Modeling the Photochrome-TiO2Interface with Bethe-Salpeter and Time-Dependent Density Functional Theory Methods.
Hybrid organic-inorganic semiconductor systems have important applications in both molecular electronics and photoresponsive materials. The characterizations of the interface and of the electronic excited-states of these hybrid systems remain a challenge for state-of-the-art computational methods, as the systems of interest are large. In the present investigation, we present for the first time a many-body Green's function Bethe-Salpeter investigation of a series of photochromic molecules adsorbed onto TiO2nanoclusters. On the basis of these studies, the performance of time-dependent density functional theory (TD-DFT) calculations is assessed. In addition, the photochromic properties of different hybrid systems are also evaluated. This work shows that qualitatively different conclusions can be reached with TD-DFT relying on various exchange-correlation functionals for such organic-inorganic interfaces and paves the way to more accurate simulation of many hybrid materials.
CEISAM UMR CNRS 6230, Université de Nantes , 2 rue de la Houssinière, BP 92208, 44322 Nantes Cedex 3, France.
Daniel
D
Escudero
Univ. Grenoble Alpes, CEA, INAC-MEM, L-Sim , F-38000 Grenoble, France.|Univ. Grenoble Alpes, CNRS, Inst NEEL , F-38042 Grenoble, France.
Ivan
http://orcid.org/0000-0003-4713-1174
I
Duchemin
Univ. Grenoble Alpes, CNRS, Inst NEEL , F-38042 Grenoble, France.
Xavier
X
Blase
CEISAM UMR CNRS 6230, Université de Nantes , 2 rue de la Houssinière, BP 92208, 44322 Nantes Cedex 3, France.|Institut Universitaire de France , 1 rue Descartes, F-75005 Paris Cedex 05, France.
Denis
http://orcid.org/0000-0002-4217-0708
D
Jacquemin