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New Journal of Physics

Low-field feature in the magnetic spectra of NV−centers in diamond

S. V. Anishchik, Victor G. Vins, Alexander Yèlisseyev, Nikita N. Lukzen, Nikolay L. Lavrik, V. A. Bagryansky

Published Feb 13, 2015• 33 citations
Publisher

Abstract

The low-magnetic-field feature in the magnetic field dependence of the luminescence of negatively charged nitrogen-vacancy (NV − ) centers in diamond has been experimentally observed for the first time. This feature, centered at the zero magnetic field—henceforth the zero field line—and observed with a magnetic field sweep of NV − center luminescence (magnetic spectrum), is quite narrow. The properties of this line are considerably different from those of other narrow NV − magnetic spectrum lines. Its amplitude is weakly dependent on the orientation of the single-crystal sample with respect to the external magnetic field. This line is also observed in a powdered sample. The shape of the line changes drastically with a change in the polarization of excitation light. The amplitude of the line non-linearly depends on excitation light intensity. For low intensities this dependence is close to the square law. We attribute the occurrence of this line to the dipole–dipole interaction between different NV − centers.

DOI
10.1088/1367-2630/17/2/023040

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The optical and ODMR spectra of nitrogen vacancy (NV) centers in diamond were investigated as applied to the development of micro-scale diamond magnetometer sensor. It is shown that the NV 0 center (unlike the NV − center) has an absorption line in the UV range. The inversion of the zero phonon line of the NV − center was observed and explained. ODMR signals in high magnetic fields (as compared with inner fields in the crystal) as well as in weak fields also were investigated. We propose the solution to the problem of the magnetometer sensitivity reduction at low magnetic field, that is of interest for quantum magnetometry applications.

