相关论文: Tracing the minimum-energy path on the free-energy…
The solution of the shortest path problem on a surface is not only a theoretical problem to be solved in the field of mathematics, but also problems that need to be solved in very different fields such as medicine, defense and construction…
The reaction between D$^+$ and H$_2$ plays an important role in astrochemistry at low temperatures and also serves as a prototype for simple ion-molecule reaction. Its ground $\tilde{X}~^1A^{\prime}$ state has a very small thermodynamic…
We present an approach that extends the theory of targeted free energy perturbation (TFEP) to calculate free energy differences and free energy surfaces at an accurate quantum mechanical level of theory from a cheaper reference potential.…
Studies of ion-molecule reactions at low temperatures are difficult because stray electric fields in the reaction volume affect the kinetic energy of charged reaction partners. We describe a new experimental approach to study ion-molecule…
A variety of methods are developed for characterising the free energy landscapes of continuum, Landau-type free energy models. Using morphologies of lipid vesicles and a multistable liquid crystal device as examples, I show that the methods…
Characterizing conformational transitions in physical systems remains a fundamental challenge, as traditional sampling methods struggle with the high-dimensional nature of molecular systems and high-energy barriers between stable states.…
We describe a self-contained procedure to evaluate the free energy of liquid and solid phases of an alloy system. The free energy of a single-element solid phase is calculated with thermodynamic integration using the Einstein crystal as the…
Temperature dependence of the thermal rate constants and kinetic isotope effects (KIE) of the CN + C2H6 gas-phase hydrogen abstraction reaction was theoretically determined within the 25-1000 K temperature range, i.e., from ultra-low to…
The thermal evolution of the energies and free energies of a set of spherical and near-spherical nuclei spanning the whole periodic table are calculated in the subtracted finite-temperature Thomas- Fermi framework with the zero-range…
Minimum energy paths for transitions such as atomic and/or spin rearrangements in thermalized systems are the transition paths of largest statistical weight. Such paths are frequently calculated using the nudged elastic band method, where…
The basic thermodynamic quantities for a non-interacting scalar field in a periodic potential composed of either a one-dimensional chain of Dirac $\delta$-$\delta^\prime$ functions or a specific potential with extended compact support are…
We propose a new method to compute the free energy or enthalpy of fluids or disordered solids by computer simulation . The main idea is to construct a reference system by freezing one representative configuration, and then carry out a…
In a previous joint experimental and theoretical study of the barrierless chemical reaction C(1D) + H2 at low temperatures (300-50 K) [K. M. Hickson, J.-C. Loison, H. Guo, Y. V. Suleimanov, J. Phys. Chem. Lett., 2015, 6, 4194.], excellent…
Free energy calculations of two crystalline phases of the molecular compound S8 were performed via molecular dynamics simulations of these crystals. The elemental sulphur S8 molecule model used in our MD calculations consists of a…
Often gaining insight into the functioning of biomolecular systems requires to follow their dynamics along a microscopic reaction coordinate (RC) on a macroscopic time scale, which is beyond the reach of current all atom molecular dynamics…
Stochastic electronic structure theories, e.g., Quantum Monte Carlo methods, enable highly accurate total energy calculations which in principle can be used to construct highly accurate potential energy surfaces. However, their stochastic…
Precipitation of the topologically close-packed Fe2Mo Laves phase at the interface between the nuclear fuel and the fuel element cladding can significantly weaken the strength characteristics of the cladding and fuel. Despite the importance…
Using a thermodynamic integration scheme, we compute the free energy cost per unit area, $\gamma$, of forming an interface between a crystal and a frozen structured wall, formed by particles frozen into the same equilibrium structure as the…
Understanding the thermodynamics of the interfacial interactions between oil and kerogen is imperative for recovering hydrocarbon in tight reservoirs, especially in unconventional shale that retains abundant hydrocarbon in kerogen…
Energetic correlations due to polymeric constraints and the locality of interactions, in conjunction with the apriori specification of the existence of a particularly low energy state, provides a method of introducing the aspect of minimal…