Reference : Electronic structure of dye-sensitized TiO 2 clusters from many-body perturbation theory
Scientific journals : Article
Physical, chemical, mathematical & earth Sciences : Physics
http://hdl.handle.net/10993/25405
Electronic structure of dye-sensitized TiO 2 clusters from many-body perturbation theory
English
Marom, Noa [Center for Computational Materials, Institute for Computational Engineering and Sciences, The University of Texas at Austin, Austin, Texas 78712, USA]
Moussa, Jonathan E. [Center for Computational Materials, Institute for Computational Engineering and Sciences, The University of Texas at Austin, Austin, Texas 78712, USA]
Ren, Xinguo [Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195, Berlin, Germany]
Tkatchenko, Alexandre mailto [Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195, Berlin, Germany]
Chelikowsky, James R. [Center for Computational Materials, Institute for Computational Engineering and Sciences, The University of Texas at Austin, Austin, Texas 78712, USA > > > ; Departments of Physics and Chemical Engineering, The University of Texas at Austin, Austin, Texas 78712, USA]
2011
Physical Review. B: Condensed Matter and Materials Physics
American Physical Society
84
24
Yes (verified by ORBilu)
International
1098-0121
1550-235X
Woodbury
NY
[en] The development of new types of solar cells is driven by the need for clean and sustainable energy. In this respect dye-sensitized solar cells (DSC) are considered as a promising route for departing from the traditional solid state cells. The physical insight provided by computational modeling may help develop improved DSCs. To this end, it is important to obtain an accurate description of the electronic structure, including the fundamental gaps and level alignment at the dye-TiO2 interface. This requires a treatment beyond ground-state density functional theory (DFT). We present a many-body perturbation theory study, within the G(0)W(0) approximation, of two of the crystalline phases of dye-sensitized TiO2 clusters, reported by Benedict and Coppens, [J. Am. Chem. Soc. 132, 2938 (2010)]. We obtain geometries in good agreement with the experiment by using DFT with the Tkatchenko-Scheffler van der Waals correction. We demonstrate that even when DFT gives a good description of the valence spectrum and a qualitatively correct picture of the electronic structure of the dye-TiO2 interface, G(0)W(0) calculations yield more valuable quantitative information regarding the fundamental gaps and level alignment. In addition, we systematically investigate the issues pertaining to G(0)W(0) calculations, namely: (i) convergence with respect to the number of basis functions, (ii) dependence on the mean-field starting point, and (iii) the validity of the assumption that the DFT wave function is a good approximation to the quasiparticle wave function. We show how these issues are manifested for dye molecules and for dye-sensitized TiO2 clusters.
http://hdl.handle.net/10993/25405
10.1103/PhysRevB.84.245115

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