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Scientific Reports

Fluorescence Polarization Switching from a Single Silicon Vacancy Colour Centre in Diamond

Yan Liu, Gengxu Chen, Youying Rong, Liam Paul McGuinness, Fedor Jelezko, Syuto Tamura, Takashi Tanii, Tokuyuki Teraji, Shinobu Onoda, Takeshi Ohshima, Junichi Isoya, Takahiro Shinada, E Wu, Heping Zeng

Published Jul 23, 2015• 16 citations
Publisher

Abstract

Single-photon emitters with stable and uniform photoluminescence properties are important for quantum technology. However, in many cases, colour centres in diamond exhibit spectral diffusion and photoluminescence intensity fluctuation. It is therefore essential to investigate the dynamics of colour centres at the single defect level in order to enable the on-demand manipulation and improved applications in quantum technology. Here we report the polarization switching, intensity jumps and spectral shifting observed on a negatively charged single silicon-vacancy colour centre in diamond. The observed phenomena elucidate the single emitter dynamics induced by photoionization of nearby electron donors in the diamond.

DOI
10.1038/srep12244

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The negatively charged silicon-vacancy (SiV${}^{\ensuremath{-}}$) center in diamond is a promising single-photon source for quantum communications and information processing. However, the center's implementation in such quantum technologies is hindered by contention surrounding its fundamental properties. Here we present optical polarization measurements of single centers in bulk diamond that resolve this state of contention and establish that the center has a $\ensuremath{\langle}111\ensuremath{\rangle}$ aligned split-vacancy structure with ${\mathrm{D}}_{3\mathrm{d}}$ symmetry. Furthermore, we identify an additional electronic level and evidence for the presence of dynamic Jahn-Teller effects in the center's 738-nm optical resonance.

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Single-photon emitters with stable and uniform photoluminescence properties are important for quantum technology. However, in many cases, colour centres in diamond exhibit spectral diffusion and photoluminescence intensity fluctuation. It is therefore essential to investigate the dynamics of colour centres at the single defect level in order to enable the on-demand manipulation and improved applications in quantum technology. Here we report the polarization switching, intensity jumps and spectral shifting observed on a negatively charged single silicon-vacancy colour centre in diamond. The observed phenomena elucidate the single emitter dynamics induced by photoionization of nearby electron donors in the diamond.
Nitrogen–vacancy (NV) colour centres in diamond are attractive fluorescence emitters owing to their unprecedented photostability and superior applicability to spin manipulation and sub-diffraction far-field optical microscopy. However, some applications are limited by the co-occurrence of dark state population and optical excitation. In this paper, we use fluorescence microscopy and correlation spectroscopy on single negatively charged NV centres in type IIa bulk diamond to unravel the population kinetics of a >100 s long-lived dark state. The bright–dark state interconversion rates show a quadratic dependence on the applied laser intensity, which implies that higher excited states are involved. Depopulation of the dark state becomes less effective at wavelengths above 532 nm, resulting in a complete fluorescence switch-off at wavelengths >600 nm. This switch is reversible by the addition of shorter wavelengths. This behaviour can be explained by a model consisting of three dark and three bright states of different excitation levels, with the most efficient interconversion via the respective higher excited states. This model accounts for the nonlinear dark state and photoswitching kinetics, as well as for the decrease of the NV's fluorescence lifetime with excitation intensity and the strong dependence of fluorescence emission on excitation intensity. Unfortunately, our data do not give enough insight to allow us to assign the different states to specific electronic states known from the literature. Nevertheless, our observations allowed us to improve the recording of fluorescence images of single NV centres with sub-diffraction spatial resolution but they also have important implications for studying their spin states.
Abstract Optical “blinking” normally refers to a switching behavior of fluorescence for quantum emissions between “ON” and “OFF” state. For quantum dots, single molecules, and nitrogen‐vacancy centers in diamond, it usually stems from conversions between two different charge states, with one emitting strong and bright fluorescence while the other scattering weak or no fluorescence. Here, a different type of blinking from single emitters in ion implanted diamond is reported, with both blinking states exhibiting detectable photoluminescence under nonresonant excitation. Thanks to the low jumping rates, the dynamics of the emission can be directly monitored. The quadratic power dependence of the conversion rates suggests the possibility of two‐photon ionization process in quantum jumps. This work provides extra insights into the photodynamics of the spectral jumps on defect‐based single‐photon emitters hosted in wide‐bandgap semiconductors.
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.
Single negatively charged nitrogen-vacancy (NV-) defect centres in diamond are attractive systems for the implementation of solid state quantum information processing (QIP) and quantum key distribution (QKD). In both approaches, the coupling of an individual NV-centre to a resonant microcavity is of interest: it would improve the optical readout of the NV-centre electron spin state in QIP and enhance the collection efficiency of the single photon fluorescence in QKD while increasing the coherence length of the emission. We theoretically demonstrate that, at room temperature, the coupling to a single-mode Fabry-Perot microcavity can be used to obtain a fluorescence spectrum narrowing without loss of total intensity. We also experimentally demonstrate the control of the fluorescence spectrum of a single NV-centre by adjusting the thickness of the microcavity. Finally, we report a doubling of the emission spectral density with respect to the single mirror configuration.
In the last decade atom-sized point defects in diamond, so called colour centres, have proven to be suitable systems for quantum information processing as well as quantum communication and sensing applications. Besides the wellknown nitrogen vacancy centre, the negatively charged silicon vacancy centre has recently proven to be a promising candidate due to its superior spectral properties such as narrow zero-phonon line widths and small phonon sidebands. In this feature article (article No.201700586) the authors summarize the center's electronic and optical properties as well as recent advances in controlling its quantum state using microwave as well as ultrafast all-optical control techniques which make it accessible for future quantum information processing applications. Moreover, the authors outline potential future experimental directions to improve the center's coherence time scale which so far is limited by phonon-induced decoherence. The cover picture shows an artistic representation of the silicon vacancy centre with its inversion-symmetric structure in a diamond crystal being addressed by an ultrashort laser pulse.
The negatively charged silicon-vacancy (SiV${}^{\ensuremath{-}}$) center in diamond is a promising single-photon source for quantum communications and information processing. However, the center's implementation in such quantum technologies is hindered by contention surrounding its fundamental properties. Here we present optical polarization measurements of single centers in bulk diamond that resolve this state of contention and establish that the center has a $\ensuremath{\langle}111\ensuremath{\rangle}$ aligned split-vacancy structure with D3d{\mathrm{D}}_{3\mathrm{d}}D3d​ symmetry. Furthermore, we identify an additional electronic level and evidence for the presence of dynamic Jahn-Teller effects in the center's 738-nm optical resonance.