Density-functional Tight-binding: Basic Concepts and Applications to Molecules and Clusters

Overview

Journal Adv Phys X

Date 2020 Nov 6

PMID 33154977

Citations 18

Authors

Fernand Spiegelman

Nathalie Tarrat

Jerome Cuny

Leo Dontot

Evgeny Posenitskiy

Carles Marti

Aude Simon

Mathias Rapacioli

Affiliations

Soon will be listed here.

Abstract

The scope of this article is to present an overview of the Density Functional based Tight Binding (DFTB) method and its applications. The paper introduces the basics of DFTB and its standard formulation up to second order. It also addresses methodological developments such as third order expansion, inclusion of non-covalent interactions, schemes to solve the self-interaction error, implementation of long-range short-range separation, treatment of excited states the time-dependent DFTB scheme, inclusion of DFTB in hybrid high-level/low level schemes (DFT/DFTB or DFTB/MM), fragment decomposition of large systems, large scale potential energy landscape exploration with molecular dynamics in ground or excited states, non-adiabatic dynamics. A number of applications are reviewed, focusing on -(i)- the variety of systems that have been studied such as small molecules, large molecules and biomolecules, bare orfunctionalized clusters, supported or embedded systems, and -(ii)- properties and processes, such as vibrational spectroscopy, collisions, fragmentation, thermodynamics or non-adiabatic dynamics. Finally outlines and perspectives are given.

Citing Articles

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References

Nishimoto Y . DFTB/PCM Applied to Ground and Excited State Potential Energy Surfaces. J Phys Chem A. 2016; 120(5):771-84. DOI: 10.1021/acs.jpca.5b10732. View

Simon A, Rapacioli M, Mascetti J, Spiegelman F . Vibrational spectroscopy and molecular dynamics of water monomers and dimers adsorbed on polycyclic aromatic hydrocarbons. Phys Chem Chem Phys. 2012; 14(19):6771-86. DOI: 10.1039/c2cp40321h. View

Kranz J, Kubillus M, Ramakrishnan R, Anatole von Lilienfeld O, Elstner M . Generalized Density-Functional Tight-Binding Repulsive Potentials from Unsupervised Machine Learning. J Chem Theory Comput. 2018; 14(5):2341-2352. DOI: 10.1021/acs.jctc.7b00933. View

Chakarova-Kack S, Schroder E, Lundqvist B, Langreth D . Application of van der Waals density functional to an extended system: adsorption of benzene and naphthalene on graphite. Phys Rev Lett. 2006; 96(14):146107. DOI: 10.1103/PhysRevLett.96.146107. View

Kubar T, Bodrog Z, Gaus M, Kohler C, Aradi B, Frauenheim T . Parametrization of the SCC-DFTB Method for Halogens. J Chem Theory Comput. 2015; 9(7):2939-49. DOI: 10.1021/ct4001922. View

Torquato P, Giusepponi D, Alisi A, Galarini R, Bartolini D, Piroddi M . Nutritional and lipidomics biomarkers of docosahexaenoic acid-based multivitamin therapy in pediatric NASH. Sci Rep. 2019; 9(1):2045. PMC: 6375912. DOI: 10.1038/s41598-018-37209-y. View

Keceli M, Zhang H, Zapol P, Dixon D, Wagner A . Shift-and-invert parallel spectral transformation eigensolver: Massively parallel performance for density-functional based tight-binding. J Comput Chem. 2015; 37(4):448-59. DOI: 10.1002/jcc.24254. View

Kubillus M, Kubar T, Gaus M, rezac J, Elstner M . Parameterization of the DFTB3 method for Br, Ca, Cl, F, I, K, and Na in organic and biological systems. J Chem Theory Comput. 2016; 11(1):332-42. DOI: 10.1021/ct5009137. View

Douglas-Gallardo O, Soldano G, Mariscal M, Sanchez C . Effects of oxidation on the plasmonic properties of aluminum nanoclusters. Nanoscale. 2017; 9(44):17471-17480. DOI: 10.1039/c7nr04904h. View

10.

Tapavicza E, Tavernelli I, Rothlisberger U . Trajectory surface hopping within linear response time-dependent density-functional theory. Phys Rev Lett. 2007; 98(2):023001. DOI: 10.1103/PhysRevLett.98.023001. View

11.

Negre C, Young K, Oviedo M, Allen L, Sanchez C, Jarzembska K . Photoelectrochemical hole injection revealed in polyoxotitanate nanocrystals functionalized with organic adsorbates. J Am Chem Soc. 2014; 136(46):16420-9. DOI: 10.1021/ja509270f. View

12.

Korchagina K, Simon A, Rapacioli M, Spiegelman F, Cuny J . Structural Characterization of Sulfur-Containing Water Clusters Using a Density-Functional Based Tight-Binding Approach. J Phys Chem A. 2016; 120(45):9089-9100. DOI: 10.1021/acs.jpca.6b08251. View

13.

Kubar T, Kleinekathofer U, Elstner M . Solvent fluctuations drive the hole transfer in DNA: a mixed quantum-classical study. J Phys Chem B. 2009; 113(39):13107-17. DOI: 10.1021/jp9073587. View

14.

Zimmerli U, Parrinello M, Koumoutsakos P . Dispersion corrections to density functionals for water aromatic interactions. J Chem Phys. 2004; 120(6):2693-9. DOI: 10.1063/1.1637034. View

15.

Oberg K . Photochemistry and Astrochemistry: Photochemical Pathways to Interstellar Complex Organic Molecules. Chem Rev. 2016; 116(17):9631-63. DOI: 10.1021/acs.chemrev.5b00694. View

16.

Radziuk D, Mohwald H . Ultrasonically treated liquid interfaces for progress in cleaning and separation processes. Phys Chem Chem Phys. 2015; 18(1):21-46. DOI: 10.1039/c5cp05142h. View

17.

Dion M, Rydberg H, Schroder E, Langreth D, Lundqvist B . van der Waals density functional for general geometries. Phys Rev Lett. 2004; 92(24):246401. DOI: 10.1103/PhysRevLett.92.246401. View

18.

Dontot L, Spiegelman F, Rapacioli M . Structures and Energetics of Neutral and Cationic Pyrene Clusters. J Phys Chem A. 2019; 123(44):9531-9543. PMC: 6917508. DOI: 10.1021/acs.jpca.9b07007. View

19.

Nishizawa H, Nishimura Y, Kobayashi M, Irle S, Nakai H . Three pillars for achieving quantum mechanical molecular dynamics simulations of huge systems: Divide-and-conquer, density-functional tight-binding, and massively parallel computation. J Comput Chem. 2016; 37(21):1983-92. DOI: 10.1002/jcc.24419. View

20.

Witek H, Morokuma K, Stradomska A . Modeling vibrational spectra using the self-consistent charge density-functional tight-binding method. I. Raman spectra. J Chem Phys. 2004; 121(11):5171-8. DOI: 10.1063/1.1775787. View