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arXiv:1011.1822 · New Journal of Physics

Ultrabright and efficient single-photon generation based on nitrogen-vacancy centres in nanodiamonds on a solid immersion lens

Tim Schröder, Friedemann Gädeke, Moritz J. Banholzer, Oliver J. Benson

Published May 26, 2011• 133 citations
arXivHTMLPDF

Abstract

Single photons are fundamental elements for quantum information technologies such as quantum cryptography, quantum information storage and optical quantum computing. Colour centres in diamond have proven to be stable single-photon sources and thus essential components for reliable and integrated quantum information technology. A key requirement for such applications is a large photon flux and a high efficiency. Paying tribute to various attempts to maximize the single-photon flux, we show that collection efficiencies of photons from colour centres can be increased with a rather simple experimental setup. To do so, we spin-coated nanodiamonds containing single nitrogen-vacancy (N-V) colour centres on the flat surface of a ZrO 2 solid immersion lens. We found stable single-photon count rates of up to 853 kcts s − 1 at saturation under continuous wave excitation while having access to more than 100 defect centres with count rates from 400 to 500 kcts s − 1 . For a blinking defect centre, we found count rates up to 2.4 Mcts s − 1 for time intervals of several tens of seconds. It seems to be a general feature that very high rates are accompanied by blinking behaviour. The overall collection efficiency of our setup of up to 4.2% is the highest yet reported for N-V defect centres in diamond. Under pulsed excitation of a stable emitter of 10 MHz, 2.2% of all pulses caused a click on the detector adding to 221 kcts s − 1 thus, opening the way towards diamond-based on-demand single-photon sources for quantum applications.

DOI
10.1088/1367-2630/13/5/055017

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Single photons are fundamental elements for quantum information technologies such as quantum cryptography, quantum information storage and optical quantum computing. Colour centres in diamond have proven to be stable single-photon sources and thus essential components for reliable and integrated quantum information technology. A key requirement for such applications is a large photon flux and a high efficiency. Paying tribute to various attempts to maximize the single-photon flux, we show that collection efficiencies of photons from colour centres can be increased with a rather simple experimental setup. To do so, we spin-coated nanodiamonds containing single nitrogen-vacancy (N-V) colour centres on the flat surface of a ZrO 2 solid immersion lens. We found stable single-photon count rates of up to 853 kcts s − 1 at saturation under continuous wave excitation while having access to more than 100 defect centres with count rates from 400 to 500 kcts s − 1 . For a blinking defect centre, we found count rates up to 2.4 Mcts s − 1 for time intervals of several tens of seconds. It seems to be a general feature that very high rates are accompanied by blinking behaviour. The overall collection efficiency of our setup of up to 4.2% is the highest yet reported for N-V defect centres in diamond. Under pulsed excitation of a stable emitter of 10 MHz, 2.2% of all pulses caused a click on the detector adding to 221 kcts s − 1 thus, opening the way towards diamond-based on-demand single-photon sources for quantum applications.
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.
For applications in Quantum Information and Quantum Key Distribution an on-demand source of single photons is desirable because absolute security is of utmost importance. Photons are quantum systems; hence encoding information onto them offers a secure alternative to classical cryptography as a measurement cannot be performed on photons without altering their properties. The Nitrogen Vacancy (NV) centre in diamond is a good source of such photons. It is photo-stable and its location in diamond offers robustness. It has zero phonon line at 637 nm and its relative short luminescence life-time of about 12 ns makes it suitable for generating single photons. This thesis covers two aspects: Firstly the characterization of defects in diamonds and subsequent selection of diamonds suitable for use in the single photon setup and secondly, the development of the experimental setup for single photon generation. This thesis sets out to describe the development of a laboratory based single photon source using the NV centre in diamond. For this purpose a suite of diamond samples were selected and subjected to various spectroscopic tests in order to characterize and classify the samples, especially the presence of the NV centres and their concentrations. The characterization of the defects was done through the use of the following spectroscopic techniques: UltravioletVisible-Near infrared spectroscopy, Infrared spectroscopy, Electron Spin Resonance and Photoluminescence. These techniques enabled us to understand the types and origins of crystal defects that were present in the diamond samples used in this study and to use this to select diamonds that are most suitable for use in generation of single photons. The experimental setup for single photon generation using the NV centre is based on a confocal microscope arrangement. Single NV centres were identified by measuring the second order autocorrelation function of the fluorescence light emitted by the sample when illuminated with a laser. This measurement was done using a Hanbury-Brown Twiss (HBT) interferometer.
The development of reliable devices to generate single photons is crucial for applications in quantum cryptography, as well as for fundamental quantum optics experiments. Due to their extremely high photostability at room temperature, optically active defects in solids, the so called color centers, are among the most promising candidates. Single NV (nitrogen-vacancy) centers in diamond have been demonstrated to be able to generate single photons and have already shown advantages compared to attenuated laser pulses in a quantum cryptography experiment. The nitrogen-vacancy center (NV center) in diamond consists of a substitutional nitrogen atom and an adjacent vacancy. This complex exhibits an optical transition with a fluorescence lifetime of 11.6 ns. The room temperature spectrum of the NV center consists of the zero-phonon line at 637 nm and broad phononic sidebands with a FWHM of more than 100 nm. Due to the existence of a shelving level the efficiency of the NV center as a single photon source is limited. Additionally, the high diffraction index of bulk diamond restricts the efficiency to collect the fluorescence light.
Single-photon sources are a fundamental element for developing quantum technologies, and sources based on colour centres in diamonds are among the most promising candidates. The well-known nitrogen vacancy centres are characterized by several limitations, and thus few other defects have recently been considered. In the present work, we characterize, in detail, native efficient single colour centres emitting in the near infra-red ( λ = 740–780 nm) in both standard IIa single-crystal and electronic-grade polycrystalline commercial chemical vapour deposited (CVD) diamond samples. In the former case, a high-temperature ( T > 1000 °C) annealing process in vacuum is necessary to induce the formation/activation of luminescent centres with good emission properties, while in the latter case the annealing process has marginally beneficial effects on the number and performance of native centres in commercially available samples. Although displaying significant variability in several photo-physical properties (emission wavelength, emission rate instabilities, saturation behaviours), these centres generally display appealing photophysical properties for applications as single photon sources: short lifetimes (0.7–3 ns), high emission rates (∼50–500 × 10 3 photons s −1 ) and strongly (>95%) polarized light. The native centres are tentatively attributed to impurities incorporated in the diamond crystal during the CVD growth of high-quality type-IIa samples, and offer promising perspectives in diamond-based photonics.
Single-photon sources represent a key enabling technology in quantum optics, and single color centers in diamond are a promising platform to serve this purpose, due to their high quantum efficiency and photostability at room temperature. The widely studied nitrogen-vacancy (NV) centers are characterized by several limitations, thus other defects have recently been considered, with a specific focus of centers emitting in the near-infra red (NIR). In the present work, we report on the coupling of native NIR-emitting centers in high-quality single-crystal diamond with solid immersion lens (SIL) structures fabricated by focused ion beam (FIB) lithography. The reported improvements in terms of light collection efficiency make the proposed system an ideal platform for the development of single-photon emitters with appealing photophysical and spectral properties.