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Spin dynamics of diamond nitrogen-vacancy centres at the ground state level anti-crossing and all-optical low frequency magnetic field sensing

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 Added by David A. Broadway
 Publication date 2016
  fields Physics
and research's language is English




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We investigate the photo-induced spin dynamics of single nitrogen-vacancy (NV) centres in diamond near the electronic ground state level anti-crossing (GSLAC), which occurs at an axial magnetic field around 1024 G. Using optically detected magnetic resonance spectroscopy, we first find that the electron spin transition frequency can be tuned down to 100 kHz for the NV{14} centre, while for the NV{15} centre the transition strength vanishes for frequencies below about 2 MHz owing to the GSLAC level structure. Using optical pulses to prepare and readout the spin state, we observe coherent spin oscillations at 1024 G for the NV{14}, which originate from spin mixing induced by residual transverse magnetic fields. This effect is responsible for limiting the smallest observable transition frequency, which can span two orders of magnitude from 100 kHz to tens of MHz depending on the local magnetic noise. A similar feature is observed for the NV{15} centre at 1024 G. As an application of these findings, we demonstrate all-optical detection and spectroscopy of externally-generated fluctuating magnetic fields at frequencies from 8 MHz down to 500 kHz, using a NV{14} centre. Since the Larmor frequency of most nuclear spin species lies within this frequency range near the GSLAC, these results pave the way towards all-optical, nanoscale nuclear magnetic resonance spectroscopy, using longitudinal spin cross-relaxation.



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The nitrogen-vacancy center (NV center) in diamond at magnetic fields corresponding to the ground state level anticrossing (GSLAC) region gives rise to rich photoluminescence (PL) signals due to the vanishing energy gap between the electron spin states, which enables to have an effect on the NV centers luminescence for a broad variety of environmental couplings. In this article we report on the GSLAC photoluminescence signature of NV ensembles in different spin environments at various external fields. We investigate the effects of transverse electric and magnetic fields, P1 centers, NV centers, and the $^{13}$C nuclear spins, each of which gives rise to a unique PL signature at the GSLAC. The comprehensive analysis of the couplings and related optical signal at the GSLAC provides a solid ground for advancing various microwave-free applications at the GSLAC, including but not limited to magnetometry, spectroscopy, dynamic nuclear polarization (DNP), and nuclear magnetic resonance (NMR) detection. We demonstrate that not only the most abundant $^{14}$NV center but the $^{15}$NV can also be utilized in such applications and that nuclear spins coupled to P1 centers can be polarized directly by the NV center at the GSLAC, through a giant effective nuclear $g$-factor arising from the NV center-P1 center-nuclear spin coupling. We report on new alternative for measuring defect concentration in the vicinity of NV centers and on the optical signatures of interacting, mutually aligned NV centers.
The protocols for the control and readout of Nitrogen Vacancy (NV) centres electron spins in diamond offer an advanced platform for quantum computation, metrology and sensing. These protocols are based on the optical readout of photons emitted from NV centres, which process is limited by the yield of photons collection. Here we report on a novel principle for the detection of NV centres magnetic resonance in diamond by directly monitoring spin-preserving electron transitions through measurement of NV centre related photocurrent. The demonstrated direct detection technique offers a sensitive way for the readout of diamond NV sensors and diamond quantum devices on diamond chips. The Photocurrent Detection of Magnetic Resonance (PDMR) scheme is based on the detection of charge carriers promoted to the conduction band of diamond by the two-photon ionization of NV- centres. Optical detection of magnetic resonance (ODMR) and PDMR are compared, by performing both measurements simultaneously. The minima detected in the measured photocurrent at resonant microwave frequencies are attributed to the spin-dependent occupation probability of the NV- ground state, originating from spin-selective non-radiative transitions.
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.
We report a study of the magnetic field dependence of photoluminescence of NV$^-$ centers (negatively charged nitrogen-vacancy centers) in diamond single crystals. In such a magnetic field dependence characteristic sharp features are observed, which are coming from Level Anti-Crossings (LACs) in a coupled electron-nuclear spin system. For sensitive detection of such LAC-lines we use lock-in detection to measure the photoluminescence intensity. This experimental technique allows us to obtain new LAC lines. Additionally, a remarkably strong dependence of the LAC-lines on the modulation frequency is found. Specifically, upon decrease of the modulation frequency from 12 kHz to 17 Hz the amplitude of the LAC-lines increases by approximately two orders of magnitude. To take a quantitative account for such effects, we present a theoretical model, which describes the spin dynamics in a 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 a coupled spin system comprising the spin-polarized NV$^-$ center. Our results are of great practical importance allowing one to optimize the experimental conditions for probing LAC-derived lines in diamond crystals comprising NV$^-$ centers and for indirect detection and identification of other paramagnetic defect centers.
We report an experimental study of the longitudinal relaxation time ($T_1$) of the electron spin associated with single nitrogen-vacancy (NV) defects hosted in nanodiamonds (ND). We first show that $T_1$ decreases over three orders of magnitude when the ND size is reduced from 100 to 10 nm owing to the interaction of the NV electron spin with a bath of paramagnetic centers lying on the ND surface. We next tune the magnetic environment by decorating the ND surface with Gd$^{3+}$ ions and observe an efficient $T_{1}$-quenching, which demonstrates magnetic noise sensing with a single electron spin. We estimate a sensitivity down to $approx 14$ electron spins detected within 10 s, using a single NV defect hosted in a 10-nm-size ND. These results pave the way towards $T_1$-based nanoscale imaging of the spin density in biological samples.
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