Predicting reaction coordinates in energy landscapes with diffusion anisotropy.

Area of Science:

• Computational Chemistry
• Statistical Mechanics
• Molecular Dynamics Simulations

Background:

• Understanding molecular dynamics in systems with metastable states is crucial for predicting chemical reactions and material properties.
• Identifying an accurate reaction coordinate is essential for efficient molecular dynamics simulations, especially in high friction regimes.
• Diffusion anisotropy significantly complicates the determination of optimal reaction coordinates.

Purpose of the Study:

• To investigate the dependence of the optimal reaction coordinate on diffusion anisotropy in model potentials.
• To extend the Spectral Gap Optimization of Order Parameters (SGOOP) method to incorporate dynamical observables.
• To accurately determine the best reaction coordinate for systems with arbitrary anisotropies.

Main Methods:

• Utilized the Spectral Gap Optimization of Order Parameters (SGOOP) method, previously developed by the authors.
• Incorporated both static and dynamic information about observables into the SGOOP framework.
• Simulated molecular dynamics in the high friction regime with a thermal bath for various model potentials.

Main Results:

• Demonstrated that the enhanced SGOOP method can accurately determine the optimal reaction coordinate even with significant diffusion anisotropy.
• Showcased the successful integration of dynamical observables, leading to improved accuracy compared to methods relying solely on static information.
• Validated the findings through comparisons with transmission coefficient calculations and existing benchmark data.

Conclusions:

• The enhanced SGOOP method provides a robust and accurate approach for identifying optimal reaction coordinates in complex molecular systems.
• This method offers significant advantages for simulating systems with anisotropic diffusion and metastable states.
• The ability to incorporate dynamical information broadens the applicability and predictive power of SGOOP for molecular simulations.