Electronic and Optical Properties of Alkaline Earth Metal Fluoride Crystals with the Inclusion of Many-Body Effects: A Comparative Study on Rutile MgF2 and Cubic SrF2

Cappellini, Giancarlo

First

Investigation

;Furthmüller, Jürgen

Second

Software

;Bechstedt, Friedhelm

Penultimate

Writing - Review & Editing

;Botti, Silvana

Last

Writing - Review & Editing

2023-01-01

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Abstract

We conducted a systematic investigation using state-of-the-art techniques on the electronic and optical properties of two crystals of alkaline earth metal fluorides, namely rutile MgF2 and cubic SrF2 . For these two crystals of different symmetry, we present density functional theory (DFT), many-body perturbation theory (MBPT), and Bethe–Salpeter equation (BSE) calculations. We calculated a variety of properties, namely ground-state energies, band-energy gaps, and optical absorption spectra with the inclusion of excitonic effects. The quantities were obtained with a high degree of convergence regarding all bulk electronic and optical properties. Bulk rutile MgF2 has distinguished ground-state and excited-state properties with respect to the other cubic fluoride SrF2 and the other members of the alkaline earth metal fluoride family. The nature of the fundamental gaps and estimates of the self-energy and excitonic effects for the two compounds are presented and discussed in detail. Our results are in good accordance with the measurements and other theoretical–computational data. A comparison is made between the excitation and optical properties of bulk rutile MgF2 , cubic SrF2 , and the corresponding clusters, for which calculations have recently been published, confirming strong excitonic effects in finite-sized systems.