Journal of Physics Conference Series•Oct 27, 2014•2 citations
The low-magnetic-field feature in the magnetic field dependence of the luminescence of negatively charged nitrogen-vacancy (NV − ) centers in diamond has been experimentally observed for the first time. This feature, centered at the zero magnetic field—henceforth the zero field line—and observed with a magnetic field sweep of NV − center luminescence (magnetic spectrum), is quite narrow. The properties of this line are considerably different from those of other narrow NV − magnetic spectrum lines. Its amplitude is weakly dependent on the orientation of the single-crystal sample with respect to the external magnetic field. This line is also observed in a powdered sample. The shape of the line changes drastically with a change in the polarization of excitation light. The amplitude of the line non-linearly depends on excitation light intensity. For low intensities this dependence is close to the square law. We attribute the occurrence of this line to the dipole–dipole interaction between different NV − centers.
The dependence of the luminescence of diamonds with negatively charged nitrogen-vacancy centers (NV-) vs. applied magnetic field (magnetic spectrum) was studied. A narrow line in zero magnetic field was discovered. The properties of this line are considerably different from those of other narrow magnetic spectrum lines. Its magnitude is weakly dependent of the orientation of the single-crystal sample to the external magnetic field. This line is also observed in a powdered sample. The shape of the line changes greatly when excitation light polarization is varied. The magnitude of the line has a non-linear relation to excitation light intensity. For low intensities this dependence is close to a square law. To explain the mechanism giving rise to this line in the magnetic spectrum, we suggest a model based on the dipole-dipole interaction between different NV- centers.
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.
We report a study of the magnetic field dependence of the photo-luminescence of NV−^-− centers (negatively charged nitrogen-vacancy centers) in diamond single crystals. In such a magnetic field dependence characteristic lines are observed, which are coming from Level Anti-Crossings (LACs) in the coupled electron-nuclear spin system. For enhancing the sensitivity, we used lock-in detection to measure the photo-luminescence intensity and observed a remarkably strong dependence of the LAC-derived lines on the modulation frequency. Upon decreasing of the modulation frequency from 12 kHz to 17 Hz the amplitude of the lines increases by approximately two orders of magnitude. To take a quantitative account for such effects, we developed a theoretical model, which describes the spin dynamics in the coupled electron-nuclear spin system under the action of an oscillating external magnetic field. Good agreement between experiments and theory allows us to conclude that the observed effects are originating from coherent spin polarization exchange in the NV−^-− center. Our results are of great practical importance allowing one to optimize the experimental conditions for probing LAC-derived lines in diamond defect centers.
With the creation of nitrogen (NV) in 1b diamond it is common to find that the absorption and emission is predominantly of negatively charged NV centres. This occurs because electrons tunnel from the substitutional nitrogen atoms to NV to form NV−–N+ pairs. There can be a small percentage of neutral charge NV0 centres and a linear increase of this percentage can be obtained with optical intensity. Subsequent to excitation it is found that the line width of the NV− zero-phonon has been altered. The alteration arises from a change of the distribution of N+ ions and a modification of the average electric field at the NV− sites. The consequence is a change to the Stark shifts and splittings giving the change of the zero-phonon line (ZPL) width. Exciting the NV− centres enhances the density of close N+ ions and there is a broadening of the ZPL. Alternatively exciting and ionizing N0 in the lattice results in more distant distribution of N+ ions and a narrowing of the ZPL. The competition between NV− and N0 excitation results in a significant dependence on excitation wavelength and there is also a dependence on the concentration of the NV− and N0 in the samples. The present investigation involves extensive use of low temperature optical spectroscopy to monitor changes to the absorption and emission spectra particularly the widths of the ZPL. The studies lead to a good understanding of the properties of the NV−–N+ pairs in diamond. There is a critical dependence on pair separation. When the NV−–N+ pair separation is large the properties are as for single sites and a high degree of optically induced spin polarization is attainable. When the separation decreases the emission is reduced, the lifetime shortened and the spin polarization downgraded. With separations of <12 A0 there is even no emission. The deterioration occurs as a consequence of electron tunneling in the excited state from NV– to N+ and an optical cycle that involves NV0. The number of pairs with the smaller separations and poorer properties will increase with the number of nitrogen impurities and it follows that the degree of spin polarization that can be achieved for an ensemble of NV− in 1b diamond will be determined and limited by the concentration of single substitutional nitrogen. The information will be invaluable for obtaining optimal conditions when ensembles of NV− are required. As well as extensive measurements of the NV− optical ZPL observations of Stark effects associated with the infrared line at 1042 nm and the optically detected magnetic resonance at 2.87 GHz are also reported.
With the creation of nitrogen (NV) in 1b diamond it is common to find that the absorption and emission is predominantly of negatively charged NV centres. This occurs because electrons tunnel from the substitutional nitrogen atoms to NV to form NV − –N + pairs. There can be a small percentage of neutral charge NV 0 centres and a linear increase of this percentage can be obtained with optical intensity. Subsequent to excitation it is found that the line width of the NV − zero-phonon has been altered. The alteration arises from a change of the distribution of N + ions and a modification of the average electric field at the NV − sites. The consequence is a change to the Stark shifts and splittings giving the change of the zero-phonon line (ZPL) width. Exciting the NV − centres enhances the density of close N + ions and there is a broadening of the ZPL. Alternatively exciting and ionizing N 0 in the lattice results in more distant distribution of N + ions and a narrowing of the ZPL. The competition between NV − and N 0 excitation results in a significant dependence on excitation wavelength and there is also a dependence on the concentration of the NV − and N 0 in the samples. The present investigation involves extensive use of low temperature optical spectroscopy to monitor changes to the absorption and emission spectra particularly the widths of the ZPL. The studies lead to a good understanding of the properties of the NV − –N + pairs in diamond. There is a critical dependence on pair separation. When the NV − –N + pair separation is large the properties are as for single sites and a high degree of optically induced spin polarization is attainable. When the separation decreases the emission is reduced, the lifetime shortened and the spin polarization downgraded. With separations of <12 A 0 there is even no emission. The deterioration occurs as a consequence of electron tunneling in the excited state from NV – to N + and an optical cycle that involves NV 0 . The number of pairs with the smaller separations and poorer properties will increase with the number of nitrogen impurities and it follows that the degree of spin polarization that can be achieved for an ensemble of NV − in 1b diamond will be determined and limited by the concentration of single substitutional nitrogen. The information will be invaluable for obtaining optimal conditions when ensembles of NV − are required. As well as extensive measurements of the NV − optical ZPL observations of Stark effects associated with the infrared line at 1042 nm and the optically detected magnetic resonance at 2.87 GHz are also reported.
The optical and ODMR spectra of nitrogen vacancy (NV) centers in diamond were investigated as applied to the development of micro-scale diamond magnetometer sensor. It is shown that the NV 0 center (unlike the NV − center) has an absorption line in the UV range. The inversion of the zero phonon line of the NV − center was observed and explained. ODMR signals in high magnetic fields (as compared with inner fields in the crystal) as well as in weak fields also were investigated. We propose the solution to the problem of the magnetometer sensitivity reduction at low magnetic field, that is of interest for quantum magnetometry applications.