An $\text{ab-initio}$ effective solid state photoluminescence by frequency constraint of cluster calculation

Abstract

Measuring the photoluminescence of defects in crystals is a common experimental technique for analysis and identification. However, current theoretical simulations typically require the simulation of a large number of atoms to eliminate finite size effects, which discourages computationally expensive excited state methods. We show how to extract the room-temperature photoluminescence spectra of defect centres in bulk from an $\text{ab-initio}$ simulation of a defect in small clusters. The finite size effect of small clusters manifests as strong coupling to low frequency vibrational modes. We find that removing vibrations below a cutoff frequency determined by constrained optimization returns the main features of the solid state photoluminescence spectrum. This strategy is illustrated for an NV${}^{-}$ defect in diamond, presenting a connection between defects in solid state and clusters; the first vibrationally resolved $\text{ab-initio}$ photoluminescence spectrum of an NV${}^{-}$ defect in a nanodiamond; and an alternative technique for simulating photoluminescence for solid state defects utilizing more accurate excited state methods.

arXiv commentAccepted for publication in the Journal of Applied Physics

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Cited by in corpus (4)

• Photoluminescence spectra of point defects in semiconductors: validation of first principles calculations
• Excited state properties of point defects in semiconductors and insulators investigated with time-dependent density functional theory
• The $N_{2}V$ color center: a ubiquitous visible and near-infrared-II quantum emitter in nitrogen-doped diamond
• Modified coherence of quantum spins in a damped pure-dephasing model