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CVD-growth of ultra-pure diamond, generation of NV centers by ion-implantation and their spectroscopic characterization for quantum technological applications

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 Added by Tanmoy Chakraborty
 Publication date 2018
  fields Physics
and research's language is English




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Abstract Applications of nitrogen-vacancy (NV) centers in diamond in quantum technology have attracted considerable attention in recent years. Deterministic generation of ensembles of NV centers can advance the research on quantum sensing, many-body quantum systems, multipartite entanglement and so on. Here we report the complete process of controlled generation of NV centers in diamond as well as their characterisation: growing diamond films through chemical vapor deposition (CVD), ion implantation and spectroscopic characterization of the defect centers using a confocal microscope. A microwave-assisted CVD set-up is presented which we constructed for the preparation of single-crystalline homoepitaxial diamond films. The films were prepared with minimized nitrogen concentration, which is confirmed through photoluminescence measurements. We demonstrate an in situ ultra high vacuum (UHV) implantation and heating process for creation of NV centers using a novel experimental set-up. For the first time hot implantation has been shown which prevents surface charging effects. We do not observe graphitization due to UHV heating. By optimizing the implantation parameters it has been possible to implant NV centers in a precise way. We present large area mapping of the samples to determine the distribution of the centers and describe the characterization of the centers by spectroscopic techniques. Reducing the decoherence caused by environmental noise is of primary importance for many applications in quantum technology. We demonstrate improvement on coherence time T_{2} of the NV spins by suppression of their interaction with the surrounding spin-bath using robust dynamical decoupling sequences.



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We characterize single nitrogen-vacancy (NV) centers created by 10-keV N+ ion implantation into diamond via thin SiO$_2$ layers working as screening masks. Despite the relatively high acceleration energy compared with standard ones (< 5 keV) used to create near-surface NV centers, the screening masks modify the distribution of N$^+$ ions to be peaked at the diamond surface [Ito et al., Appl. Phys. Lett. 110, 213105 (2017)]. We examine the relation between coherence times of the NV electronic spins and their depths, demonstrating that a large portion of NV centers are located within 10 nm from the surface, consistent with Monte Carlo simulations. The effect of the surface on the NV spin coherence time is evaluated through noise spectroscopy, surface topography, and X-ray photoelectron spectroscopy.
Stimulated emission is the process fundamental to laser operation, thereby producing coherent photon output. Despite negatively-charged nitrogen-vacancy (NV$^-$) centres being discussed as a potential laser medium since the 1980s, there have been no definitive observations of stimulated emission from ensembles of NV$^-$ to date. Reasons for this lack of demonstration include the short excited state lifetime and the occurrence of photo-ionisation to the neutral charge state by light around the zero-phonon line. Here we show both theoretical and experimental evidence for stimulated emission from NV$^-$ states using light in the phonon-sidebands. Our system uses a continuous wave pump laser at 532 nm and a pulsed stimulating laser that is swept across the phononic sidebands of the NV$^-$. Optimal stimulated emission is demonstrated in the vicinity of the three-phonon line at 700 nm. Furthermore, we show the transition from stimulated emission to photoionisation as the stimulating laser wavelength is reduced from 700nm to 620 nm. While lasing at the zero-phonon line is suppressed by ionisation, our results open the possibility of diamond lasers based on NV centres, tuneable over the phonon-sideband. This broadens the applications of NV magnetometers from single centre nanoscale sensors to a new generation of ultra-precise ensemble laser sensors, which exploit the contrast and signal amplification of a lasing system.
We investigated the depth dependence of coherence times of nitrogen-vacancy (NV) centers through precisely depth controlling by a moderately oxidative at 580{deg}C in air. By successive nanoscale etching, NV centers could be brought close to the diamond surface step by step, which enable us to trace the evolution of the number of NV centers remained in the chip and to study the depth dependence of coherence times of NV centers with the diamond etching. Our results showed that the coherence times of NV centers declined rapidly with the depth reduction in their last about 22 nm before they finally disappeared, revealing a critical depth for the influence of rapid fluctuating surface spin bath. By monitoring the coherence time variation with depth, we could make a shallow NV center with long coherence time for detecting external spins with high sensitivity.
An efficient atom-photon-interface is a key requirement for the integration of solid-state emitters such as color centers in diamond into quantum technology applications. Just like other solid state emitters, however, their emission into free space is severely limited due to the high refractive index of the bulk host crystal. In this work, we present a planar optical antenna based on two silver mirrors coated on a thin single crystal diamond membrane, forming a planar Fabry-Perot cavity that improves the photon extraction from single tin vacancy (SnV) centers as well as their coupling to an excitation laser. Upon numerical optimization of the structure, we find theoretical enhancements in the collectible photon rate by a factor of 60 as compared to the bulk case. As a proof-of-principle demonstration, we fabricate single crystal diamond membranes with sub-$mu$m thickness and create SnV centers by ion implantation. Employing off-resonant excitation, we show a 6-fold enhancement of the collectible photon rate, yielding up to half a million photons per second from a single SnV center. At the same time, we observe a significant reduction of the required excitation power in accordance with theory, demonstrating the functionality of the cavity as an optical antenna. Due to its planar design, the antenna simultaneously provides similar enhancements for a large number of emitters inside the membrane. Furthermore, the monolithic structure provides high mechanical stability and straightforwardly enables operation under cryogenic conditions as required in most spin-photon interface implementations.
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