Lifetime effects and satellites in the photoelectron spectrum of tungsten metal

Autor: C. Kalha, L. E. Ratcliff, J. J. Gutiérrez Moreno, S. Mohr, M. Mantsinen, N. K. Fernando, P. K. Thakur, T.-L. Lee, H.-H. Tseng, T. S. Nunney, J. M. Kahk, J. Lischner, A. Regoutz
Přispěvatelé: Barcelona Supercomputing Center
Jazyk: angličtina
Rok vydání: 2022
Předmět:
Zdroj: UPCommons. Portal del coneixement obert de la UPC
Universitat Politècnica de Catalunya (UPC)
Popis: Tungsten (W) is an important and versatile transition metal and has a firm place at the heart of many technologies. A popular experimental technique for the characterization of tungsten and tungsten-based compounds is x-ray photoelectron spectroscopy (XPS), which enables the assessment of chemical states and electronic structure through the collection of core level and valence band spectra. However, in the case of tungsten metal, open questions remain regarding the origin, nature, and position of satellite features that are prominent in the photoelectron spectrum. These satellites are a fingerprint of the electronic structure of the material and have not been thoroughly investigated, at times leading to their misinterpretation. The present work combines high-resolution soft and hard x-ray photoelectron spectroscopy (SXPS and HAXPES) with reflected electron energy loss spectroscopy (REELS) and a multitiered ab initio theoretical approach, including density functional theory (DFT) and many-body perturbation theory (G0W0 and GW + C ), to disentangle the complex set of experimentally observed satellite features attributed to the generation of plasmons and interband transitions. This combined experiment-theory strategy is able to uncover previously undocumented satellite features, improving our understanding of their direct relationship to tungsten's electronic structure. Furthermore, it lays the groundwork for future studies into tungsten-based mixed-metal systems and holds promise for the reassessment of the photoelectron spectra of other transition and post-transition metals, where similar questions regarding satellite features remain. CK acknowledges the support from the Department of Chemistry, UCL. NKF acknowledges support from the Engineering and Physical Sciences Research Council (EP/L015277/1). AR acknowledges the support fromthe Analytical Chemistry Trust Fund for her CAMS-UK Fellowship. LER acknowledges support from an EPSRC Early Career Research Fellowship (EP/P033253/1). JL and JMK acknowledge funding from EPSRC under Grant No. EP/R002010/1 and from a Royal Society University Research Fellowship (URF/R/191004). This work used the ARCHER UK National Supercomputing Service via JL’s membership of the HEC Materials Chemistry Consortium of UK, which is funded by EPSRC (EP/L000202). JJGM and SM acknowledge the support from the FusionCAT project (001-P-001722) cofinanced by the European Union Regional Development Fund within the framework of the ERDF Operational Program of Catalonia 2014-2020 with a grant of 50% of total cost eligible, the access to computational resources at MareNostrum and the technical support provided by BSC (RES-QS-2020-3-0026). Part of this work was carried out using supercomputer resources provided under the EU-JA Broader Approach collaboration in the Computational Simulation Centre of International Fusion Energy Research Centre (IFERC-CSC) Peer Reviewed "Article signat per 13 autors/es: C. Kalha, L. E. Ratcliff, J. J. Gutiérrez Moreno, S. Mohr, M. Mantsinen, N. K. Fernando, P. K. Thakur, T.-L. Lee, H.-H. Tseng, T. S. Nunney, J. M. Kahk, J. Lischner, and A. Regoutz"
Databáze: OpenAIRE
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