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Structure and energetics of dye-sensitized NiO interfaces in water from ab-initio MD and large-scale GW calculations

Alekos Segalina1*, Sébastien Lèbegue1, Dario Rocca1, Simone Piccinin2*, Mariachiara Pastore1*

1 Université de Lorraine & CNRS, LPCT, UMR 7019, F-54000 Nancy, France

2 Consiglio Nazionale delle Ricerche, Istituto Officina dei Materiali, Trieste, Italy

* Corresponding authors emails: alekos.segalina@univ-lorraine.fr, piccinin@iom.cnr.it, mariachiara.pastore@univ-lorraine.fr
DOI10.24435/materialscloud:63-be [version v1]

Publication date: Jul 16, 2021

How to cite this record

Alekos Segalina, Sébastien Lèbegue, Dario Rocca, Simone Piccinin, Mariachiara Pastore, Structure and energetics of dye-sensitized NiO interfaces in water from ab-initio MD and large-scale GW calculations, Materials Cloud Archive 2021.108 (2021), doi: 10.24435/materialscloud:63-be.


The energy level alignment across solvated molecule/semiconductor interfaces is a crucial property for the correct functioning of dye-sensitized photo-electrodes, where, following the absorption of solar light, a cascade of interfacial hole/electron transfer processes has to efficiently take place. In light of the difficulty of performing X-ray photoelectron spectroscopy measurements at the molecule/solvent/metal-oxide interface, being able to accurately predict the level alignment by first-principles calculations on realistic structural models would represent an important step toward the optimization of the device. In this respect dye/NiO surfaces, employed in p-type dye-sensitized solar cells, are undoubtedly challenging for ab initio methods and, also for this reason, much less investigated than the n-type dye/TiO2 counterpart. Here we consider the C343-sensitized NiO surface in water and combine ab initio Molecular Dynamics (AIMD) simulations with GW (G0W0) calculations, performed along the MD trajectory, to reliably describe the structure and energetics of the interface when explicit solvation and finite temperature effects are accounted for. We show that the differential perturbative correction on the NiO and molecule states obtained at GW level is mandatory to recover the correct (physical) interfacial energetics, allowing hole transfer from the semiconductor valence band to the HOMO of the dye. Moreover, the calculated average driving force quantitatively agrees with the experimental estimate.

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File name Size Description
146.8 MiB AIMD production run of the C343@NiO(100) interface in explicit water. The simulation box, having dimensions 8.35X8.35X33.40 Å**3, consists of the C343@NiO interface and 42 water molecules. (gzip-compressed text file)


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Metadata, except for email addresses, are licensed under the Creative Commons Attribution Share-Alike 4.0 International license.

External references

Journal reference
A. Segalina, S. Lèbegue, D. Rocca, S. Piccinin, M. Pastore, J. Chem. Theory Comput., under review


ab initio molecular dynamics simulation p-type DSSC NiO C343@NiO interface energy level alignment GW

Version history:

2021.108 (version v1) [This version] Jul 16, 2021 DOI10.24435/materialscloud:63-be