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arXiv:1407.6244 · New Journal of Physics

Singlet levels of the NV−centre in diamond

Lachlan J. Rogers, M W Doherty, M S J Barson, S Onoda, T Ohshima, N B Manson

Published Jan 27, 2015• 46 citations
arXivHTMLPDF

Abstract

The characteristic transition of the centre at 637 nm is between and triplet states. There are also intermediate and singlet states, and the infrared transition at 1042 nm between these singlets is studied here using uniaxial stress. The stress shift and splitting parameters are determined, and the physical interaction giving rise to the parameters is considered within the accepted electronic model of the centre. It is established that this interaction for the infrared transition is due to a modification of electron–electron Coulomb repulsion interaction. This is in contrast to the visible 637 nm transition where shifts and splittings arise from modification to the one-electron Coulomb interaction. It is also established that a dynamic Jahn–Teller interaction is associated with the singlet state, which gives rise to a vibronic level 115 cm −1 above the electronic state. Arguments associated with this level are used to provide experimental confirmation that the is the upper singlet level and is the lower singlet level.

DOI
10.1088/1367-2630/17/1/013048

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The characteristic transition of the centre at 637 nm is between and triplet states. There are also intermediate and singlet states, and the infrared transition at 1042 nm between these singlets is studied here using uniaxial stress. The stress shift and splitting parameters are determined, and the physical interaction giving rise to the parameters is considered within the accepted electronic model of the centre. It is established that this interaction for the infrared transition is due to a modification of electron–electron Coulomb repulsion interaction. This is in contrast to the visible 637 nm transition where shifts and splittings arise from modification to the one-electron Coulomb interaction. It is also established that a dynamic Jahn–Teller interaction is associated with the singlet state, which gives rise to a vibronic level 115 cm −1 above the electronic state. Arguments associated with this level are used to provide experimental confirmation that the is the upper singlet level and is the lower singlet level.
An emission band in the infrared (IR) is shown to be associated with a transition within the negative nitrogen-vacancy centre in diamond. The band has a zero-phonon line at 1046 nm, and uniaxial stress and magnetic field measurements indicate that the emission is associated with a transition between 1 E and 1 A 1 singlet levels. Inter-system crossing to these singlets causes the spin polarization that makes the NV - centre attractive for quantum information processing, and the IR emission band provides a new avenue for using the centre in such applications.
The negative Nitrogen-Vacancy (NV) colour centre in diamond is an atomic-level impurity that is remarkably well suited for quantum information processing and quantum metrology applications. Underlying these properties is the fact that optical illumination causes the NV centre to preferentially populate one of its three spin levels. The mechanism that gives rise to this spin polarisation has not been well understood, despite intense research interest in the NV centre and its applications. This thesis arrives at an account of the spin polarisation mechanism, although a detailed theoretical treatment remains outstanding. The energy level structure of the NV centre is investigated using techniques of solid state spectroscopy. These include absorption and photoluminescence measurements made on diamonds at cryogenic and room temperatures in the presence of uniaxial stress, magnetic fields, and microwaves. Pulsed light experiments allow the dynamic processes within the NV centre to be measured. It is shown that at room temperature the orbital doublet excited state behaves like an orbital singlet, and this description is elegantly confirmed by single-site observations. This picture of the excited state is inconsistent with cryogenic measurements, and its behaviour is examined across a range of temperatures in order to resolve this tension. It is shown that electron-vibration interaction accounts for the quenching of orbital properties in the excited state with temperature. A new optical transition within the NV centre is reported at a wavelength of 1042 nm. It is established that this transition occurs between the intermediate singlet levels which are thought to provide the decay pathway that produces spin polarisation. The results are consistent with this understanding, and the order and properties of these singlet levels are established. Electron-vibration interaction is observed to be important within the singlet system. It is shown that electron-vibration interaction is an important detail in the NV optical pumping cycle. Taking it into consideration leads to the first plausible physical description of the spin polarisation mechanism. -- provided by Candidate.
Nonradiative Transitions 3E → 1A1 and 1E~^{1}\tilde {E}1E~ → 3A2 in the NV– Center in Diamond
A mechanism is proposed for a nonradiative transition between excited energy levels of the NV– center in diamond. The nonradiative transition between the levels of the spin triplet and the singlet is possible due to the spin–orbit interaction with simultaneous excitation of vibrational (vibronic) states of the cluster and the excitation of lattice phonons and, hence, can be obtained in the second order of perturbation theory. For describing this process, the spin–vibronic interaction operator and nonzero matrix elements ensuring nonradiative transitions are obtained. It is found that the matrix elements are proportional to the overlap integrals for one-particle electron wavefunctions. It is shown that the rate of transitions 3E → 1A1 and 1E~^{1}\tilde {E}1E~ → 3A2 are described by identical expressions. Therefore, the nonradiative transitions considered here are explained not by a multiphonon process, but by the excitation of vibronic states of atoms of the NV– center. Numerical estimates are in good agreement with experimental data.
Uniaxial stress perturbations establish the 1.257 eV 'H2' zero-phonon line as an electric-dipole allowed transition at the centre of a C 2v point group. Taken in conjunction with a simple one-electron model, the magnitudes of the perturbations support recent suggestions that the H2 centre is a negative charge state of the well-known nitrogen-vacancy-nitrogen 'H3' centre. The H2 zero-phonon line is 0.9 meV higher in energy in 13 C diamond than in 12 C diamond. The shift is consistent, within large uncertainties, with the shift expected from the temperature dependence of the line. A local vibrational mode involving predominantly carbon atoms is identified.
The N3 centre in diamond consists of three nitrogen atoms and one vacancy. We show that the N3 zero-phonon line, at 2.985 eV in natural diamond, is shifted by in diamond doped with , with no detectable change in the vibronic bandshape. In diamond, the energies of all the phonons seen in the vibronic band appear to be reduced from diamond in the ratio , and the zero-phonon is shifted by . The carbon isotope shift can be understood in terms of contributions from the lattice expansion, of from the different vibrational frequencies in the ground and excited electronic states, and from the Jahn - Teller effect in the excited state.
The negatively charged nitrogen-vacancy (NV(-)) center in diamond is considered to be one of the most promising solid state systems for quantum information applications. Excited states of the NV(-) center play a center role in the proposed applications. Using a combination of first-principles calculations and vibronic interaction model analysis, we establish the presence of a dynamic Jahn-Teller effect in the (3)E excited state. The calculated temperature-dependent dephasing rate for the zero phonon line as well as the splitting of the first two vibronic states are in good agreement with experiment.