Molecular simulations of interfacial systems: challenges, applications and future perspectives

ABSTRACT

We present a comprehensive review of methods and applications of molecular simulations of interfacial systems. We give a detailed overview of the main techniques and major challenges in the following aspects of solid and fluid surfaces: adsorption at solid surfaces, interfacial transport and surface-to-bulk partitioning. We summarise methods to estimate macroscopic properties interfaces (adsorption isotherms, surface tension and contact angle) and ways to extract quantitative information about fluctuating liquid surfaces. We demonstrate the usage of these methods on recent applications from the fields of atmospheric science, material science and biophysics. The two main goals of this review are: (i) to provide guidance in practical questions, such as choosing software, force field, level of theory, system geometry, and finding the appropriate selective surface analysis methods based on the type of the interface and the nature of the physical problem to be studied; and (ii) to highlight domains where molecular simulations can bring about substantial advances in our understanding in important questions of applied science as a function of future method development and adaptation for applied fields.

KEYWORDS:

• Molecular dynamics
• grand canonical Monte Carlo
• enhanced sampling
• interfaces
• nanoparticles

Acknowledgments

The authors thank Miguel Jorge, Ranjit Bahadur, Lynn Russell, Paul L. Barclay and Jennifer Lukes for agreeing to reproduce figures from their publications. Vlasis G. Mavrantzas is acknowledged for sharing invaluable insights in the topic of polymer simulations.

Disclosure statement

No potential conflict of interest was reported by the author(s).

Additional information

Funding

M. D. and A. N. acknowledge the the Swiss National Science Foundation (Project number: CRSK-2 195329) for funding. A. N. acknowledges ERC project PyroTRACH (ERC-2016-CoG) funded from H2020-EU.1.1. - Excellent Science - European Research Council (ERC), project ID 726165 for funding. K. S. K. would like to acknowledge the co-finance support by Greece and the European Union (European Social Fund- ESF) through the Operational Programme Human Resources Development, Education and Lifelong Learning 2014–2020 in the context of the project ‘Study of the rheology of polymer nanocomposite melts by combining atomistic simulations and constitutive modelling (PNC Rheo)’ (MIS 5047161). M. N. D. S. C. would like to acknowledge the financial support of FCT/MEC through national funds (grant UIDB/50006/2020).