City University of Hong Kong（香港城市大学香港清洁能源研究所）
One of the hallmarks of molecular dynamics in deeply supercooled liquids is the non-exponential character of the relaxation functions. It has been a long standing issue if 'universal' features govern the lineshape of glassy dynamics independent of any particular molecular structure or interaction. In the paper, we elucidate this matter by giving a comprehensive comparison of the spectral shape of depolarized light scattering and dielectric data of deeply supercooled liquids. The light scattering spectra of very different systems, e.g. hydrogen bonding and van der Waals liquids but also ionic s…
The hydrogen-bonding interpolymer complexation between poly(acrylic acid) (PAA) and the poly(N,N-dimethylacrylamide) (PDMAM) side chains of the negatively charged graft copolymer poly(acrylic acid-co-2-acrylamido-2-methyl-1-propane sulfonic acid)-graft-poly(N, N dimethylacrylamide) (P(AA-co-AMPSA)-g-PDMAM), containing 48 wt % of PDMAM, and shortly designated as G48, has been studied by small-angle neutron scattering in aqueous solution. Complexation occurs at low pH (pH < 3.75), resulting in the formation of negatively charged colloidal particles, consisting of PAA/PDMAM hydrogen-bonding inter…
We present results for a lattice model of bio-polymers where the type of $β$-sheet formation can be controlled by different types of hydrogen bonds depending on the relative orientation of close segments of the polymer. Tuning these different interaction strengths leads to low-temperature structures with different types of orientational order. We perform simulations of this model and so present the phase diagram, ascertaining the nature of the phases and the order of the transitions between these phases.
Supercooled water exhibits remarkably slow dynamics similar to the behavior observed for various glass-forming liquids. The local order of tetrahedral structures due to hydrogen-bonds (H-bonds) increases with decreasing temperature. Thus, it is important to clarify the temperature dependence of the H-bond breakage process. This was investigated here using molecular dynamics simulations of TIP4P supercooled water. The two-dimensional (2D) potential of mean force (PMF) is presented using combinations of intermolecular distance and angle between two water molecules. The saddle point of the 2D PMF…
Urea denatures proteins due to its strong tendency to dehydrate the first solvation shell via urea-residue preferential binding. However, even after extensive experimental and computational investigations, the influence of urea on the stability of secondary structures remains elusive. For example, contrary to the common understanding, experimental studies have indicated that specific polypeptides, such as poly-alanine or alanine-rich systems, may even show an improved tendency to form secondary structures in aqueous urea. We investigate this seemingly counter-intuitive behaviour using over 15$…
Extensive molecular dynamics computer simulations have been conducted for ethanol-water liquid mixtures in the water-rich side of the composition range, with 10, 20 and 30 mol % of the alcohol, at temperatures between room temperature and the experimental freezing point of the given mixture. All-atom type (OPLS) interatomic potentials have been assumed for ethanol, in combination with two kinds of rigid water models (SPC/E and TIP4P/2005). Both combinations have provided excellent reproductions of the experimental X-ray total structure factors at each temperature; this provided a strong basis …
We numerically investigate the metastable equilibrium structure of deep supercooled and glassy water under pressure, covering the range of densities corresponding to the experimentally produced high-density and very-high-density amorphous phases. At $T = 188$ K, a continuous increase in density is observed on varying pressure from $2.5$ to $13$ kbar, with no signs of first-order transitions. Exploiting a recently proposed approach to the analysis of the radial distribution function -- based on topological properties of the hydrogen-bond network -- we are able to identify well-defined local geo…
Monte Carlo computer simulations in the canonical and grand canonical statistical ensemble were used to explore the properties of the central force (CF1) water model. The intramolecular structure of the H$_2$O molecule is well reproduced by the model. Emphasis was made on hydrogen bonding, and on the tehrahedral, $q$, and translational, $τ$, order parameters. An energetic definition of the hydrogen bond gives more consistent results for the average number of hydrogen bonds compared to the one-parameter distance criterion. At 300 K, an average value of 3.8 was obtained. The $q$ and $τ$ metrics …
