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Register a new userSynthesis of Luminescent Eu defects in diamond
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Lanthanides are vital components in lighting, imaging technologies and future quantum memory applications due to their narrow optical transitions and long spin coherence times. Recently, diamond has become a preeminent platform for realization of many experiments in quantum information science. In this work, we demonstrate a promising approach to incorporate Eu ions into single crystal diamond and nanodiamonds, providing a means to harness the exceptional characteristics of both lanthanides and diamond in a single material. Polyelectrolytes are used to electrostatically assemble Eu(III) chelate molecules on diamond and subsequently chemical vapor deposition is employed for the growth of a high quality diamond crystal. Photoluminescence, cathodoluminescence and time resolved fluorescence measurements show that the Eu atoms retain the characteristic optical signature of Eu(III) upon incorporation into the diamond lattice. Computational modelling supports the experimental findings, corroborating that Eu3+ in diamond is a stable configuration within the diamond bandgap. The versatility of the synthetic technique is further illustrated through the creation of the well-studied Cr defect center. Together these defect centers demonstrate the outstanding chemical control over the incorporation of impurities into diamond enabled by the electrostatic assembly together with chemical vapour deposition growth.
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Atomic-size spin defects in solids are unique quantum systems. Most applications require nanometer positioning accuracy, which is typically achieved by low energy ion implantation. So far, a drawback of this technique is the significant residual implantation-induced damage to the lattice, which strongly degrades the performance of spins in quantum applications. In this letter we show that the charge state of implantation-induced defects drastically influences the formation of lattice defects during thermal annealing. We demonstrate that charging of vacancies localized at e.g. individual nitrogen implantation sites suppresses the formation of vacancy complexes, resulting in a tenfold-improved spin coherence time of single nitrogen-vacancy (NV) centers in diamond. This has been achieved by confining implantation defects into the space charge layer of free carriers generated by a nanometer-thin boron-doped diamond structure. Besides, a twofold-improved yield of formation of NV centers is observed. By combining these results with numerical calculations, we arrive at a quantitative understanding of the formation and dynamics of the implanted spin defects. The presented results pave the way for improved engineering of diamond spin defect quantum devices and other solid-state quantum systems.
The incorporation of Eu into the diamond lattice is investigated in a combined theoretical-experimental study. The large size of the Eu ion induces a strain on the host lattice, which is minimal for the Eu-vacancy complex. The oxidation state of Eu is calculated to be 3+ for all defect models considered. In contrast, the total charge of the defect-complexes is shown to be negative -1.5 to -2.3 electron. Hybrid-functional electronic-band-structures show the luminescence of the Eu defect to be strongly dependent on the local defect geometry. The 4-coordinated Eu substitutional dopant is the most promising candidate to present the typical Eu3+ luminescence, while the 6-coordinated Eu-vacancy complex is expected not to present any luminescent behaviour. Preliminary experimental results on the treatment of diamond films with Eu-containing precursor indicate the possible incorporation of Eu into diamond films treated by drop-casting. Changes in the PL spectrum, with the main luminescent peak shifting from approximately 614 nm to 611 nm after the growth plasma exposure, and the appearance of a shoulder peak at 625 nm indicate the potential incorporation. Drop-casting treatment with an electronegative polymer material was shown not to be necessary to observe the Eu signature following the plasma exposure, and increased the background luminescence.
In this work, we present a computational scheme for isolating the vibrational spectrum of a defect in a solid. By quantifying the defect character of the atom-projected vibrational spectra, the contributing atoms are identified and the strength of their contribution determined. This method could be used to systematically improve phonon fragment calculations. More interestingly, using the atom-projected vibrational spectra of the defect atoms directly, it is possible to obtain a well-converged defect spectrum at lower computational cost, which also incorporates the host-lattice interactions. Using diamond as the host material, four test case defects, each presenting a distinctly different vibrational behaviour, are considered: a heavy substitutional dopant (Eu), two intrinsic defects (neutral vacancy and split interstitial), and the negatively charged N-vacancy center. The heavy dopant and split interstitial present localized modes at low and high frequencies, respectively, showing little overlap with the host spectrum. In contrast, the neutral vacancy and the N-vacancy center show a broad contribution to the upper spectral range of the host spectrum, making them challenging to extract. Independent of the vibrational behaviour, the main atoms contributing to the defect spectrum can be clearly identified. Recombination of their atom-projected spectra results in the isolated defect spectrum.
We used optical confocal microscopy to study optical properties of diamond 50 nm nanocrystals first irradiated with an electron beam, then dispersed as a colloidal solution and finally deposited on a silica slide. At room temperature, under CW laser excitation at a wavelength of 514.5 nm we observed perfectly photostable single Nitrogen-Vacancy (NV) colour defects embedded in the nanocrystals. From the zero-phonon line around 575 nm in the spectrum of emitted light, we infer a neutral NV0 type of defect. Such nanoparticle with intrinsic fluorescence are highly promising for applications in biology where long-term emitting fluorescent bio-compatible nanoprobes are still missing.
We report a systematic investigation on the spectral splitting of negatively charged, nitrogen-vacancy (NV-) photo-luminescent emission in single crystal diamond induced by strain engineering. The stress fields arise from MeV ion-induced conversion of diamond to amorphous and graphitic material in regions proximal to the centers of interest. In low-nitrogen sectors of a HPHT diamond, clearly distinguishable spectral components in the NV- emission develop over a range of 4.8 THz corresponding to distinct alignment of sub-ensembles which were mapped with micron spatial resolution. This method provides opportunities for the creation and selection of aligned NV- centers for ensemble quantum information protocols.
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