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Optics Express

Lifetime investigation of single nitrogen vacancy centres in nanodiamonds

Jelle Storteboom, Philip R. Dolan, Stefania Castelletto, Xiangping Li, Miṅ Gu

Published Apr 22, 2015• 89 citations
Publisher

Abstract

In this paper we investigate at room temperature the excited state lifetime of single NV(-)/NV0 in nanodiamonds at a variety of excitation wavelengths from 510 to 570 nm. The average lifetimes of 25 nanodiamonds with similar sizes exhibit constant values over the entire investigated spectral window. We conclude that the variation observed can be attributed to the specific nanodiamonds. Therefore it is sample dependent, rather than related to the photo-physical properties of the defects. Our study is relevant for the potential use of nanodiamonds containing NV in application where the lifetime is used for sensing the local nano-environment.

DOI
10.1364/oe.23.011327

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In this paper we investigate at room temperature the excited state lifetime of single NV(-)/NV0 in nanodiamonds at a variety of excitation wavelengths from 510 to 570 nm. The average lifetimes of 25 nanodiamonds with similar sizes exhibit constant values over the entire investigated spectral window. We conclude that the variation observed can be attributed to the specific nanodiamonds. Therefore it is sample dependent, rather than related to the photo-physical properties of the defects. Our study is relevant for the potential use of nanodiamonds containing NV in application where the lifetime is used for sensing the local nano-environment.
Colour centres in nanodiamonds provide robust sources of fluorescence and can be used as triggered sources of single photons at room temperature. However, practical devices require stability over thousands of hours of operation, and the use of strong pulsed optical excitation, placing significant burden on the robustness of the emitters that requires bespoke testing. In this work we report the response of single NV centres in nanodiamonds of 50 nm and 100 nm diameter to accelerated lifetime testing, exciting the defects close to saturation around 1013 times to simulate the minimum operational lifetime of a practical device. For nanodiamonds 50 nm in diameter, observed changes in the fluorescence intensity and lifetime suggest a progressive size reduction as a result of the pulsed laser excitation, combined with the introduction of non-radiative centres on or near the nanodiamond surface which affect the quantum efficiency of the NV centre and ultimately lead to photobleaching of the emission. We find examples of NV centres in 100 nm nanodiamonds for which triggered single photon emission remains stable for over these accelerated lifetime tests, demonstrating their suitability for use in practical devices.
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.
Diamond is unique. Whether mechanical, thermal, electrical or optical, its properties are within the most extreme compared to those of any other material. This, together with the fact that in the last fifty years the synthesis of artificial diamond has become a reality, makes it very attractive for engineering and technological purposes. The range of diamond-based applications is very diverse and, among the others, includes its use in mechanical machining, high-power high-frequency electronics and high transmissivity optics. -- Diamond is also host to a wide variety of crystallographic defects. Appropriately controlled, they can be used to tune the characteristics of the material, but even more interestingly they often possess attractive optical properties on their own. In particular, nitrogen-vacancy (NV) centres in diamond have been the subject of extensive study in the last few years. They possess unique room-temperature optical and spin properties which make them promising systems for solid-state qubits in quantum information technologies and for emerging applications in biotechnology, nanomedicine and high resolution magnetometry, such as drug delivery, fluorescent biomarking and spin imaging. -- This thesis is focused on NV centres in diamond. I first present an extensive review on diamond as a material, describing in detail its physical properties, the methods that have been developed to synthesise it and some of its possible applications. I then move the attention specifically to NV centres in nanodiamonds (NDs), i.e. diamond crystals in the nanometre size range (0-100 nm). They are a potential candidate for emerging technologies including high-resolution magnetometry and biomedical imaging. For these applications, specific material requirements, such as the small size of the diamond nanocrystals and the optical stability of the hosted NV centres, are crucial. The NV stability with respect to the nanodiamond size and surface is the central theme of this thesis. I analyse the optical behaviour of NV centres in nanodiamond while varying a number of key parameters such as size, surface termination and diamond origin. Based on the measurements, I conclude whether the nanodiamond size and the NV surface proximity are factors that must be taken into consideration in order to control the material and realise nanotechnologies based on NV centres in nanodiamonds.
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.
Abstract The nitrogen-vacancy (NV) center is one of the most prominent candidates for quantum technologies, and its efficient utilization requires control over its spontaneous emission rate. Here, we report the wavelength-selective enhancement and suppression of NV center emission lifetime at room temperature by modifying the local density of optical states (LDOS) around them. The results are explained using the Barnett–Loudon sum rule and also supported by the LDOS calculations. Two complementary measurement geometries are employed to study the direction-dependent emission behavior from the nanodiamonds decorated on the top of photonic crystals. The lifetime distributions are compared with a proper reference sample using the Kolmogorov–Smirnov test to verify the distinct nature of lifetime distributions. The wavelength-selective enhancement or suppression of emission rates would be useful for NV center-based high-resolution imaging and effective readout of its charge states.
Nitrogen-vacancy (NV) centers in single-crystal CVD diamond are promising candidates for quantum sensing due to their remarkable optical and spin properties [1]. These defects exhibit stable photoluminescence (PL), long spin coherence times, and high sensitivity to external fields [2]. In this study, we present a room-temperature PL characterization of NV centers excited with a 532 nm laser. The setup was optimized for high signal-to-noise ratio and spectral resolution. Key parameters analyzed include emission intensity, zero-phonon line (ZPL) at ~637 nm, phonon sidebands, and the charge state distribution between NV⁰ and NV⁻. The NV⁻ state, crucial for spin-based sensing, is evaluated to understand its stability under different nitrogen doping conditions [3]. The relative intensities of NV⁰ and NV⁻ provide insights into nitrogen incorporation and vacancy formation. These results contribute to optimizing synthesis conditions for enhanced NV⁻ concentration, supporting the advancement of diamond-based quantum sensing technologies.