The local intermolecular structure and related dynamics in the liquid cis-trans N-methylformamide mixture at ambient temperature and density conditions have been systematically studied by employing Born-Oppenheimer molecular dynamics simulation techniques. Particular attention has been paid to the local structure around the cis- and trans- conformers and the formation and dynamics of hydrogen bonds with their closest neighbors. The calculated atom-atom radial distribution functions are in very good agreement with available experimental data and reveal the existence of different types of hydrog…
The interactions of a hydrophilic surface with water can significantly influence the characteristics of the liquid water interface. In this manuscript, we explore this influence by studying the molecular structure of liquid water at a disordered surface with tunable surface-water interactions. We combine all-atom molecular dynamics simulations with a mean field model of interfacial hydrogen bonding to analyze the effect of surface-water interactions on the structural and energetic properties of the liquid water interface. We find that the molecular structure of water at a weakly interacting (i…
Recent studies have shown the possibility of water transport across carbon nanotubes, even in the case of nanotubes with small diameter (0.822 nm). In this case, water shows subcontinuum transport following an ordered 1D structure stabilized by hydrogen bonds. In this work, we report MD simulations describing the effect of a perpendicular electric field in this single-file water transport in carbon nanotubes. We show that water permeation is substantially reduced for field intensities of 2-3 V/nm and it is no longer possible under perpendicular fields of 4 V/nm.
The electron spin-lattice relaxation of TEMPO and TEMPONE was measured at temperatures between 5 and 80 K in crystalline and glassy ethanol using X-band electron paramagnetic resonance spectroscopy. The experimental data at the lowest temperatures studied were explained in terms of electron-nuclear dipolar interaction between the paramagnetic center and the localized excitations, whereas at higher temperatures low-frequency vibrational modes from the host matrix and Raman processes should be considered. The strong impact of hydrogen bonding between the dopant molecule and ethanol host on the s…
In this paper we develop the first equation of state for alcohol containing mixtures which includes the effect of steric hindrance between the two electron lone pair hydrogen bond acceptor sites on the alcohol's hydroxyl oxygen. The theory is derived for multi-component mixtures within Wertheim's multi-density statistical mechanics in a second order perturbation theory. The accuracy of the new approach is demonstrated by application to pure methanol and ethanol and binary ethanol / water mixtures. It is demonstrated that the new approach gives a substantial improvement in the prediction of hyd…
We present a model for the description of orientational relaxation in hydrogen-bonding liquids. The model contains two relaxation parameters which regulate the intensity and efficiency of dissipation, as well as the memory function which is responsible for the short-time relaxation effects. It is shown that the librational portion of the orientational relaxation is described by an algebraic $\sim t^{-3/2}$ contribution, on top of which more rapid and non-monotonous decays caused by the memory effects are superimposed. The long-time behavior of the orientational relaxation is exponential, altho…
Dense suspensions of hard particles in a liquid can exhibit strikingly counter-intuitive behavior, such as discontinuous shear thickening (DST) [1-8] and reversible shear jamming (SJ) into a state with finite yield stress [9-13]. Recent studies identified a stress-activated crossover from hydrodynamic interactions to frictional particle contacts to be key for these behaviors [2-4, 6-8, 10, 14]. However, many suspensions exhibit only DST and not SJ. Here we show that particle surface chemistry can play a central role in creating conditions that allow for SJ. We find the system's ability to form…
In this Letter, we present a simple model of aqueous interfacial molecular structure and we use this model to isolate the effects of hydrogen bonding on the dielectric properties of the liquid water-vapor interface. By comparing this model to the results of atomistic simulation we show that the anisotropic distribution of molecular orientations at the interface can be understood by considering the behavior of a single water molecule interacting with the average interfacial density field via an empirical hydrogen bonding potential. We illustrate that the depth dependence of this orientational a…
