Photoluminescence Lineshapes for Color Centers in Silicon Carbide from Density Functional Theory Calculations

Hashemi, Arsalan; Linderalv, Christopher; Krasheninnikov, Arkady V.; Ala-Nissila, Tapio; Erhart, Paul; Komsa, Hannu-Pekka

doi:10.48550/arxiv.2010.01508

Cited by 1 publication

(2 citation statements)

References 59 publications

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“…The calculation of these spectral functions is difficult for two main reasons. The first reason is that the evaluation of overlap integrals χ a1 e0 χ a1 gp or χ a1 es χ a1 g0 entering equations (13) and ( 15) is computationally very challenging, since, generally speaking, normal modes in the ground and the excited state will not be identical. The two sets of modes are related via the so-called Duschinsky transformation.…”

Section: Coupling To A1 Modes a General Formulationmentioning

confidence: 99%

“…11 A few other recent studies have calculated optical lineshapes of point defects. [12][13][14] Most of the published work used fairly small supercells, which yields an incomplete description of the phonon spectrum. It can be concluded that the status of calculations of optical lineshapes of point defects defects is much behind that of molecules where very accurate calculations are now being routinely performed.…”

Section: Introductionmentioning

confidence: 99%

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Vibrational and vibronic structure of isolated point defects: the nitrogen-vacancy center in diamond

Razinkovas,

Doherty,

Manson

et al. 2020

Preprint

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We present a theoretical study of vibrational and vibronic properties of a point defect in the dilute limit by means of first-principles density functional theory calculations. As an exemplar we choose the negatively charged nitrogen-vacancy center, a solid-state system that has served as a testbed for many protocols of quantum technology. We achieve low effective concentrations of defects by constructing dynamical matrices of large supercells containing tens of thousands of atoms. The main goal of the paper is to calculate luminescence and absorption lineshapes due to coupling to vibrational degrees of freedom. The coupling to symmetric a1 modes is computed via the Huang-Rhys theory. Importantly, to include a nontrivial contribution of e modes we develop an effective methodology to solve the multi-mode E ⊗ e Jahn-Teller problem. Our results show that for NV centers in diamond a proper treatment of e modes is particularly important for absorption. We obtain good agreement with experiment for both luminescence and absorption. Finally, the remaining shortcomings of the theoretical approach are critically reviewed. The presented theoretical approach will benefit identification and future studies of point defects in solids.I.

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Section: Coupling To A1 Modes a General Formulationmentioning

confidence: 99%