Delocalization of dark and bright excitons in flat-band materials and the optical properties of V2O5

Vitaly Gorelov, Lucia Reining, Martin Feneberg, Rüdiger Goldhahn, André Schleife, Walter R.L. Lambrecht, Matteo Gatti

Research output: Contribution to journalArticlepeer-review

Abstract

The simplest picture of excitons in materials with atomic-like localization of electrons is that of Frenkel excitons, where electrons and holes stay close together, which is associated with a large binding energy. Here, using the example of the layered oxide V2O5, we show how localized charge-transfer excitations combine to form excitons that also have a huge binding energy but, at the same time, a large electron-hole distance, and we explain this seemingly contradictory finding. The anisotropy of the exciton delocalization is determined by the local anisotropy of the structure, whereas the exciton extends orthogonally to the chains formed by the crystal structure. Moreover, we show that the bright exciton goes together with a dark exciton of even larger binding energy and more pronounced anisotropy. These findings are obtained by combining first principles many-body perturbation theory calculations, ellipsometry experiments, and tight binding modelling, leading to very good agreement and a consistent picture. Our explanation is general and can be extended to other materials.

Original languageEnglish (US)
Article number94
Journalnpj Computational Materials
Volume8
Issue number1
DOIs
StatePublished - Dec 2022

ASJC Scopus subject areas

  • Modeling and Simulation
  • Materials Science(all)
  • Mechanics of Materials
  • Computer Science Applications

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