Rongzheng Wan

A charge-driven molecular water pump

Understanding and controlling the transport of water across nanochannels is of great importance for designing novel molecular devices, machines and sensors and has wide applications, including the desalination of seawater. Nanopumps driven by electric or magnetic fields can transport ions and magnetic quanta, but water is charge-neutral and has no magnetic moment. On the basis of molecular dynamics simulations, we propose a design for a molecular water pump. The design uses a combination of charges positioned adjacent to a nanopore and is inspired by the structure of channels in the cellular membrane that conduct water in and out of the cell (aquaporins). The remarkable pumping ability is attributed to the charge dipole-induced ordering of water confined in the nanochannels, where water can be easily driven by external fields in a concerted fashion. These findings may provide possibilities for developing water transport devices that function without osmotic pressure or a hydrostatic pressure gradient.

Water-mediated signal multiplication with Y-shaped carbon nanotubes

Molecular scale signal conversion and multiplication is of particular importance in many physical and biological applications, such as molecular switches, nano-gates, biosensors, and various neural systems. Unfortunately, little is currently known regarding the signal processing at the molecular level, partly due to the significant noises arising from the thermal fluctuations and interferences between branch signals. Here, we use molecular dynamics simulations to show that a signal at the single-electron level can be converted and multiplied into 2 or more signals by water chains confined in a narrow Y-shaped nanochannel. This remarkable transduction capability of molecular signal by Y-shaped nanochannel is found to be attributable to the surprisingly strong dipole-induced ordering of such water chains, such that the concerted water orientations in the 2 branches of the Y-shaped nanotubes can be modulated by the water orientation in the main channel. The response to the switching of the charge signal is very rapid, from a few nanoseconds to a few hundred nanoseconds. Furthermore, simulations with various water models, including TIP3P, TIP4P, and SPC/E, show that the transduction capability of the Y-shaped carbon nanotubes is very robust at room temperature, with the interference between branch signals negligible.

Dynamics of single-file water chains inside nanoscale channels: physics, biological significance and applications

Transportation of water across nanochannels is of great importance for biological activities as well as for designing novel molecular devices/machines/sensors, which has wide applications in nanotechnology. With the development of experimental and computational facilities and technologies, it becomes possible to study the water dynamics inside and across the nanoscale channels by both experiments and numerical simulations. When the radius of a nanochannel is appropriate, the water molecules inside the channel form a single-file structure. Water confined in these nanoscale channels usually exhibits different dynamics not seen in the bulk system, including the wet - dry transition due to confinement, concerted hydrogen-bond orientations and flipping, concerted motion of water molecules and wavelike density distribution pattern. The permeation of water across the channels also shows unique behaviours, such as extra-high permeability, excellent on - off gating behaviour with response to the external mechanical and electrical signals and noises, reduction and enhancement by charge distributions on the channel walls, as well as directional transportation by a combination of charges close to a channel. In this review, we examine some of the recent advances in the dynamics of these single-file water molecules inside very narrow nanochannels.

Kinetics of water filling the hydrophobic channels of narrow carbon nanotubes studied by molecular dynamics simulations.

The kinetics of water filling narrow single-walled carbon nanotubes was studied using molecular dynamics simulations. The time required to fully fill a nanotube was linear with respect to the tube length. We observed that water molecules could enter into nanotubes of different lengths, either from one end or from both ends. The probability of having a nanotube filled completely from both ends increased exponentially with the tube length. For short tubes, filling usually proceeded from only one end. For long tubes, filling generally proceeded from both tube ends over three stages, i.e., filling from one end, filling from both ends, and filling from both ends with the dipole reorientation of water molecules to give a concerted ordering within the fully filled tube. The water molecules in the partially filled nanotube were hydrogen bonded similarly to those in the fully filled nanotube. Simulations for the reference Lennard-Jones fluid without hydrogen bonds were also performed and showed that the filling behavior of water molecules can be attributed to strong intermolecular hydrogen bonding.

Enhancement of Water Evaporation on Solid Surfaces with Nanoscale Hydrophobic-Hydrophilic Patterns

Using molecular dynamics simulations, we show that the evaporation of nanoscale water on hydrophobic-hydrophilic patterned surfaces is unexpectedly faster than that on any surfaces with uniform wettability. The key to this phenomenon is that, on the patterned surface, the evaporation rate from the hydrophilic region only slightly decreases due to the correspondingly increased water thickness; meanwhile, a considerable number of water molecules evaporate from the hydrophobic region despite the lack of water film. Most of the evaporated water from the hydrophobic region originates from the hydrophilic region by diffusing across the contact lines. Further analysis shows that the evaporation rate from the hydrophobic region is approximately proportional to the total length of the contact lines.

Evaporation of Tiny Water Aggregation on Solid Surfaces with Different Wetting Properties

The evaporation of a tiny amount of water on the solid surface with different wettabilities has been studied by molecular dynamics simulations. From nonequilibrium MD simulations, we found that, as the surface changed from hydrophobic to hydrophilic, the evaporation speed did not show a monotonic decrease as intuitively expected, but increased first, and then decreased after it reached a maximum value. The analysis of the simulation trajectory and calculation of the surface water interaction illustrate that the competition between the number of water molecules on the water-gas surface from where the water molecules can evaporate and the potential barrier to prevent those water molecules from evaporating results in the unexpected behavior of the evaporation. This finding is helpful in understanding the evaporation on biological surfaces, designing artificial surfaces of ultrafast water evaporating, or preserving water in soil.

Asymmetric transportation induced by thermal noise at the nanoscale

Based on a simple model, we theoretically show that asymmetric transportation is possible in nanoscale systems experiencing thermal noise without the presence of external fluctuations. The key to this theoretical advance is that the correlation lengths of the thermal fluctuations become significantly long for nanoscale systems. This differs from macroscopic systems in which the thermal noises are usually treated as white noise. Our observation does not violate the second law of thermodynamics, since at the nanoscale, extra energy is required to keep the asymmetric structure against thermal fluctuations.

Water permeation across nanochannels with defects

Defects are common in fabricated nanochannels. In this paper, water permeation across a single-walled carbon nanotube with defects was studied using molecular dynamics simulations. It is found that the impact on water permeation is negligible when the density of the defects is small, while a significant reduction in water permeation is observed when the density of the defects is high. These findings should be helpful in both understanding water permeation across nanochannels and designing efficient artificial nanochannel.

Diffusing of an ammonia molecule in water in a very short time period

The diffusion of an ammonia molecule (NH3) in water was investigated by molecular dynamic simulations. It is found that the diffusion shows negative correlation with its dipole orientation.

Intrinsic autocorrelation time of picoseconds for thermal noise in water.

Whether thermal noise is colored or white is of fundamental importance. In conventional theory, thermal noise is usually treated as white noise so that there are no directional transportations in the asymmetrical systems without external inputs, since only the colored fluctuations with appropriate autocorrelation time length can lead to directional transportations in the asymmetrical systems. Here, on the basis of molecular dynamics simulations, we show that the autocorrelation time length of thermal noise in water is ~10 ps at room temperature, which indicates that thermal noise is not white in the molecular scale while thermal noise can be reasonably assumed as white in macro- and meso-scale systems. The autocorrelation time length of thermal noise is intrinsic, since the value is almost unchanged for different temperature coupling methods. Interestingly, the autocorrelation time of thermal noise is correlated with the lifetime of hydrogen bonds, suggesting that the finite autocorrelation time length of thermal noise mainly comes from the finite lifetime of the interactions between neighboring water molecules.