SCC-DFTB parameters for simulating hybrid gold-thiolates compounds.
We present a parametrization of a self-consistent charge density functional-based tight-binding scheme (SCC-DFTB) to describe gold-organic hybrid systems by adding new Au-X (X = Au, H, C, S, N, O) parameters to a previous set designed for organic molecules. With the aim of describing gold-thiolates systems within the DFTB framework, the resulting parameters are successively compared with density functional theory (DFT) data for the description of Au bulk, Aun gold clusters (n = 2, 4, 8, 20), and Aun SCH3 (n = 3 and 25) molecular-sized models. The geometrical, energetic, and electronic parameters obtained at the SCC-DFTB level for the small Au3 SCH3 gold-thiolate compound compare very well with DFT results, and prove that the different binding situations of the sulfur atom on gold are correctly described with the current parameters. For a larger gold-thiolate model, Au25 SCH3 , the electronic density of states and the potential energy surfaces resulting from the chemisorption of the molecule on the gold aggregate obtained with the new SCC-DFTB parameters are also in good agreement with DFT results.
Laboratoire Interfaces, Traitements, Organisation Et Dynamique Des Systèmes (ITODYS), CNRS UMR 7086, Université Paris Diderot Sorbonne Paris Cité, Bâtiment Lavoisier, 15 Rue Jean Antoine De Baïf, Paris Cedex 13, 75205, France.
Arnaud
A
Fihey
Bremen Center for Computational Materials Science (BCCMS), Universität Bremen, Am Fallturm 1, Bremen, 28359, Germany.
Christian
C
Hettich
Laboratoire Interfaces, Traitements, Organisation Et Dynamique Des Systèmes (ITODYS), CNRS UMR 7086, Université Paris Diderot Sorbonne Paris Cité, Bâtiment Lavoisier, 15 Rue Jean Antoine De Baïf, Paris Cedex 13, 75205, France.
Jérémy
J
Touzeau
Laboratoire Interfaces, Traitements, Organisation Et Dynamique Des Systèmes (ITODYS), CNRS UMR 7086, Université Paris Diderot Sorbonne Paris Cité, Bâtiment Lavoisier, 15 Rue Jean Antoine De Baïf, Paris Cedex 13, 75205, France.
François
F
Maurel
Laboratoire Interfaces, Traitements, Organisation Et Dynamique Des Systèmes (ITODYS), CNRS UMR 7086, Université Paris Diderot Sorbonne Paris Cité, Bâtiment Lavoisier, 15 Rue Jean Antoine De Baïf, Paris Cedex 13, 75205, France.
Aurélie
A
Perrier
Bremen Center for Computational Materials Science (BCCMS), Universität Bremen, Am Fallturm 1, Bremen, 28359, Germany.
Christof
C
Köhler
Bremen Center for Computational Materials Science (BCCMS), Universität Bremen, Am Fallturm 1, Bremen, 28359, Germany.
Bálint
B
Aradi
Bremen Center for Computational Materials Science (BCCMS), Universität Bremen, Am Fallturm 1, Bremen, 28359, Germany.
Thomas
T
Frauenheim
chemisorption; density functional theory; gold cluster; potential energy surface; thiolate molecule; tight-binding