RT Journal Article
T1 Solid−Liquid Interfacial Free Energy from Computer Simulations: Challenges and Recent Advances
A1 Pasquale, Nicodemo Di
A1 Algaba Fernández, Jesús
A1 Jiménez Blas, Felipe
A1 Rovigatti, Lorenzo
AB The study of interfacial properties in liquid−liquid and liquid−vapor systemshas a history of nearly 200 years, with significant contributions from scientific luminaries suchas Thomas Young and Willard Gibbs. However, a similar level of understanding of solid−liquidinterfaces has emerged only more recently, largely because of the numerous complicationsassociated with the thermodynamics needed to describe them. The accurate calculation of theinterfacial free energy of solid−liquid systems is central to determining which interfaces will beobserved and their properties. However, designing and analyzing the molecular dynamicssimulations required to do this remains challenging, unlike the liquid−liquid or liquid−vaporcases, because of the unique complications associated with solid−liquid systems. Specifically,the lattice structure of solids introduces spatial directionality, and atomic configurations insolids can be altered by stretching. The primary aim of this review is to provide an overview ofthe numerical approaches developed to address the challenge of calculating the interfacial freeenergy in solid−liquid systems. These approaches are classified as (i) direct methods, whichcompute interfacial free energies explicitly, albeit often through convoluted procedures, and (ii) indirect methods, which derive thesefree energies as secondary results obtained from the analysis of simulations of an idealized experimental configuration. We alsodiscuss two key topics related to the calculation of the interfacial free energy of solid−liquid systems: nucleation theory and curvedinterfaces, which represent important problems where research remains highly active
PB American Chemical Society
SN 0009-2665
SN 1520-6890 (electrónico)
YR 2025
FD 2025-05
LK https://hdl.handle.net/10272/25558
UL https://hdl.handle.net/10272/25558
LA eng
NO Di Pasquale, N., Algaba, J., Montero de Hijes, P., Sanchez-Burgos, I., Tejedor, A. R., Yeandel, S. R., Blas, F. J., Davidchack, R. L., Espinosa, J. R., Freeman, C. L., Harding, J. H., Laird, B. B., Sanz, E., Vega, C., & Rovigatti, L. (2025). Solid–Liquid Interfacial Free Energy from Computer Simulations: Challenges and Recent Advances. Chemical Reviews. https://doi.org/10.1021/acs.chemrev.4c00833
NO We acknowledge support from CECAM and CCP5 through theCECAM/CCP5 sandpit grant (EP/V028537/1) awarded toN.D.P. and L.R. J.H., C.F., and S.Y. acknowledge support fromthe “Crystallization in the Real World” program grant (EPSRCGrant number EP/R018820/1). E.Sanz and C.Vega acknowledge funding from Grant PID2022-136919NB-C31 of theSpanish Ministry of Science and Innovation. J. R. E. acknowledges funding from the Ramon y Cajal fellowship (RYC2021-030937-I) and from the Spanish scientific plan and committeefor research: project reference PID2022-136919NA-C33. F.J.B.and J.A. acknowledge grant Refs. PID2021-125081NB-I00 andPID2024-158030NB-I00 were financed by MCIN/AEI/10.13039/501100011033 and FEDER EU, and Universidadde Huelva (P.O. FEDER EPIT1282023), also co-financed byEU FEDER funds. F.J.B. and J.A. also acknowledge resourcesprovided by Supercomputing and Bioinnovation Center of theUniversity of Malaga in Picasso under Grant No. FI-2024-1-0017, Barcelona Supercomputing Center in Mare Nostrumunder Grants No. FI-2023-2-0041 and FI-2023-3-0001, andCentro de Supercomputación de Galicia (CESGA, Santiago deCompostela, Spain)
DS Repositorio Institucional de la Universidad de Huelva
RD 30 may 2026