Impact of hole polaron formation on excitonic transitions in MgO from first principles

Nabi, A. Sameer; Sharifzadeh, Sahar

doi:10.1103/mpb2-3wrb

Impact of hole polaron formation on excitonic transitions in MgO from first principles

Journal Article · Thu Dec 18 00:00:00 EST 2025 · Physical Review Materials

DOI:https://doi.org/10.1103/mpb2-3wrb· OSTI ID:3011354

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Boston Univ., MA (United States)

Here, we present a first-principles investigation of the excitonic properties of magnesia (MgO), an ionic insulator known to host hole polarons. We combine a density functional theory-based approach for structural relaxation in the presence of the hole and many-body perturbation theory to describe the excitonic properties. We determine that the hole polaron introduces new in-gap occupied states 0.6–0.8 eV above the valence band maximum that lead to two low-energy peaks in the optical spectrum. The predicted redshift of the lowest-energy transition due to polaron formation of 0.8 eV agrees well with the experimental Stokes shift of 0.8–0.9 eV. Analysis of the exciton wave function indicates that the electron-hole pair consists of a localized hole and delocalized electron, but that the wave function retains its Wannier-Mott character even in the presence of the hole polaron. Our study demonstrates that combining these previously established methods allows for a relatively computationally inexpensive approach to studying the exciton polaron in materials where only one charge carrier forms a polaron.

View Accepted Manuscript (DOE)

Research Organization:: Boston Univ., MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; SC0023402

OSTI ID:: 3011354

Journal Information:: Physical Review Materials, Journal Name: Physical Review Materials Journal Issue: 12 Vol. 9; ISSN 2475-9953

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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