The formation of soluble hydrogen-bonding interpolymer complexes between poly(acrylic acid) (PAA) and poly(acrylic acid-co-2-acrylamido-2-methyl-1-propane sulfonic acid)-graft-poly(N, N dimethylacrylamide) (P(AA-co-AMPSA)-g-PDMAM) at pH = 2.0 was studied. A viscometric study showed that in semidilute solution a physical gel is formed, due to the interconnection of the anionic P(AA-co-AMPSA) backbone of the graft copolymer, in a transient network, by means of the complexes formed between the PDMAM side chains of the graft copolymer and PAA. Dynamic and static light scattering measurements, in c…
Liquid polymorphism is an intriguing phenomenon which has been found in a few single-component systems, the most famous being water. By supercooling liquid Te to more than 130 K below its melting point and performing simultaneous small-angle and wide-angle X-ray scattering measurements, we observe clear maxima in its thermodynamic response functions around 615 K, suggesting the possible existence of liquid polymorphism. A close look at the underlying structural evolution shows the development of intermediate-range order upon cooling, most strongly around the thermodynamic maxima, which we attr…
In this article we study in detail the Q-vector dependence of the collective dynamics in simulated deeply supercooled SPC/E water. The evolution of the system has been followed for 250 ns at low T, allowing a clear identification of a two step relaxation process. We present evidence in favor of the use of the mode coupling theory for supercooled liquid as framework for the description of the slow alpha-relaxation dynamics in SPC/E water, notwithstanding the fact that the cage formation in this system is controlled by the formation of an open network of hydrogen bonds as opposed to packing cons…
Weak hydrogen bonds, such as O-H$\cdotsπ$ and C-H$\cdots$O, are pivotal in a wide range of important natural and industrial processes including biochemical assembly, molecular recognition, and chemical selectivity. In this study we use neutron diffraction in conjunction with comprehensive H/D isotopic substitution to obtain a detailed spatial and orientational picture of the structure in benzene-methanol solution. This system provides us with a prototypical situation where the aromatic ring can act as an hydrogen bond acceptor (via the $π$ electron density) and/or a hydrogen bond donor (via th…
We present a probabilistic approach to water-water hydrogen bonding that allows one to obtain an analytic expression for the number of bonds per water molecule as a function of both its distance to a hydrophobic particle and hydrophobe radius. This approach can be used in the density functional theory (DFT) and computer simulations to examine particle size effects on the hydration of particles and on their solvent-mediated interaction. For example, it allows one to explicitly identify a water hydrogen bond contribution to the external potential whereto a water molecule is subjected near a hydr…
We have investigated the diffusion and structure of TIP4P/2005 water confined in carbon nanotubes subjected to external electric fields. A wide range of diameters has been used to show a highly size-dependent behavior of the water diffusion. We also found that the diffusion is extremely affected by the intensity of the applied field. However, is the relative direction between the field and the tube axis that causes the most intriguing behavior. Electric fields forming angles of $0^{\circ}$ and $45^{\circ}$ with the tube axis were found to slow down the water dynamics by increasing organization…
Water and glycerol are well-known to facilitate the structural relaxation of amorphous protein matrices. However, several studies evidenced that they may also limit fast ($\sim$ pico-nanosecond, ps-ns) and small-amplitude ($\sim$ Å) motions of proteins, which govern their stability in freeze-dried sugar mixtures. To determine how they interact with proteins and sugars in glassy matrices and, thereby, modulate their fast dynamics, we performed molecular dynamics (MD) simulations of lysozyme/trehalose/glycerol (LTG) and trehalose/glycerol (TG) mixtures at low glycerol and water concentrations. U…
Spherical truncations of Coulomb interactions in standard models for water permit efficient molecular simulations and can give remarkably accurate results for the structure of the uniform liquid. However truncations are known to produce significant errors in nonuniform systems, particularly for electrostatic properties. Local molecular field (LMF) theory corrects such truncations by use of an effective or restructured electrostatic potential that accounts for effects of the remaining long-ranged interactions through a density-weighted mean field average and satisfies a modified Poisson's equat…
