Characterization of oxygen defects in diamond by means of density functional theory calculations

Abstract

Point defects in diamond are of high interest as candidates for realizing solid state quantum bits, bioimaging agents, or ultrasensitive electric or magnetic field sensors. Various artificial diamond synthesis methods should introduce oxygen contamination in diamond, however, the incorporation of oxygen into diamond crystal and the nature of oxygen-related point defects are largely unknown. Oxygen may be potentially interesting as a source of quantum bits or it may interact with other point defects which are well established solid state qubits. Here we employ plane-wave supercell calculations within density functional theory, in order to characterize the electronic and magneto-optical properties of various oxygen-related defects. Beside the trivial single interstitial and substitutional oxygen defects we also consider their complexes with vacancies and hydrogen atoms. We find that oxygen defects are mostly electrically active and introduce highly correlated orbitals that pose a challenge for density functional theory modeling. Nevertheless, we are able to identify the fingerprints of substitutional oxygen defect, the oxygen-vacancy and oxygen-vacancy-hydrogen complexes in the electron paramagnetic resonance spectrum. We demonstrate that first principles calculations can predict the motional averaging of the electron paramagnetic resonance spectrum of defects that are subject to Jahn-Teller distortion. We show that the high-spin neutral oxygen-vacancy defect exhibits very fast non-radiative decay from its optical excited state that might hinder to apply it as a qubit.

Ab initio theory of the nitrogen-vacancy center in diamond

“…(7a-c) in Ref. 187 (see also references therein). As a consequence, Γ tunnel Γ rad , therefore, the phonon sideband of the absorption spectrum should be calculated as the combination of the A 1 phonons in the Huang-Rhys approximation (predominant contribution) plus direct calculation from the ground state vibration function towards the high symmetry polaronic solution caused by the E phonons.…”

Ultrafast Orbital Depolarization and Defect-Localized Phonon Dynamics Induced by Quantum Resonance between Multi-Nitrogen Vacancy Defects

“…Therefore, the current NA transition dynamics should be at least semiquantitatively correct as was demonstrated in the single NV defect case [2], and the above deviations between the HSE06 and PBE functionals are irrelevant to the suggested physical insights and conclusions on the depolarization dynamics and phonon modes in this study. Actually, the PBE functional has been widely adopted in many defect cases including structures [3][4][5][6],…”

“…energies [3,7,8] and phonon modes [4,6,9]. Balancing the computational cost and accuracy, we chose the PBE functional to semiquantitatively describe the NA transition dynamics among the defect orbitals at the ambient temperature.…”

“…It should be noted that the power spectra exhibit peaks around 1300 cm −1 , which is close to the experimentally observed Raman peak frequency of a diamond crystal, 1330 cm −1 . 1,8 The current simple power spectra of the defect orbital energies still can reproduce such a representative Raman mode.…”

Features of the impurity composition of diamonds from placers of the northeastern Siberian craton

“…Методом масс-спектрометрии доказано вхождение кислорода в решётку алмаза [13]. Теоретические расчёты с помощью метода DFT показали [14], что энергетически выгодными структурами кислородных центров являются замещающий кислород и кислород в сочетании с вакансией и атомом водорода. Как было отмечено выше, в 17 кристаллах из россыпи Маят нами зафиксирована люминесценция кислородсодержащих центров, но ни в одном из них не обнаружены ЭПР-центры ОК1 и N3, а также их оптические аналоги S1, 440,3 нм и 635,7 нм.…”