Spectroscopic signatures of nonpolarons: the case of diamond.

Phys Chem Chem Phys

nanomat/Q-MAT/CESAM and European Theoretical Spectroscopy Facility, Université de Liège, B-4000, Belgium.

Published: May 2022

Polarons are quasi-particles made from electrons interacting with vibrations in crystal lattices. They derive their name from the strong electron-vibration polar interactions in ionic systems, that induce spectroscopic and optical signatures of such quasi-particles. In this paper, we focus on diamond, a non-polar crystal with inversion symmetry which nevertheless shows interesting signatures stemming from electron-vibration interactions, better denoted "nonpolaron" signatures in this case. The (non)polaronic effects are produced by short-range crystal fields, while long-range quadrupoles only have a small influence. The corresponding many-body spectral function has a characteristic energy dependence, showing a plateau structure that is similar to but distinct from the satellites observed in the polar Fröhlich case. We determine the temperature-dependent spectral function of diamond by two methods: the standard Dyson-Migdal approach, which calculates electron-phonon interactions within the lowest-order expansion of the self-energy, and the cumulant expansion, which includes higher orders of electron-phonon interactions. The latter corrects the nonpolaron energies and broadening, providing a more realistic spectral function, which we examine in detail for both conduction and valence band edges.

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http://dx.doi.org/10.1039/d2cp01012gDOI Listing

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