The relevance of structural variability in the time-domain for computational reflection anisotropy spectroscopy at solid-liquid interfaces.
J Phys Condens Matter
; 36(18)2024 Feb 06.
Article
en En
| MEDLINE
| ID: mdl-38253003
ABSTRACT
In electrochemistry, reactions and charge-transfer are to a large extent determined by the atomistic structure of the solid-liquid interface. Yet due to the presence of the liquid electrolyte, many surface-science methods cannot be applied here. Hence, the exact microscopic structure that is present under operating conditions often remains unknown. Reflection anisotropy spectroscopy (RAS) is one of the few techniques that allow for anin operandoinvestigation of the structure of solid-liquid interfaces. However, an interpretation of RAS data on the atomistic scale can only be obtained by comparison to computational spectroscopy. While the number of computational RAS studies related to electrochemical systems is currently still limited, those studies so far have not taken into account the dynamic nature of the solid-liquid interface. In this work, we investigate the temporal evolution of the spectroscopic response of the Au(110) missing row reconstruction in contact with water by combiningab initiomolecular dynamics with computational spectroscopy. Our results show significant changes in the time evolution of the RA spectra, in particular providing an explanation for the typically observed differences in intensity when comparing theory and experiment. Moreover, these findings point to the importance of structural surface/interface variability while at the same time emphasising the potential of RAS for probing these dynamic interfaces.
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1
Colección:
01-internacional
Base de datos:
MEDLINE
Idioma:
En
Revista:
J Phys Condens Matter
Asunto de la revista:
BIOFISICA
Año:
2024
Tipo del documento:
Article
País de afiliación:
Alemania