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New Journal of Physics

Spin-flip and spin-conserving optical transitions of the nitrogen-vacancy centre in diamond

Philippe Tamarat, N. B. Manson, J. P. Harrison, Roger L. McMurtrie, Alexander P. Nizovtsev, Charles Santori, Raymond G. Beausoleil, Philipp Neumann, T. Gaebel, Fedor Jelezko, Philip Hemmer, Jörg Wrachtrup

Published Apr 30, 2008• 186 citations
Publisher

Abstract

We map out the first excited state sublevel structure of single nitrogen-vacancy (NV) colour centres in diamond. The excited state is an orbital doublet where one branch supports an efficient cycling transition, while the other can simultaneously support fully allowed optical Raman spin-flip transitions. This is crucial for the success of many recently proposed quantum information applications of the NV defects. We further find that an external electric field can be used to completely control the optical properties of a single centre. Finally, a group theoretical model is developed that explains the observations and provides good physical understanding of the excited state structure.

DOI
10.1088/1367-2630/10/4/045004

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We map out the first excited state sublevel structure of single nitrogen-vacancy (NV) colour centres in diamond. The excited state is an orbital doublet where one branch supports an efficient cycling transition, while the other can simultaneously support fully allowed optical Raman spin-flip transitions. This is crucial for the success of many recently proposed quantum information applications of the NV defects. We further find that an external electric field can be used to completely control the optical properties of a single centre. Finally, a group theoretical model is developed that explains the observations and provides good physical understanding of the excited state structure.
Optical and microwave double resonance techniques are used to obtain the excited state structure of single nitrogen-vacancy centers in diamond. The excited state is an orbital doublet and it is shown that it can be split and associated transition strengths varied by external electric fields and by strain. A group theoretical model is developed. It gives a good account of the observations and contributes to an improved understanding of the electronic structure of the center. The findings are important for quantum information processing and other applications of the center.
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 (N-V⁻) colour centre in diamond has potential applications in quantum information processing and single photon generation. It is currently the only known defect in a solid detected at a single site level that has a non-zero spin in the electronic ground state. For the proposed applications it is desirable to have a good understanding of the electronic structure and photodynamics of the centre, however this is currently not the case. Various models have been proposed to explain the fluorescence characteristics observed in single site experiments. The challenge has been to also account for the properties of the centre well-known from observations of the fluorescence from large ensembles of N-V⁻ in diamond. Firstly, that a non-Boltzmann population distribution between the. ground state spin levels is induced by optical excitation. Secondly, that the fluorescence intensity exhibits a strong dependence on the spin orientation. The models proposed to date either cannot account for these properties, or do so only by invoking optical processes that are arbitrary or, in some cases, not physical. In this thesis an alternative model is presented. The derivation of the model, from group theoretical considerations, does not form part of this thesis. This thesis is concerned primarily with a series of independent measurements to determine the transition rates which govern the photodynamics of the centre. When these transition rates are known, there will be no free parameters in the model and the N-V⁻ emission can be simulated for an arbitrary optical field by solving the classical rate equations. To conclude the first part of this thesis, a two-pulse optical excitation is considered and the results of experiment are compared to the predictions of the model. The latter part of t his thesis is concerned with optically detecting single N-V⁻ centres. A confocal microscope system, to enable single site detection, was developed as part of this work. The photon statistics from a single N-V⁻ centre is compared to the statistics predicted by the model. The implications for the modelling of individual N-V⁻ photon statistics are discussed.
We investigate spin-dependent decay and intersystem crossing (ISC) in the optical cycle of single negatively charged nitrogen-vacancy (NV) centres in diamond. We use spin control and pulsed optical excitation to extract both the spin-resolved lifetimes of the excited states and the degree of optically induced spin polarization. By optically exciting the centre with a series of picosecond pulses, we determine the spin-flip probabilities per optical cycle, as well as the spin-dependent probability for ISC. This information, together with the independently measured decay rate of singlet population, provides a full description of spin dynamics in the optical cycle of NV centres. The temperature dependence of the singlet population decay rate provides information about the number of singlet states involved in the optical cycle.
We report a study of the 3E excited-state structure of single negatively charged nitrogen-vacancy (NV) defects in diamond, combining resonant excitation at cryogenic temperatures and optically detected magnetic resonance. A theoretical model is developed and shows excellent agreement with experimental observations. In addition, we show that the two orbital branches associated with the 3E excited state are averaged when operating at room temperature. This study leads to an improved physical understanding of the NV defect electronic structure, which is invaluable for the development of diamond-based quantum information processing.
Nitrogen-vacancy (NV) complex in diamond is one of the most prominent solid state defects as the negatively charged NV defect (NV−) is a leading contender for quantum technologies. In quantum information processing applications, NV− is photoexcited that often leads to photoionization to neutral NV defect, NV0, and re-ionization back to NV− should occur to control the S=1 spin of NV−. As a consequence, understanding the photophysics of NV0 is crucial for controlling NV−. Furthermore, recent studies have shown that the S=1/2 electron spin of NV0 can also be initialized and read out at certain conditions that turns single NV0 a potential quantum bit. Quantum optics protocols rest on detailed knowledge on the electronic structure of the given system, which is obviously missing for NV0 in diamond. In this study, we combine the group theory and density functional theory calculations toward exploring the nature of the ground and excited states of NV0. We show that the effective three-electron system of NV0 leads to high correlation effects that make this system very challenging for ab initio simulations.