Theoretical Methods for Better Core Level Photoelectron Spectroscopy

Informations projet

THEOCORPES

N° de convention de subvention: 892943

DOI

10.3030/892943

Projet clôturé

Date de signature de la CE 4 Mars 2020

Date de début 1 Août 2021

Date de fin 30 Août 2023

Financé au titre de

• EXCELLENT SCIENCE - Marie Skłodowska-Curie Actions

Coût total

€ 154 193,28

Contribution de l’UE

€ 154 193,28

Coordonné par

TARTU ULIKOOL
Estonia

Periodic Reporting for period 1 - THEOCORPES (Theoretical Methods for Better Core Level Photoelectron Spectroscopy)

Période du rapport: 2021-08-01 au 2023-07-31

Résumé du contexte et des objectifs généraux du projet

Core level X-ray Photoelectron Spectroscopy (XPS) is an analytical technique for determining the chemical compositions of surfaces. It is widely used in both the academia and the industry. XPS is one of the primary methods used to study the fundamental mechanisms of processes such as heterogeneous catalysis, corrosion, and the preparation of protective or functional surface coatings. However, the analysis of recorded XPS spectra is sometimes very challenging. The aim of this project was to develop new and improved computational methods for modelling core level XPS, to enable XPS users to extract more useful information from their measurements.

Travail effectué depuis le début du projet jusqu’à la fin de la période considérée dans le rapport et principaux résultats atteints jusqu’à présent

This project was mainly focused on developing and extending the scope of the Δ-Self-Consistent-Field (ΔSCF) method for predicting core electron binding energies. In particular, work has been underway to enable ΔSCF calculations of core electron binding energies in a wider range of chemical elements that what was previously possible. Another key aim has been to further develop computational methods for modelling core level XPS in solids. In addition, together with collaborators, the ΔSCF approach and other computational methods have been used to aid the analysis and interpretation of experimental XPS measurements.

Progrès au-delà de l’état des connaissances et impact potentiel prévu (y compris l’impact socio-économique et les conséquences sociétales plus larges du projet jusqu’à présent)

(i) The prediction of absolute core electron binding energies in elements of the first transition series has been demonstrated. (ii) An improved method for predicting absolute core electron binding energies in solids has been presented – this method combines the ΔSCF approach with the GW method from many-body perturbation theory. (iii) Computational methods have been used to analyze in detail the photoelectron spectrum of tungsten metal. (iv) In collaboration with J. Lischner from Imperial College London, an approach for predicting X-ray absorption spectra (XAS) of molecules that combines the ΔSCF approach with time-dependent density functional theory has been developed. (v) Results from this project have been presented at major international conferences and workshops including the 2023 March meeting of the American Physical Society, the Psi-k 2022 conference in Lausanne, and the Faraday discussion on photoelectron spectroscopy and the future of surface analysis, London 2022.

Graphical abstract of Kahk et al., J. Chem. Theory Comput. 19, 3276 (2023)