The aging of aggregated structures of monoglycerides in hydrophobic medium is described by a set of different techniques. Polarized microscopy was used to study the mesomorphic behavior as a function of time. Differential scanning calorimetry was utilized to quantitatively monitor changes in the latent heat in different phase transformations that take place in the aging system. Infrared spectroscopy was applied to detect the formation of hydrogen bonding between surfactants. The X-ray diffraction patterns fingerprinted the molecular arrangement in different emerging phases. Infra-red spectrosc…
We improve a lattice model of water introduced by Sastry, Debenedetti, Sciortino, and Stanley to give insight on experimental thermodynamic anomalies in supercooled phase, taking into account the correlations between intra-molecular orientational degrees of freedom. The original Sastry et al. model including energetic, entropic and volumic effect of the orientation-dependent hydrogen bonds (HBs), captures qualitatively the experimental water behavior, but it ignores the geometrical correlation between HBs. Our mean-field calculation shows that adding these correlations gives a more water-like …
Hypothesis: The structural details, viscosity trends and dynamic phenomena in t-butanol/water solutions are closely related on the molecular scales across the entire composition range. Utilizing the experimental small- and wide-angle x-ray scattering (SWAXS) method, molecular dynamics (MD) simulations and the complemented-system approach method developed in our group it is possible to comprehensively describe the structure-viscosity-dynamics relationship in such structurally versatile hydrogen-bonded molecular liquids, as well as in similar, self-assembling systems with pronounced molecular an…
The viscosity of supercooled water has been a subject of intense study, in particular with respect to its temperature dependence. Much less is known, however, about the influence of dynamical effects on the viscosity in its supercooled state. Here we address this issue for the first time, using molecular dynamics simulations to investigate the shear-rate dependence of the viscosity of supercooled water as described by the TIP4P/Ice model. We show the existence of a distinct cross-over from Newtonian to non-Newtonian behavior characterized by a power-law shear-thinning regime. The viscosity red…
In this work we develop a new classical perturbation theory for water which incorporates the transition to tetrahedral symmetry in both the dispersion and hydrogen bonding contributions to the free energy. This transition is calculated self-consistently using Wertheim's thermodynamic perturbation theory. However, since the reference fluid structure to the hydrogen bonding theory itself depends on hydrogen bonding, the theory represents an approach which goes beyond perturbation theory. The theory is shown to accurately represent the thermodynamics of pure water. It is demonstrated that the new…
We present a direct comparison of the number of dynamically correlated molecules in the shear-mechanical and dielectric relaxations of the following seven supercooled organic liquids: triphenylethylene, tetramethyl-tetraphenyl-trisiloxane, polyphenyl ether, perhydrosqualene, polybutadiene, decahydroisoquinoline, and tripropylene glycol. For each liquid we observe that the numbers of dynamically correlated molecules in the shear and in the dielectric relaxation are proportional. We show that this proportionality can be explained by the constancy of the decoupling index of the shear and dielectr…
Equations of state for hydrogen bonding fluids are typically described by two energy scales. A short range highly directional hydrogen bond energy scale, as well as a reference energy scale which accounts for dispersion and orientationally averaged multi-pole attractions. These energy scales are always treated independently. In recent years, extensive first principles quantum mechanics calculations on small water clusters have shown that both hydrogen bond and reference energy scales depend on the number of incident hydrogen bonds of the water molecule. In this work we propose a new methodolog…
We employ the Distance Matrix method to investigate metabasin dynamics in supercooled water. We find that the motion of the system consists in the exploration of a finite region of configuration space (enclosing several distinct local minima), named metabasin, followed by a sharp crossing to a different metabasin. The characteristic time between metabasin transitions is comparable to the structural relaxation time, suggesting that these transitions are relevant for the long time dynamics. The crossing between metabasins is accompanied by very rapid diffusional jumps of several groups of dynami…
We resolved the hydrogen bond transition from the mode of ordinary water to its hydration in terms of its phonon stiffness (vibration frequency shift), order of fluctuation (line width), and number fraction (phonon abundance) upon chage injection by solvation.
