Muralidhar Nalabothula

Davide Sangalli

Fulvio Paleari

Sven Reichardt

Ludger Wirtz

Excitons, bound electron-hole pairs, are responsible for strong optical resonances near the bandgap in low-dimensional materials and wide-bandgap insulators. Although current ab initio methods can accurately determine exciton energies and eigenstates, their symmetries have been much less explored. In this work, we employ standard group-theory methods to analyse the transformation properties of excitonic states, obtained by solving the BSE, under crystal symmetry operations. We develop an approach to assign irreducible-representation labels to excitonic states, providing a state-of-the-art framework for analysing their symmetries and selection rules (including, for example, the case of exciton-phonon coupling). Complementary to the symmetry classification, we introduce the concept of total crystal angular momentum for excitons in the presence of rotational symmetries, allowing the derivation of conservation laws. Furthermore, we demonstrate how these symmetry properties can be exploited to greatly enhance the computational efficiency of exciton calculations with the BSE. We apply our methodology to three prototypical systems to understand the role of symmetries in different contexts: (i) For LiF, we present the symmetry analysis of the entire excitonic dispersion and examine the selection rules for optical absorption. (ii) In the calculation of resonant Raman spectra of monolayer MoSe2, we demonstrate how the conservation of total crystal angular momentum governs exciton-phonon interactions, leading to the observed resonant enhancement. (iii) In bulk hBN, we analyze the role of symmetries for the coupling of finite-momentum excitons to finite-momentum phonons and their manifestation in the phonon-assisted luminescence spectra. This work establishes a general and robust framework for understanding the symmetry properties of excitons in crystals, providing a foundation for future studies.

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