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Journal of Physics Condensed Matter

Optical hole-bleaching by level anti-crossing and cross relaxation in the N-V centre in diamond

Keith Holliday, Neil B. Manson, Max Glasbeek, Eric van Oort

Published Oct 2, 1989• 48 citations
Publisher

Abstract

The authors have studied the behaviour of an optical hole in the 3 A to 3 E zero-phonon absorption of the nitrogen-vacancy centre in type 1b diamond under the influence of an externally applied magnetic field. Spin cross relaxation and level anti-crossing phenomena in the 3 A ground state are displayed as sudden reductions of the optical hole depth (hole-bleaching) for specific orientations and strengths of the applied magnetic field.

DOI
10.1088/0953-8984/1/39/021

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The authors have studied the behaviour of an optical hole in the 3 A to 3 E zero-phonon absorption of the nitrogen-vacancy centre in type 1b diamond under the influence of an externally applied magnetic field. Spin cross relaxation and level anti-crossing phenomena in the 3 A ground state are displayed as sudden reductions of the optical hole depth (hole-bleaching) for specific orientations and strengths of the applied magnetic field.
Under optical illumination in the blue or green, negatively charged nitrogen vacancy centres in diamond emit in the red. The intensity of this emission varies slightly depending on spin state occupation. Optical transitions occur predominantly without change of spin projection. However, excited ms=±1 states can decay non-radiatively to the ground ms=0 state via intermediary singlet states. With continuous excitation, this effect transfers most of the population to the ms=0 state resulting in decay becoming almost entirely radiative so that optical emission is stronger than when all spin states are occupied equally. However, under optical illumination the ms=0 polarization is reduced when an applied magnetic field induces avoided crossings between energy levels. The spin states are mixed and some population is diverted into the ms=±1 states with consequent reduction in optical emission. The change of emission can be calculated from a rate equation model involving the spin states of the ground and excited levels plus one singlet level [5]. The spin states of the excited levels are also affected by strain and in this work we calculate the variation in optical emission with changing magnetic field for various fixed values of strain.
Abstract Nitrogen-vacancy (NV) centers in diamond have become an important tool for quantum technologies. All of these applications rely on long coherence times of electron and nuclear spins associated with these centers. Here, we study the energy level anti-crossings of an NV center in diamond coupled to a first-shell 13C nuclear spin in a small static magnetic field. These level anti-crossings (LACs) occur for specific orientations of the static magnetic field due to the strong non-secular components of the Hamiltonian. At these orientations we observe decoherence-free subspaces, where the electron spin coherence times ( T 2 * ) are 5–7 times longer than those at other orientations. Another interesting property at these LACs is that individual transition amplitudes are dominated by a single component of the magnetic dipole moment. Accordingly, this can be used for vector detection of microwave magnetic fields with a single NV center. This is particularly important to precisely control the center using numerical optimal control techniques.
We investigate the properties of spin states in the electronic ground state of a single nitrogen-vacancy center (NV_) in13C-enriched diamond. The analysis is based on application of a method that uses a complete set of commuting operators. Our results demonstrate that there are a two double degeneracy of energy levels in this system which is not removed by magnetic field and it may be consider like a special case of LAC. The change in properties of the spin states of the NV-center at the level anti-crossing is being considered as a possible reason for change in the intensity of NV-centers photoluminescence.
In brown diamond, the long-lived emission at 2.818 eV is known to be due to a localized center in the photoexcited triplet state. In this paper, the emission intensity of the 2.818-eV center is studied as a function of the strength of an externally applied magnetic field. The cross-relaxation (CR) with N-V centers, P1{\mathit{P}}_{1}P1​ centers, and g=2 doublet spins of unknown origin, as well as level anticrossing (LAC), is found to affect the phosphorescence intensity for certain magnetic-field strengths and orientations. The CR dynamics is studied optically by measuring the phosphorescence transients induced by microwave pulses resonant with a spin transition in the photoexcited triplet state. Under CR conditions, spin population relaxation in the excited triplet state becomes faster and deviates from a single-exponential recovery behavior. The triplet-state kinetics including CR effects is studied theoretically, and a double-exponential recovery is predicted. Based on an analysis of the kinetics, the experimental microwave recovery transients under the CR conditions are satisfactorily simulated. The CR rate is estimated to be (5.0\ifmmode\pm\else\textpm\fi{}1.5)\ifmmode\times\else\texttimes\fi{}102{10}^{2}102 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$ for the CR with the N-V center and (8.0\ifmmode\pm\else\textpm\fi{}2.5)\ifmmode\times\else\texttimes\fi{}102{10}^{2}102 ${\mathrm{s}}^{\mathrm{\ensuremath{-}}1}$ for the CR with the g=2 doublet species.
Recent developments in magnetic field sensing with negatively charged nitrogen-vacancy centers (NV) in diamond employ magnetic-field (MF) dependent features in the photoluminescence (PL) and eliminate the need for microwaves (MW). Here, we study two approaches towards improving the magnetometric sensitivity using the ground-state level anti-crossing (GSLAC) feature of the NV center at a background MF of 102.4 mT. Following the first approach, we investigate the feature parameters for precise alignment in a dilute diamond sample; the second approach extends the sensing protocol into absorption via detection of the GSLAC in the diamond transmission of a 1042nm laser beam. This leads to an increase of GSLAC contrast and results in a magnetometer with a sensitivity of 0.45 nT/√Hz and a photon shot-noise limited sensitivity of 12.2 pT/√Hz.
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.