We experimentally realized and elucidated kinetically limited evaporation where the molecular gas dynamics close to the liquid–vapour interface dominates the overall transport. This process fundamentally dictates the performance of various evaporative systems and has received significant theoretical interest. However, experimental studies have been limited due to the difficulty of isolating the interfacial thermal resistance. Here, we overcome this challenge using an ultrathin nanoporous membrane in a pure vapour ambient. We demonstrate a fundamental relationship between the evaporation flux and driving potential in a dimensionless form, which unifies kinetically limited evaporation under different working conditions. We model the nonequilibrium gas kinetics and show good agreement between experiments and theory. Our work provides a general figure of merit for evaporative heat transfer as well as design guidelines for achieving efficient evaporation in applications such as water purification, steam generation, and thermal management.

We derive the equation of motion for non-Markovian dissipative particle dynamics (NMDPD) by introducing the history effects on the time evolution of the system. Our formulation is based on the generalized Langevin equation, which describes the motions of the centers of mass of clusters comprising microscopic particles. The mean, friction, and fluctuating forces in the NMDPD model are directly constructed from an underlying molecular dynamics (MD) system without any scaling procedure. For the validation of our formulation, we construct NMDPD models from high-density Lennard-Jones systems, in which the typical time scales of the coarse-grained particle motions and the fluctuating forces are not fully separable. The NMDPD models reproduce the temperatures, diffusion coefficients, and viscosities of the corresponding MD systems more accurately than the dissipative particle dynamics models based on a Markovian approximation. Our results suggest that the NMDPD method is a promising alternative for simulating mesoscale flows where a Markovian approximation is not valid.

Evaporation is a ubiquitous phenomenon found in nature and widely used in industry. Yet a fundamental understanding of interfacial transport during evaporation remains limited to date owing to the difficulty of characterizing the heat and mass transfer at the interface, especially at high heat fluxes (>100 W/cm). In this work, we elucidated evaporation into an air ambient with an ultrathin (≈200 nm thick) nanoporous (≈130 nm pore diameter) membrane. With our evaporator design, we accurately monitored the temperature of the liquid-vapor interface, reduced the thermal-fluidic transport resistance, and mitigated the clogging risk associated with contamination. At a steady state, we demonstrated heat fluxes of ≈500 W/cm across the interface over a total evaporation area of 0.20 mm. In the high flux regime, we showed the importance of convective transport caused by evaporation itself and that Fick's first law of diffusion no longer applies. This work improves our fundamental understanding of evaporation and paves the way for high flux phase-change devices.

We propose a new coarse-grained (CG) molecular simulation technique based on the Mori-Zwanzig (MZ) formalism along with the iterative Boltzmann inversion (IBI). Non-Markovian dissipative particle dynamics (NMDPD) taking into account memory effects is derived in a pairwise interaction form from the MZ-guided generalized Langevin equation. It is based on the introduction of auxiliary variables that allow for the replacement of a non-Markovian equation with a Markovian one in a higher dimensional space. We demonstrate that the NMDPD model exploiting MZ-guided memory kernels can successfully reproduce the dynamic properties such as the mean square displacement and velocity autocorrelation function of a Lennard-Jones system, as long as the memory kernels are appropriately evaluated based on the Volterra integral equation using the force-velocity and velocity-velocity correlations. Furthermore, we find that the IBI correction of a pair CG potential significantly improves the representation of static properties characterized by a radial distribution function and pressure, while it has little influence on the dynamic processes. Our findings suggest that combining the advantages of both the MZ formalism and IBI leads to an accurate representation of both the static and dynamic properties of microscopic systems that exhibit non-Markovian behavior.

We investigate the mechanical properties of π-conjugated polymeric materials composed of regioregular poly(3-hexylthiophene) (P3HT) and fullerene C60 using coarse-grained molecular dynamics simulations. Specifically, we perform tensile simulations of P3HT:C60 composites with varied degrees of polymerization and C60 mass fractions to obtain their stress-strain responses.Decomposition of stress tensor into kinetic energy and virial contributions indicates that the tensile moduli of the pure P3HT samples are greatly dependent on non-bonded interactions and on bonded interactions associated with bond-stretching, while the addition of C60 leads to an increase in the tensile modulus originating from enhanced non-bonded interactions associated with C60. Additionally, the tensile strength of the P3HT:C60 samples correlates well with molecular chain entanglements, which are characterized by the average number of kinks per chain obtained from primitive path analysis. We also find that the upper and lower yield points characterizing strain softening become more pronounced with increasing C60 mass fraction.Persistent homology analysis indicates that the emergence of the yield points correlates well with the coalescence of microvoids in the course of tensile deformation, resulting in the generation of larger voids. These results provide a fundamental understanding of the molecular determinants of the mechanical properties of π-conjugated polymer-fullerene composites, which can also help to interpret and predict the mechanical properties of other polymer composites containing fullerene.