相关论文: Reaction coordinates and rate constants for liquid…
Understanding the underlying mechanism of crystal nucleation during solidification is a fundamental aspect in the prediction and control of materials properties. Classical nucleation theory (CNT) assumes that homogeneous nucleation occurs…
Identifying reaction coordinates(RCs) is an active area of research, given the crucial role RCs play in determining the progress of a chemical reaction. The choice of the reaction coordinate is often based on heuristic knowledge. However,…
Understanding the driving forces behind the nucleation of different polymorphs is of great importance for material sciences and the pharmaceutical industry. This includes understanding the reaction coordinate that governs the nucleation…
The nucleation rates derived for the condensation from a supersaturated vapor are examined both in the classical theory and in the modern coarse-grained field theory. By virtue of the scaling variable $\lambda_Z$ it is shown that the method…
Using state-of-the-art rare-event sampling simulations, we precisely characterize the nucleation of liquid droplets from a supersaturated Lennard-Jones gas and uncover a key physical feature: critical clusters nucleate with a density that…
The task of a first principles theoretical calculation of the rate of gas to liquid nucleation has remained largely incomplete despite the existence of reliable results from unbiased simulation studies at large supersaturation. Although the…
Using the entropy $S$ as a reaction coordinate, we determine the free energy barrier associated with the formation of a liquid droplet from a supersaturated vapor for atomic and molecular fluids. For this purpose, we develop the $\mu VT-S$…
Molecular dynamics (MD) simulation is applied to the condensation process of supersaturated vapors of methane, ethane, and carbon dioxide. Simulations of systems with up to a million particles were conducted with a massively parallel MD…
Condensation of a liquid droplet from a supersaturated vapour phase is initiated by a prototypical nucleation event. As such it is challenging to compute its rate from atomistic molecular dynamics simulations. In fact at realistic…
Reaction coordinates (RCs) are low-dimensional representations of complex dynamical systems that capture their long-term dynamics. In this work, we focus on the criteria of lumpability and decomposability, previously established for…
Reaction Coordinates (RCs) are indicators of hidden, low-dimensional mechanisms that govern the long-term behavior of high-dimensional stochastic processes. We present a novel and general variational characterization of optimal RCs and…
We performed molecular dynamics (MD) simulations of the nucleation of water vapor in order to test nucleation theories. Simulations were performed for a wide range of supersaturation ratios (S = 3-25) and water temperatures (Tw=300-390K).…
Nucleation in supersaturated vapor is investigated with two series of molecular dynamics simulations in the canonical ensemble. The applied methods are: (a) analysis of critical nuclei at moderate supersaturations by simulating equilibria…
Among the challenges in discriminating between theoretical approaches to the glass transition is obtaining suitable data. In particular, particle--resolved data in liquids supercooled past the mode--coupling crossover has until recently…
The process of nucleation of vapor bubbles from a superheated liquid and of liquid droplets from a supersaturated vapor is investigated using the Modified-Core van der Waals model Density Functional Theory (Lutsko, JCP 128, 184711 (2008)).…
The classical nucleation theory (CNT) and its modified versions provide a convenient framework for describing the nucleation process under the capillary approximation. However, these models often predict nucleation rates that depart…
Crystallization of supersaturated liquids usually starts by heterogeneous nucleation. Mounting evidence shows that even homogeneous nucleation in simple liquids takes place in two steps; first a dense amorphous precursor forms, and the…
The evaluation of nucleation rates from molecular dynamics trajectories is hampered by the slow nucleation time scale and impact of finite size effects. Here, we show that accurate nucleation rates can be obtained in a very general fashion…
Reservoir computing (RC) is a state-of-the-art machine learning method that makes use of the power of dynamical systems (the reservoir) for real-time inference. When using biological complex systems as reservoir substrates, it serves as a…
The conventional theory of homogeneous and heterogeneous nucleation in a supersaturated vapor is tested by Monte Carlo simulations of the lattice gas (Ising) model with nearest-neighbor attractive interactions on the simple cubic lattice.…