Contribution of the density-functional-based tight-binding scheme to the description of water clusters: methods, applications and extension to bulk systems

ABSTRACT

This review is dedicated to the application of the self-consistent-charge density-functional-based tight-binding (SCC-DFTB) approach to describe the structures, energetics, thermodynamic and spectral properties of water clusters, in the context of both fundamental and applied studies. We first present modifications implemented in the parametrisation of the potential that is mandatory to describe molecular aggregates as well as methods for global optimisation and determination of macroscopic properties. Then a number of applications of atmospherical and astrophysical interest, involving collaborations between theoreticians and experimentalists, are discussed to exemplify past and present contributions of SCC-DFTB to those two domains. Most applications presented in this review take advantage of the computational efficiency of SCC-DFTB to conduct extensive molecular dynamics simulations to obtain spectral and thermodynamic properties of water clusters. We also show some new results related to ongoing studies on both water clusters with impurities and liquid water.

KEYWORDS:

• SCC-DFTB
• water
• clusters
• molecular dynamics

Acknowledgments

We acknowledge the computing mesocenter CALMIP ‘Unité Mixte de Service du CNRS’ (UMS CNRS 3667) in Toulouse for generous allocation of computer resources (p0059, p1320 and p17002).

Disclosure statement

No potential conflict of interest was reported by the authors.

ORCID

A. Simon http://orcid.org/0000-0002-2315-9490

J. Cuny http://orcid.org/0000-0002-7882-9156

Additional information

Funding

This work has been funded by the Agence Nationale de la Recherche (ANR) project grant [ANR-13- BS08-0005] “PARCS” (Polycyclic Aromatic Hydrocarbons Reactivity in Cryogenic Solids)”, with support from the French research network EMIE (Edifices Moléculaires Isolés et Environnés, GDR 3533 of CNRS). It has also been partially supported through the NEXT (Nano, mesures EXtrêmes, Théorie) grant [ANR-10-LABX-0037] in the framework of the ”Programme des Investissements d'Avenir”.