2024/03/12 by Louis Alaerts, Yihuang Xiong, Alaerts, Louis +5
Earth and Planetary Sciences · Materials Science · Physics and Astronomy · #Cold Atom Physics and Bose-Einstein Condensates #Diamond and Carbon-based Materials Research #FOS: Physical sciences #High-pressure geophysics and materials #Materials Science (cond-mat.mtrl-sci)
paper · pdf · doi:10.48550/arxiv.2403.07771
openalex publication_date 2024/03/12 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/31
Point defects in semiconductors are attractive candidates for quantum information science applications owing to their ability to act as spin-photon interface or single-photon emitters. However, the coupling between the change of dipole moment upon electronic excitation and stray electric fields in the vicinity of the defect, an effect known as Stark shift, can cause significant spectral diffusion in the emitted photons. In this work, using first principles computations, we revisit the methodology to compute the Stark shift of point defects up to the second order. The approach consists of applying an electric field on a defect in a slab and monitoring the changes in the computed zero-phonon line (i.e., difference in energy between the ground and excited state) obtained from constraining the orbital occupations (constrained-DFT). We study the Stark shift of the negatively charged nitrogen-vacancy (NV) center in diamond using this slab approach. We discuss and compare two approaches to ensure a negatively charged defect in a slab and we show that converged values of the Stark shift measured by the change in dipole moment between the ground and excited states (Δμ) can be obtained. We obtain a Stark shift of Δμ=2.68D using the semi-local GGA-PBE functional and of Δμ=2.23D using the HSE hybrid-functional. These values are in good agreement with experimental results. We also show that modern of theory of polarization can be used on constrained-DFT to obtain Stark shifts in very good agreement with the slab computations.