ZNO (10-10) SURFACE SENSITIZED WITH CYANOACRYLATED TERTHIOPHENE: A THEORETICAL INVESTIGATION OF THE PHOTO-EXCITED CHARGE-TRANSFER

Published in 12/12/2023 - ISBN: 978-65-272-0088-8

Paper Title
ZNO (10-10) SURFACE SENSITIZED WITH CYANOACRYLATED TERTHIOPHENE: A THEORETICAL INVESTIGATION OF THE PHOTO-EXCITED CHARGE-TRANSFER
Authors
  • Vinicius Alves Bastos
  • Tales José da Silva
  • Marilia Junqueira Caldas
Modality
Pôster
Subject area
Simulação computacional / Teoria
Publishing Date
12/12/2023
Country of Publishing
Brasil
Language of Publishing
Inglês
Paper Page
https://www.even3.com.br/anais/workshop-do-ineo-2023/611890-zno-(10-10)-surface-sensitized-with-cyanoacrylated-terthiophene--a-theoretical-investigation-of-the-photo-excited
ISBN
978-65-272-0088-8
Keywords
Dye-Sensitized Solar Cells, charge transfer, ZnO, oligothiophenes, DFT, GW, BSE
Summary
Dye-Sensitized Solar Cells (DSSCs) are an important class of photovoltaic devices in which the electron-transporting layer is sensitized by an organic dye to facilitate the charge transfer of electrons photo-generated in the active layer. Recently, Oerhlein et. al. [1] have investigated ZnO nanocrystals sensitized by cyanoacrylated oligothiophene molecules (nTCs), for application in DSSCs, and reported molecule-to-surface photo-excited charge transfer. Motivated by this work, we have performed a theoretical investigation of the ZnO (10-10) surface [2] functionalized by a cyanoacrylated terthiophene molecule (3TC), covering first the isolated systems, i.e., molecule and surface, proceeding to the chemically bonded system (3TC@ZnO). We adopted the local basis formulation of Density Functional Theory as implemented in the FHI-aims code [3] for treating the isolated 3TC, and the planewave formulation in the Quantum Espresso code [4] for the ZnO surface and the 3TC@ZnO bonded system. The PBE exchange-correlation functional [5] was used in the geometry optimizations and electronic structure calculations, and the PBE0 [6] for the final electronic structure analyses. Specifically for the isolated 3TC, we further performed a BSE-GW calculation [7] using FHI-aims on top of the PBE0 ground state. We find that 3TC displays a strong optical excitation around 2.7eV, due to the HOMO?LUMO transition, with the HOMO localized on the 3T part and the LUMO on the C termination, then characterizing a donor-acceptor system. Regarding the 3TC@ZnO, we obtained from the structural calculations a molecule-surface binding energy of -2.26eV, indicating stable chemical bonding [8]. The electronic structure results present appropriate molecule-substrate energy level alignment, i.e., the HOMO in the middle of the gap and the LUMO in the conduction band, and molecule-to-surface charge extension of the LUMO state. In summary, the 3TC@ZnO system shows encouraging features for application in DSSCs. [1] A. N. Oerhlein et al., Phys. Chem. Chem. Phys. 21, 6991 (2019); [2] A. Dominguez et al., J. Appl. Phys. 115, 203720 (2014); [3] V. Blum et al., Comput. Phys. Commun. 180, 2175 (2009); [4] P. Giannozzi et al., J. Phys. Condens. Matter. 21, 395502 (2009); [5] J. P. Perdew, K. Burke, and M. Ernzerhof, Phys. Rev. Lett. 77, 3865 (1996); [6] C. Adamo and V. Barone, J. Chem. Phys. 110, 6158 (1999); [7] C. Liu et al., J. Chem. Phys. 152, 044105 (2020); [8] I. Arbouch et al., Phys. Chem. Chem. Phys. 19, 29389 (2017). The authors thank HPC-USP and CENAPAD-SP for computational resources, and CNPq and INCT-INEO for financial support.
Title of the Event
Workshop do INEO 2023
City of the Event
Nazaré Paulista
Title of the Proceedings of the event
Anais do Workshop INEO 2023
Name of the Publisher
Even3
Means of Dissemination
Meio Digital
DOI
LinkGet DOI

How to cite

BASTOS, Vinicius Alves; SILVA, Tales José da; CALDAS, Marilia Junqueira. ZNO (10-10) SURFACE SENSITIZED WITH CYANOACRYLATED TERTHIOPHENE: A THEORETICAL INVESTIGATION OF THE PHOTO-EXCITED CHARGE-TRANSFER.. In: Anais do workshop INEO 2023. Anais...Nazaré Paulista(SP) Hotel Estância Atibainha, 2023. Available in: https//www.even3.com.br/anais/workshop-do-ineo-2023/611890-ZNO-(10-10)-SURFACE-SENSITIZED-WITH-CYANOACRYLATED-TERTHIOPHENE--A-THEORETICAL-INVESTIGATION-OF-THE-PHOTO-EXCITED. Access in: 23/06/2024

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