By confining water in nanopores, so narrow that the liquid cannot freeze, it is possible to explore its properties well below its homogeneous nucleation temperature TH ~ 235 K. In particular, the dynamical parameters of water can be measured down to 180 K approaching the suggested glass transition temperature Tg ~ 165 K. Here we present experimental evidence, obtained from Nuclear Magnetic Resonance and Quasi-Elastic Neutron Scattering spectroscopies, of a well defined decoupling of transport properties (the self-diffusion coefficient and the average translational relaxation time), which impli…
Molecular dynamics simulations have been performed on TIP4P/2005 supercooled water to investigate the molecular diffusion and shear viscosity at various timescales and assess the Stokes-Einstein (SE) and Stokes-Einstein-Debye (SED) relations. For this purpose, we calculated various time correlation functions, such as the mean-squared displacement, stress relaxation function, density correlation function, hydrogen-bond correlation function, rotational correlation function of molecular orientation, non-Gaussian parameter, and four-point correlation function. Our study of the SE and SED relations…
We use systematic 8 ns ab initio molecular dynamics (AIMD) to study the structure and dynamics of water in bulk, and close to both hydrophobic and hydrophilic (carbonyl) groups of tetramethylurea (TMU). We observe crossovers in the dynamical behavior around the hydrophobic group at $T_X = 256 \pm 4$K and another one at $265 \pm 5$K related to the relative strength of water-water and water-carbonyl hydrogen bonds (HBs). For bulk water, the temperature of the apparent divergence in relaxation times is located at $T_c = 210 \pm 10$K. To better identify the effects arising from the hydrophilic car…
Hydrogen bonding to chloride ions has been frequently discussed over the past 5 decades. Still, the possible role of such secondary intermolecular bonding interactions in hydrogen bonded networks has not been investigated in any detail. Here we consider computer models of concentrated aqueous LiCl solutions and compute usual hydrogen bond network characteristics, such as distributions of cluster sizes and of cyclic entities, both for models that take and do not take chloride ions into account. During the analysis of hydrogen bonded rings, a significant amount of 'solvent separated anion pairs'…
Within the so-called "no-man's land" between about 150 and 235 K, crystallization of bulk water is inevitable. The glasslike freezing and a liquid-to-liquid transition of water, predicted to occur in this region, can be investigated by confining water in nanometer-sized pores. Here we report the molecular dynamics of water within the pores of a metal-organic framework using dielectric spectroscopy. The detected temperature-dependent dynamics of supercooled water matches that of bulk water as reported outside the borders of the no-man's land. In confinement, a different type of water is formed,…
The violation of Stokes--Einstein (SE) relation $D\sim (η/T)^{-1}$ between the shear viscosity $η$ and the translational diffusion constant $D$ at temperature $T$ is of great importance for characterizing anomalous dynamics of supercooled water. Determining which time scales play key roles in the SE violation remains elusive without the measurement of $η$. Here we provide comprehensive simulation results of the dynamic properties involving $η$ and $D$ in TIP4P/2005 supercooled water. This enabled the thorough identification of the appropriate time scales for SE relation $Dη/T$. In particular, …
Importance of nuclear quantum effects on the structure of supercooled water around its liquid--liquid critical point
Center for Advanced Systems Understanding (CASUS)（先进系统理解中心）；Helmholtz Zentrum Dresden-Rossendorf（德累斯顿-罗斯多夫亥姆霍兹中心）；Paderborn University（帕德博恩大学）；Technische Universität Dresden（德累斯顿工业大学）
