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Charge and Spin Dynamics and Destabilization of Shallow Nitrogen-Vacancy Centers under UV and Blue Excitation
Abstract
Shallow nitrogen-vacancy (NV) centers in diamond offer opportunities to study photochemical reactions, including photogeneration of radical pairs, at the single-molecule regime. A prerequisite is a detailed understanding of charge and spin dynamics of NVs exposed to the short-wavelength light required to excite chemical species. Here, we investigate the charge and spin dynamics of shallow NVs under 445 and 375 nm illumination. With blue excitation, charge-state preparation is power-dependent, and modest spin initialization fidelity is observed. Under UV excitation, charge-state preparation is power-independent and no spin polarization is observed. Aging of NVs under prolonged UV exposure manifests in a reduced charge stability and spin contrast. We attribute this aging to modified local charge environments of near-surface NVs and identify distinct electronic traps only accessible at short wavelengths. Finally, we evaluate the prospects of NVs to probe photogenerated radical pairs based on measured sensitivities and outline possible sensing schemes. Show more
Publication status
publishedExternal links
Journal / series
Nano LettersPublisher
American Chemical SocietySubject
nitrogen-vacancy(NV) center; quantum sensing; photoionization; optically detected magnetic resonance(ODMR); radical pairsFunding
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