Polaronic structure of excess electrons and holes for a series of bulk iron oxides

Autor:	Kevin M. Rosso, Christian S. Ahart, Jochen Blumberger
Rok vydání:	2020
Předmět:	Materials science Goethite General Physics and Astronomy Electron hole Electron Hematite engineering.material Polaron Hybrid functional Chemical physics visual_art visual_art.visual_art_medium engineering Physical and Theoretical Chemistry Lepidocrocite Spin (physics)
Zdroj:	Physical Chemistry Chemical Physics. 22:10699-10709
ISSN:	1463-9084 1463-9076
DOI:	10.1039/c9cp06482f
Popis:	Iron oxides such as hematite (α-Fe2O3) play an important role in diverse fields ranging from biogeochemistry to photocatalysis. Here we perform calculations of both the electron and electron hole polaron structures and associated reorganisation energies for a series of bulk iron oxides: hematite (α-Fe2O3), lepidocrocite (γ-FeOOH), goethite (α-FeOOH) and white rust (Fe(OH)2). Through the use of gap-optimized hybrid functionals and large supercells under periodic boundary conditions, we remove some of the complications and uncertainties present in earlier cluster model calculations. It is found that while the electron hole polaron in these materials generally localises onto a single iron site, the electron polaron localises across two iron sites of the same spin layer as a consequence of the lower reorganisation energy for electrons compared to holes. An exception to these trends is the hole of goethite, which according to our calculations does not form a localised polaron.
Databáze:	OpenAIRE
Externí odkaz:	https://explore.openaire.eu/search/publication?articleId=doi_dedup___::f2b98487bffe2abb9b070fed6b6e68f5 https://doi.org/10.1039/c9cp06482f Zobrazit plný text záznamu