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Physica B Condensed Matter

NV centers in diamond: spin-selective photokinetics, optical ground-state spin alignment and hole burning

Alexander P. Nizovtsev, S. Ya. Kilin, Fedor Jelezko, I. Popa, A. Gruber, Jörg Wrachtrup

Published Dec 1, 2003• 35 citations
Publisher
DOI
10.1016/j.physb.2003.09.014

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Nitrogen-vacancy (NV) centers in diamond have attracted significant interest because of their excellent spin and optical characteristics for quantum information and metrology. To exploit these characteristics, precise control of the orientation of the NV axis in the lattice is essential. Here we show that the orientation of more than 99% of the NV centers can be aligned along the [111] axis by chemical vapor deposition homoepitaxial growth on (111) substrates. We also discuss the alignment mechanisms. Our result enables a fourfold improvement in the magnetic field sensitivity and opens new avenues to the optimum design of NV center devices.

arXiv:1403.5057•Applied Physics Express•Apr 9, 2014•138 citations
The spin-selective photokinetics of a single matrix-isolated impurity molecule with a triplet-triplet optical transition, T 0–T 1, is considered and the manifestations of the photokinetics in the fluorescence excitation spectra and intensity autocorrelation functions g (2)(τ) of the molecule undergoing narrow-band optical excitation is studied to resolve the fine structure of the transition. The rates of intersystem crossings (ISCs) T 1→S→T 0 to and from a nonradiating singlet state S of the molecule and the rate of population relaxation among the ground (T 0) state sublevels can be obtained from the spectra and g (2)(τ) using the analytical expressions obtained. New experiments on an individual NV defect center in nanocrystals of diamond, where, for the first time, the fine structure of its triplet-triplet 3 A-3 E zero-phonon optical transition (~637 nm) at 1.4 K was resolved, are interpreted. It is concluded that the rate of the ISC transition from the m S =0 sublevel of the excited 3 E state to the singlet 1 A state (~1 kHz) is much slower than the rates from the m S =±1 substates, while the rates of ISC transitions to different m S substates of the ground 3 A state are close to each other (~1 Hz). As a result, only the optical transition between m S =0 sublevels in the 3 A-3 E manifold contributes strongly to the fluorescence. The experimentally observed double-exponential decay of the g (2)(τ) function is explained by the two pathways available to the center for it to leave the S state: (i) the S→ T 0(m S )=0) transition and (ii) the S→T 0(m S =±1) transitions followed by the slow spin-lattice relaxation T 0(m S =±1)→T 0(m S =0) (rate ~0.1 Hz). The work is important for studies where the NV center is used as a single photon source or for quantum information processing.
Selective alignment of nitrogen-vacancy (NV) centers in diamond is an important technique towards its applications. Quantification of the alignment ratio is necessary to design the optimized diamond samples. However, this is not a straightforward problem for dense ensemble of the NV centers. We estimate the alignment ratio of ensemble NV centers along the [111] direction in (111) diamond by optically detected magnetic resonance measurements. Diamond films deposited by N2 doped chemical vapor deposition have NV center densities over 1 × 1015 cm−3 and alignment ratios over 75%. Although spin coherence time (T2) is limited to a few μs by electron spins of nitrogen impurities, the combination of the selective alignment and the high density can be a possible way to optimize NV-containing diamond samples for the sensing applications.
Nitrogen-vacancy (NV) centers in diamond have attracted significant interest because of their excellent spin and optical characteristics for quantum information and metrology. To exploit these characteristics, precise control of the orientation of the NV axis in the lattice is essential. Here we show that the orientation of more than 99% of the NV centers can be aligned along the [111] axis by chemical vapor deposition homoepitaxial growth on (111) substrates. We also discuss the alignment mechanisms. Our result enables a fourfold improvement in the magnetic field sensitivity and opens new avenues to the optimum design of NV center devices.