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Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)

Quenching dynamics and photo-physics of nitrogen-vacancy centres in nanodiamonds

Reece P. Roberts, Mathieu L. Juan, Gabriel Molina‐Terriza

Published Jun 1, 2017• 0 citations
Publisher

Abstract

The Nitrogen Vacancy (NV) centre is a point defect consisting of a nitrogen-vacancy lattice pair embedded in diamond. The NV centre has two stable charge states, the neutral charge state and the (NV0) and the negatively charged state (NV-) with photo induced interconversion between these two states [1]. The NV centre is an intensively studied material that has shown a wide range of applications in both Physics and Biology due to its high stability and interesting optical properties. Applications ranging from imaging and tracking biological structures, to nanoscale sensing, to applications in highly controlled quantum experiments have all been realised using these centres [2, 3]. However, these applications rely only on the NV-charge stage and often neglect the effects of the neutral charge state. As a result the NV0charge state has not received the same level of study as the NV-state and the effects of the interconversion between the two states are poorly understood, even though it can have a significant effect on the emitted fluorescence.

DOI
10.1109/cleoe-eqec.2017.8087613

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The Nitrogen Vacancy (NV) centre is a point defect consisting of a nitrogen-vacancy lattice pair embedded in diamond. The NV centre has two stable charge states, the neutral charge state and the (NV0) and the negatively charged state (NV-) with photo induced interconversion between these two states [1]. The NV centre is an intensively studied material that has shown a wide range of applications in both Physics and Biology due to its high stability and interesting optical properties. Applications ranging from imaging and tracking biological structures, to nanoscale sensing, to applications in highly controlled quantum experiments have all been realised using these centres [2, 3]. However, these applications rely only on the NV-charge stage and often neglect the effects of the neutral charge state. As a result the NV0charge state has not received the same level of study as the NV-state and the effects of the interconversion between the two states are poorly understood, even though it can have a significant effect on the emitted fluorescence.
The nitrogen vacancy (NV) center in diamond is the most widely studied color center in diamond for its wide range of applications in both physics and biology. The negatively charged state ${\mathrm{NV}}^{\ensuremath{-}}$ is often favored for its better spin-optical properties, whereas the presence of the neutral charge state NV0{\mathrm{NV}}^{0}NV0 is often minimized or neglected by using a single optimized excitation wavelength. In many cases, the use of additional laser wavelengths has an important impact on the NV optical properties and can lead to a dramatically quenched fluorescence. Through measurements of the photophysics of the NV center we show in this work that this quenching mechanism is mediated by charge state interconversion providing additional channels for nonradiative decay. Our results show that this mechanism is also sensitive to the spin state of the ${\mathrm{NV}}^{\ensuremath{-}}$. A better understanding of this physical mechanism will help mitigate the spin and charge state depolarization effects that are detrimental for quantum technology applications.
The nitrogen–vacancy centre (NV) has drawn much attention for over a decade, yet detailed knowledge of the photophysics needs to be established. Under typical conditions, the NV can have two stable charge states, negative (NV − ) or neutral (NV 0 ), with photo-induced interconversion of these two states. Here, we present detailed studies of the ionization dynamics of single NV centres in bulk diamond at room temperature during illumination and its dependence on the excitation wavelength and power. We apply a recent method which allows us to directly measure the charge state of a single NV centre, and observe its temporal evolution. We find that the steady-state NV − population is always ⩽75% for 450–610 nm excitation wavelength. In combination with saturation measurements, we show that the optimal excitation wavelength is around 510–540 nm. Furthermore, the relative absorption cross-section of NV − is determined for 540–610 nm, revealing a double-peak structure. Finally, the energy of the NV − ground state of 2.6 eV below the conduction band is measured. These results reveal new insights into the charge state dynamics of the NV centre.
The NV defect center in diamond forms a pseudo-atomic quantum system with discreet optically excitable transitions between ground and excited states in the gap between valence and conduction bands, making the NV center a deep-level defect center in diamond. For the negatively charged NV center (NV-), both the ground and excited states are spin triplets (S=1) and coupling between optical and spin states provides unique opportunities for optical detection of magnetic resonance (ODMR) and quantum metrology under ambient conditions. As an atomically sized point defect that is stable in single nanodiamonds as small as a few nanometers, the NV center enables spin based imaging of temperature, electric fields, magnetic fields and mechanical strain with nanoscale spatial resolution. Made of carbon, nanodiamonds are also ideal nanoparticles for use in biological systems, exhibiting extremely low cytotoxicity, no photo bleaching and exceptional contrast in transmission electron and light microscopy. With the ability to act as both a passive, non perturbing sensor (e.g. a diamagnetic material used for sensing magnetic fields) and a connection point for two way, direct coupling of far field optics to NV−^-− spins and indirectly to the highly localized neighborhood of atoms, electronic states and phonon modes in the local vicinity, NV diamond provides a route to nanoscale field sensing and spin based optical microscopy. These sensors are also stable in nanodiamonds. For nanoparticles, the reduction in particle diameter dramatically enhances the proportion of the material that is surface exposed, enhancing any surface related properties. Nitrogen Vacancy centers in nanodiamonds provide another example of material properties that vary with particle size. In chapter 5, evidence that modulation of nanodiamonds fluorescent emissions by electrical perturbations in their surrouding environment allows transduction of local electrodynamics into a far field optical signal capable of mapping action potentials in cardiomyocytes in presented. The unifying theme for all of the work presented in this dissertation is to enable the use of magnetic resonance signals and interactions for imaging and sensing in previously inaccessible regimes. The specific focus is on methods and techniques to enable nanoscale physical sensing and functional imaging in live tissues, with the ultimate aim to lay the predicate for the combination of both without compromise.
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.
The nitrogen-vacancy (NV) centre in diamond is a perfect candidate for quantum sensing applications applied to numerous fields of science. Past studies improved the sensitivity of diamonds containing NV centres by increasing their density or prolonging their coherence time. However, few studies discussed the effects of other defects inside the diamond crystal on the sensitivity of the NV centres. In this study, we demonstrated the implication of single substitutional nitrogen defects on the fluorescence emission, charge state stability, coherence time and sensitivity of the NV centres. We found that there is an optimal concentration of nitrogen defects that allows diamond samples to have a high-density of NV centres and high fluorescence without significantly affecting the coherence time. This results will inform the correct choice of diamond characteristics for current and future quantum sensing applications with the NV centres.
One of the most common impurities in synthetic diamond is single substitutional nitrogen, which is incorporated in the diamond lattice substituting a carbon atom. If the nitrogen is adjacent to a vacancy in the diamond lattice, it forms the nitrogen-vacancy (NV) colour centre (CC). The negatively charged state of this CC, NV-, is particularly well studied since its quantum properties are suitable for applications such as quantum information processing, single-photon sources and optical magnetometry. NV CCs in the neutral state (NV0) are less widely studied. This CC exhibits broadband luminescence at slightly shorter wavelengths than NV-, and hence is also potentially of interest for tuneable and ultrafast visible laser applications. In this report, we present a detailed study of the laser-related spectroscopic properties of a diamond containing NV0 and NV-CCs.