Kinetics of first-order phase transitions from microcanonical thermostatistics
arXiv:2004.08587 · doi:10.1088/1742-5468/aba687
Abstract
More than a century has passed since van't Hoff and Arrhenius formulated their celebrated rate theories, but there are still elusive aspects in the temperature-dependent phase transition kinetics of molecular systems. Here I present a theory based on microcanonical thermostatistics that establishes a simple and direct temperature dependence for all rate constants, including the forward and the reverse rate constants, the equilibrium constant, and the nucleation rate. By considering a generic model that mimic the microcanonical temperature of molecular systems in a region close to a first-order phase transition, I obtain shape-free relations between kinetics and thermodynamics physical quantities which are validated through stochastic simulations. Additionally, the rate theory is applied to results obtained from protein folding and ice nucleation experiments, demonstrating that the expressions derived here can be used to describe the experimental data of a wide range of molecular systems.
arXiv comment22 pages, 5 figures
References in corpus (21)
- An efficient, multiple range random walk algorithm to calculate the density of states
- Path ensembles averages in systems driven far-from-equilibrium
- Inequivalence of ensembles in a system with long range interactions
- Feedback-optimized parallel tempering Monte Carlo
- Optimizing the ensemble for equilibration in broad-histogram Monte Carlo simulations
- Microcanonical Analyses of Peptide Aggregation Processes
- Microcanonical entropy inflection points: Key to systematic understanding of transitions in finite systems
- Generalized Ensemble and Tempering Simulations: A Unified View
- Make life simple: unleash the full power of the parallel tempering algorithm
- Multicanonical Simulations Step by Step
- Systematic Microcanonical Analyses of Polymer Adsorption Transitions
- Canonical free-energy barrier of particle and polymer cluster formation
- Extended gaussian ensemble solution and tricritical points of a system with long-range interactions
- Multicanonical entropy like-solution of statistical temperature weighted histogram analysis method (ST-WHAM)
- Microcanonical thermostatistics of coarse-grained proteins with amyloidogenic propensity
- Amyloid Fibril Solubility
- Exploiting a semi-analytic approach to study first order phase transitions
- Optimized broad-histogram simulations for strong first-order phase transitions: Droplet transitions in the large-Q Potts model
- Microcanonical thermostatistics analysis without histograms: cumulative distribution and Bayesian approaches
- Optimal Coordinate as a General Method in Stochastic Dynamics
- The extended gaussian ensemble and metastabilities in the Blume-Capel model