Photochemical anisotropy and direction-dependent optical absorption properties in semiconductors

Photochemical reactions on semiconductors are anisotropic, since they occur with different rates on surfaces of different orientation. Understanding the origin of this anisotropy is crucial to engineering more efficient photocatalysts. In this work, we use hybrid density functional theory (DFT) to identify the surfaces associated with the largest number of photo-generated carriers in different semiconductors. For each material we create a spherical heat map of the probability of optical transitions at different wave vectors. These maps allow to identify the directions associated with the majority of the photo-generated carriers and can thus be used to make predictions about the most reactive surfaces for photochemical applications. Results indicate that it is generally possible to correlate the heat maps with the anisotropy of the bands observed in conventional band-structure plots, as previously suggested. However, we also demonstrate that conventional bands-structure plots do not always provide all the informations and that taking into account the contribution of all possible transitions weighted by their transition dipole moments is crucial to obtain a complete picture.

Identifier
Source https://archive.materialscloud.org/record/2022.23
Metadata Access https://archive.materialscloud.org/xml?verb=GetRecord&metadataPrefix=oai_dc&identifier=oai:materialscloud.org:1246
Provenance
Creator Ricca, Chiara; Aschauer, Ulrich
Publisher Materials Cloud
Publication Year 2022
Rights info:eu-repo/semantics/openAccess; Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode
OpenAccess true
Contact archive(at)materialscloud.org
Representation
Language English
Resource Type Dataset
Discipline Materials Science and Engineering