Computation of the equilibrium three-particle entropy for dense atomic fluids by molecular dynamics simulation
Luca Maffioli, Nathan Clisby, Federico Frascoli, BD Todd
The Journal of Chemical Physics | AMER INST PHYSICS | Published : 2019
We have computed the two- and three-particle contribution to the entropy of a Weeks-Chandler-Andersen fluid via molecular dynamics simulations. The three-particle correlation function and entropy were computed with a new method which simplified the calculation. Results are qualitatively similar to Lennard-Jones systems. We observed a numerical instability in the three-particle contribution. This phenomenon has been previously detected when the traditional method is used; thus, it is likely to be intrinsic in the computation. While the effect of statistical fluctuations can be removed through an extrapolation procedure, the discretization error due to the finite bin size is more difficult to ..View full abstract
Awarded by Australian Research Council under the Future Fellowship scheme
N.C. gratefully acknowledges support from the Australian Research Council under the Future Fellowship scheme (Project No. FT130100972).