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Electronic structure of the nitrogen-vacancy color center in diamond.

David A. Redman

Published Jan 1, 1991• 0 citations
OpenAlex

Abstract

The nitrogen - vacancy (N-V) center is a point defect found in diamonds containing substitutional nitrogen impurities. It arises after exposure to ionizing radiation and subsequent thermal annealing. The physical structure of the center has previously been identified as a substitutional nitrogen atom located adjacent to a neutral carbon vacancy, but prior to this work knowledge of its electronic structure was very incomplete. The results presented here are intended to establish the energy level structure of the N-V center unambiguously, using nonlinear laser spectroscopy in concert with paramagnetic resonance experiments. A new technique which achieves sub-Hertz resolution in nearly degenerate four-wave mixing (NDFWM) and optical two-beam coupling experiments was applied to determine the decay rates of excited states in the N-V center. Laser-enhanced EPR experiments were performed to assign spin character to the ground state. Fluorescent emission of the center was used to determine excited state energies. In particular, these results resolve earlier conflicting reports of the N-V ground state structure and offer a picture of state energies and dynamics consistent with all observations to date. The principal results of this thesis may be summarized as follows. We show that the ground state of the center consists of a spin triplet ground state with a zero-field splitting of 2.88 GHz and a spin-lattice relaxation time of 1.170 $\pm$ 0.003 ms. The first parity-allowed transition occurs to a triplet excited state at 1.944 eV with a lifetime of 13.3 $\pm$ 0.2 ns. The first metastable singlet excited state is shown to have a lifetime of 265.3 $\pm$ 0.6 ms at room temperature and its temperature dependence measured between 77 and 295 K. Through low temperature studies the mechanism for ground state spin-lattice relaxation is determined to be a two-phonon process involving 63 meV optical phonons. Finally, the origin of satellite lines in the persistent hole-burning spectrum is tentatively explained using our picture of the energy level structure and used to infer a zero-field spin splitting in the excited triplet state of 0.6 GHz.

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Over the past few years, the detection of single N-V centers in diamond has attracted much interest, since it is expected to lead to innovative applications in various domains of quantum information. The N-V center in diamond is a defectconsisting of a substitutional nitrogen atom adjacent to a carbon-atom vacancy. The optical transition between the 3A ground state and the 3E excited state has a very high quantum efficiency allowing single defect spectroscopy. Because of the paramagnetic nature of the ground electronic state, single N-V defects are believed to be promising candidates for solid state quantum computation. To date, however, the photophysics of the defect is not entirely understood. The existence of a singlet metastable state 1A was challenged in a series of papers reporting hole-burning, optically detected magnetic resonance and single molecule experiments. We present here an overview of recent low and room temperature data, indicating the important role of a metastable state of the defect in single center experiments.

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The nitrogen-vacancy center in diamond exhibits a zero-phonon transition art 637 nm that has been assigned as an A→E transition at a site with trigonal symmetry.1 Paramagnetic resonance studies revealed a triplet feature that was originally assigned to an excited state.2 More recently, it was argued that the triplet signal actually arose from the ground state,3,4We employ a new method of ultra-high-resolution nearly degenerate four-wave-mixing (NDFWM) spectroscopy, as well as persistent hole burning and electron paramagnetic resonance, to measure the metastable spin singlet excited-state lifetime and the g round-state spin-lattice relaxation time and also to prove that the ground state is indeed a triplet.

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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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Electronic structure of the N-Vcenter in diamond: Experiments

Alan Lenef, Steven W. Brown, David A. Redman +3 more

Quantum-beat spectroscopy has been used to observe excited states of the N-V center in diamond. For the 1.945-eV optical transition, direct evidence is presented for the existence of GHz-scale fine structure, together with a much larger 46-${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ level splitting in the E state. An interference effect observed in transient four-wave-mixing response is explained with a polarization selection rule involving Zeeman coherence among magnetic sublevels. Also, detailed dephasing measurements versus temperature and wavelength have identified the decay mechanisms operative among the various states. A comparison of these results with ab initio calculations of excited electronic structure and interactions based on several multielectron models supports the conclusion that the N-V center is a neutral, two-electron center governed by a strong Jahn-Teller effect and weak spin-spin interactions. \textcopyright{} 1996 The American Physical Society.

