Shuangliang Zhao

Blocking effect of benzene-like fluid transport in nanoscale block-pores

Abstract The flux through nanoscale pore is one of the key quantities in many processes including membrane applications and fluid separation. Whereas many efforts have been dedicated to the investigation of the fluid flux in nano-channels, the fluid transport behaviours in the block-pores, which contain distinct parts with different geometries or interactions with fluid, are still poorly understood. In this work, by combining both non-equilibrium dynamics simulation and density functional theory, we developed an efficient method for investigating the fluid flux in the block-pores, with which the fluxes of benzene in graphene block slit pores containing a hydrophobic and a hydrophilic region are thereafter investigated. We demonstrate that a region with a stronger interaction with fluid generates a bottleneck for the fluid flow, which greatly suppresses the flux in the pore even though there is no geometrical variation. By tuning the fluid-substrate interaction, the flux inside can be controlled. This study gives clues for the practical application of membrane design.

Melting dynamics of short dsDNA chains in saline solutions

DNA melting has attracted much attention due to its importance in understanding the life-reproduction and metabolism and in the applications of modern DNA-based technologies. While numerous works have been contributed to the determination of melting profiles in diverse environments, the understanding of DNA melting dynamics is still limited. By employing three-site-per-nucleotide (3SPN) double-stranded DNA (dsDNA) model, we here demonstrate the melting dynamics of an isolated short dsDNA under different conditions (different temperatures, ionic concentrations and DNA chain lengths)xa0can be accessed byxa0coarse-grainedxa0simulation studies. We particularly show that at dilute ionic concentration the dsDNA, regardless being symmetric or asymmetric, opens at both ends with roughly equal probabilities, while at high ionic concentration the asymmetric dsDNA chain opens at the A-T-rich end. The comparisons of our simulation results to available data are discussed, and overall good agreements have been found.

Thermostat effect on water transport dynamics across CNT membranes

Abstract Whereas numerous experimental and simulation studies have been contributed to the investigation of fluid transport across membranes in the past decades, there is a significant discrepancy between experiments and simulations in the magnitude of fluid permeability and the degree of flow rate enhancement. Here, we show that one of the causes of the discrepancy is the variety of thermostating object, via which the temperature of fluid flow in non-equilibrium molecular simulations is controlled. By thermostating either the water system or the membrane material with Langevin method, we examine the temperatures of water flows in two types of membranes, the amounts of absorbed water molecules, fluid velocities, slip lengths and water fluxes. We show that thermostating the CNT membrane brings overall enhanced water flow than directly thermostating the water system. Moreover, increasing the temperature coupling time in the thermostat gives rise to an enhancement of water flux, while weakens the stability of system temperature. In addition to explaining the disparate simulation results on fluid transport in nanopores, this work provides guidelines for diagnosing the setting of NEMD simulations.

Confinement Effect on Molecular Conformation of Alkanes in Water-Filled Cavitands: A Combined Quantum/Classical Density Functional Theory Study

The depletion force exerted on an alkane molecule from surrounding solvent may greatly alter its conformation. Such a behavior is closely related to the selective molecular recognition, molecular sensors, self-assembly, and so on. Herein, we report a multiscale theoretical study on the conformational change of a single alkane molecule confined in water-filled cavitands, in which the quantum and classical density functional theories (DFTs) are combined to determine the grand potential of alkane-water system. Specifically, the intrinsic free energy of the alkane molecule is tackled by quantum DFT, while the solvent effect arising from the solvent density inhomogeneity in confined space is addressed by classical DFT. By varying the alkane chain length, pore size, and wettability of inner pore surface, we find that pore confinement and hydrophilic inner surface facilitate the alkane conformational change from extended state to helical state, which becomes more significant as the alkane chain length increases. Our findings, which are in line with previous experimental observations, provide not only the microscopic mechanism but also theoretical guidance for elaborately manipulating molecular conformation at the nanoscale.