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Journal of Applied Spectroscopy

Manifestation in IR-Luminescence of Cross Relaxation Processes between NV-Centers in Weak Magnetic Fields

D. S. Filimonenko, Valery M. Yasinskii, Alexander P. Nizovtsev, S. Ya. Kilin, Fedor Jelezko

Published Jan 1, 2022• 3 citations
Publisher
DOI
10.1007/s10812-022-01290-z

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We present a combined experimental and theoretical study of the effect of magnetic field on the luminescence from an ensemble of NV centers in diamond. It was found that the intensity of infrared luminescence associated with transitions between singlet levels of NV centers shows a pronounced increase of a near-zero magnetic field. The influence of the power and polarization of laser radiation on the amplitude and shape of the revealed local maximum in IR-luminescence of NV centers is investigated. An eight-level photophysical model of an NV center in the presence of an arbitrarily directed magnetic field has been constructed and on its basis the calculation has been performed of the luminescence intensity emitted by an ensemble of NV center, both in the visible and infrared regions of the spectrum. It is shown that the phenomenological allowance for the cross-relaxation of NV centers between each other and with other paramagnetic centers in a diamond within the framework of this model allows describing the experimentally observed fluorescence features of an ensemble of NV centers in the presence of weak magnetic fields.
Quantum relaxometry based on nitrogen-vacancy (NV) centers in diamond is an easy-to-use technique that detects magnetic noise by measuring the longitudinal relaxation of NV centers. It is favored in chemical and biological applications due to the robustness against imperfect spin control. By tuning the energy level, NV relaxometry can detect magnetic noise generated by other spins and obtain magnetic resonance spectra through cross relaxation. However, the inhomogeneous broadening of NV centers greatly limits the spectral resolution of cross-relaxation spectra. Here we demonstrate a hole-burning technique to remove the inhomogeneous broadening. We utilize a weak pump field to deplete specific NV centers during the relaxation measurement, which contribute a reverse signal in the cross-relaxation spectra with a much narrower linewidth. Our method retains the convenience and sensitivity of NV relaxometry, opening up new avenues for high-resolution magnetic resonance spectroscopy in complex scenarios.
Here, we investigate the magnetic field dependent photoluminescence (PL) of a fiber-coupled diamond single crystal with a high density of nitrogen vacancy (NV) centers. Angle-dependent magnetic field sweep measurements between 0 and 111 mT were performed using an oscillating illumination combined with lock-in techniques. Besides the expected superposed PL of differently oriented NV centers, a zoo of features in the PL are found. These features can be associated with level anti-crossings and cross relaxations. In particular, PL measurements allowed us to detect auto-cross relaxation between coupled NV centers. Moreover, the PL measurements at low magnetic fields show dips suggesting an interaction of NV centers with additional spin defects. The results presented here are not only a study for NV-based fiber-coupled sensors made of diamond, but also show a way to investigate with manageable effort and purely an optical multispin interaction with at least one NV center as a constituent.