Small Polarons and Surface Defects in Metal Oxide Photocatalysts Studied Using XUV Reflection–Absorption Spectroscopy

Bandaranayake, Savini; Hruska, Emily; Londo, Stephen; Biswas, Somnath; Baker, L. Robert

doi:10.1021/acs.jpcc.0c07047

Small Polarons and Surface Defects in Metal Oxide Photocatalysts Studied Using XUV Reflection–Absorption Spectroscopy

Journal Article · Tue Sep 29 00:00:00 EDT 2020 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.0c07047· OSTI ID:1660432

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The Ohio State Univ., Columbus, OH (United States); The Ohio State University
The Ohio State Univ., Columbus, OH (United States)

In photocatalytic transition metal oxides, the surface electronic structure and carrier kinetics are complicated by both charge trapping at defects and self-trapping by small polaron formation. These effects are specific to both the material and the type of defect or surface states involved. Here we review recent studies on ultrafast photoexcited charge carrier dynamics at the surfaces of alpha-Fe₂O₃ (hematite) and NiO and at the interface of a alpha-Fe₂O₃/NiO heterojunction using extreme ultraviolet (XUV) reflection-absorption spectroscopy. We study dynamics of small polaron formation at hematite surfaces showing that the rate of carrier self-trapping is slower than in the bulk due to a greater lattice reorganization energy required for surface polaron formation. We also show that surface dynamics of hematite can be systematically tuned to control carrier transport properties through surface functionalization. To better understand the impact of defects on carrier events, we study charge carrier recombination of NiO. It is shown that O vacancies have no detrimental effect on carrier lifetime while grain boundaries cause fast recombination. Finally, we study a model heterojunction consisting of alpha-Fe₂O₃ and NiO and find that interfacial charge transfer across these two materials occurs by a two-step mechanism where the interfacial electric field drives fast exciton dissociation followed by hole injection from alpha-Fe2O3 to NiO. Finally, these examples illustrate future opportunities to observe surface electron dynamics in photocatalytic materials with element and chemical state resolution using ultrafast XUV spectroscopy.

View Accepted Manuscript (DOE)

Research Organization:: The Ohio State Univ., Columbus, OH (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; US Air Force Office of Scientific Research (AFOSR)

Grant/Contract Number:: SC0014051

OSTI ID:: 1660432

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 42 Vol. 124; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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