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arXiv:0806.0895 · New Journal of Physics

Infrared emission of the NV centre in diamond: Zeeman and uniaxial stress studies

Lachlan J. Rogers, Seiji Armstrong, Matthew J. Sellars, Neil B. Manson

Published Oct 31, 2008• 194 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1088/1367-2630/10/10/103024

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Optical pumping cycle of the negative nitrogen-vacancy centre in diamond

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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.

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How far into the infrared can a colour centre in diamond emit?

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arXiv:1807.08889•New Journal of Physics•Oct 30, 2018•129 citations
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.
Infrared emission has been observed for the nitrogen-vacancy (NV −) colour centre in diamond, in addition to the characteristic red emission of this centre [1]. However, this infrared emission zero-phonon line at 1046 nm is about four orders of magnitude weaker than the red emission. This is somewhat surprising, as a third of the population is known to decay without the red emission and the infrared emission is considered to be associated with the alternative decay path. The most obvious explanation is a competing effcient non-radiative decay. There are few reports of diamond emitting at wavelengths longer than 1000 nm. Colour centres in diamond have strong electron-phonon coupling and, of course, the phonon energies in diamond are high. These properties suggest that non-radiative decay could dominate the transition whenever the electronic energy lies in the infrared. This would be a general phenomena and would account for the weak IR emission observed for this centre. It would also account for why there are so few reports of emission from diamond in the infrared.
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.
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.
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.
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.