Replica exchange statistical temperature Monte Carlo.

The replica exchange statistical temperature Monte Carlo algorithm (RESTMC) is presented, extending the single-replica STMC algorithm [J. Kim, J. E. Straub, and T. Keyes, Phys. Rev. Lett. 97, 050601 (2006)] to alleviate the slow convergence of the conventional temperature replica exchange method (t-REM) with increasing system size. In contrast to the Gibbs-Boltzmann sampling at a specific temperature characteristic of the standard t-REM, RESTMC samples a range of temperatures in each replica and achieves a flat energy sampling employing the generalized sampling weight, which is automatically determined via the dynamic modification of the replica-dependent statistical temperature. Faster weight determination, through the dynamic update of the statistical temperature, and the flat energy sampling, maximizing energy overlaps between neighboring replicas, lead to a considerable acceleration in the convergence of simulations even while employing significantly fewer replicas. The performance of RESTMC is demonstrated and quantitatively compared with that of the conventional t-REM under varying simulation conditions for Lennard-Jones 19, 31, and 55 atomic clusters, exhibiting single- and double-funneled energy landscapes.