Physical review. B, Condensed matter•May 15, 1996•68 citations
The nitrogen - vacancy (N-V) center is a point defect found in diamonds containing substitutional nitrogen impurities. It arises after exposure to ionizing radiation and subsequent thermal annealing. The physical structure of the center has previously been identified as a substitutional nitrogen atom located adjacent to a neutral carbon vacancy, but prior to this work knowledge of its electronic structure was very incomplete. The results presented here are intended to establish the energy level structure of the N-V center unambiguously, using nonlinear laser spectroscopy in concert with paramagnetic resonance experiments. A new technique which achieves sub-Hertz resolution in nearly degenerate four-wave mixing (NDFWM) and optical two-beam coupling experiments was applied to determine the decay rates of excited states in the N-V center. Laser-enhanced EPR experiments were performed to assign spin character to the ground state. Fluorescent emission of the center was used to determine excited state energies. In particular, these results resolve earlier conflicting reports of the N-V ground state structure and offer a picture of state energies and dynamics consistent with all observations to date. The principal results of this thesis may be summarized as follows. We show that the ground state of the center consists of a spin triplet ground state with a zero-field splitting of 2.88 GHz and a spin-lattice relaxation time of 1.170 ±\pm± 0.003 ms. The first parity-allowed transition occurs to a triplet excited state at 1.944 eV with a lifetime of 13.3 ±\pm± 0.2 ns. The first metastable singlet excited state is shown to have a lifetime of 265.3 ±\pm± 0.6 ms at room temperature and its temperature dependence measured between 77 and 295 K. Through low temperature studies the mechanism for ground state spin-lattice relaxation is determined to be a two-phonon process involving 63 meV optical phonons. Finally, the origin of satellite lines in the persistent hole-burning spectrum is tentatively explained using our picture of the energy level structure and used to infer a zero-field spin splitting in the excited triplet state of 0.6 GHz.
Over the past few years, the detection of single N-V centers in diamond has attracted much interest, since it is expected to lead to innovative applications in various domains of quantum information. The N-V center in diamond is a defectconsisting of a substitutional nitrogen atom adjacent to a carbon-atom vacancy. The optical transition between the 3A ground state and the 3E excited state has a very high quantum efficiency allowing single defect spectroscopy. Because of the paramagnetic nature of the ground electronic state, single N-V defects are believed to be promising candidates for solid state quantum computation. To date, however, the photophysics of the defect is not entirely understood. The existence of a singlet metastable state 1A was challenged in a series of papers reporting hole-burning, optically detected magnetic resonance and single molecule experiments. We present here an overview of recent low and room temperature data, indicating the important role of a metastable state of the defect in single center experiments.
The nitrogen-vacancy center in diamond exhibits a zero-phonon transition art 637 nm that has been assigned as an A→E transition at a site with trigonal symmetry.1 Paramagnetic resonance studies revealed a triplet feature that was originally assigned to an excited state.2 More recently, it was argued that the triplet signal actually arose from the ground state,3,4We employ a new method of ultra-high-resolution nearly degenerate four-wave-mixing (NDFWM) spectroscopy, as well as persistent hole burning and electron paramagnetic resonance, to measure the metastable spin singlet excited-state lifetime and the g round-state spin-lattice relaxation time and also to prove that the ground state is indeed a triplet.
The silicon-vacancy (SiV) and nitrogen-vacancy (NV) centers in diamond are commonly regarded as prototypical defects for solid-state quantum information processing. Here, we show that when silicon and nitrogen are simultaneously introduced into the diamond lattice, these defects can strongly interact and form larger complexes. Nitrogen atoms strongly bind to Si and SiV centers, and complex formation can occur. Using a combination of hybrid density functional theory and group theory, we analyze the electronic structure and provide various useful physical properties, such as hyperfine structure, quasilocal vibrational modes, and a zero-phonon line, to enable experimental identification of these complexes. We demonstrate that the presence of substitutional silicon adjacent to nitrogen significantly shifts the donor level toward the conduction band, resulting in an activation energy for the SiN center that is comparable to phosphorus. We also find that the neutral SiNV center is of particular interest due to its photon emission at $\ensuremath{\sim}1530\phantom{\rule{0.28em}{0ex}}\mathrm{nm}$, which falls within the CCC band of telecom wavelengths and its paramagnetic nature. In addition, the optical transition associated with the SiNV0{\mathrm{SiNV}}^{0}SiNV0 color center exhibits very small electron-phonon coupling (Huang-Rhys factor = 0.78) resulting in high quantum efficiency (Debye-Waller factor = 46%) for single-photon emission. These features render this new center very attractive for a potential application in scalable quantum telecommunication networks.
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.
The nitrogen-vacancy (NV) lattice defect in diamond, consisting of an N substitutional atom and an adjacent C vacancy, is commonly observed in two charge states, negative (NV−) and neutral (NV0). The NV− defect exhibits spin state-dependent fluorescence and is, therefore, amenable to optical methods for spin-state readout, while the NV0 is not. Hence, the NV− defect is much more useful for quantum sensing and quantum information processing. However, only NV0 electroluminescence has been observed, even from centers showing NV− in photoluminescence. In the present work, we use first-principles electronic structure calculations to determine adiabatic charge transition levels for the conversion of NV− to NV0 in the presence of substitutional N or P impurities, which provide the charge of the NV− center. We find that the adiabatic charge transition levels in the presence of such impurities lie at energies close to or lower than the zero-phonon line of the NV− center and that these energies only decrease as the concentration of N donors increases. This work, therefore, elucidates the absence of observed electroluminescence from the NV− and proposes a path toward observation of the phenomenon.
Quantum-beat spectroscopy has been used to observe excited states of the N-V center in diamond. For the 1.945-eV optical transition, direct evidence is presented for the existence of GHz-scale fine structure, together with a much larger 46-${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ level splitting in the E state. An interference effect observed in transient four-wave-mixing response is explained with a polarization selection rule involving Zeeman coherence among magnetic sublevels. Also, detailed dephasing measurements versus temperature and wavelength have identified the decay mechanisms operative among the various states. A comparison of these results with ab initio calculations of excited electronic structure and interactions based on several multielectron models supports the conclusion that the N-V center is a neutral, two-electron center governed by a strong Jahn-Teller effect and weak spin-spin interactions. \textcopyright{} 1996 The American Physical Society.