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Nanotechnology

Nitrogen-driven plasma modulation for tuning silicon-vacancy formation in diamond

Rahul Raj, N. Chandrasekaran, Konda Gokuldoss Pradeep, M. S. Ramachandra Rao

Published Jul 11, 2025• 0 citations
Publisher

Abstract

Abstract Silicon-vacancy (SiV) centers in diamond are promising for quantum photonics due to their narrow zero-phonon line and excellent photonic properties. Here, we demonstrate controlled growth of delta-doped SiV layers in nanocrystalline diamond films by a single-step microwave plasma chemical vapor deposition growth process. By manipulating nitrogen flow during growth, we achieved a uniform layer of SiVs in diamond while maintaining consistent microstructural properties throughout the film. While a correlation between microstructural change and doping density is observed, optical emission spectroscopy analysis reveals that the mechanism between the two processes is different. Atom probe tomography confirms the uniform distribution of silicon atoms in the diamond matrix, even at concentrations as high as 3.6 × 1021 cm−3. The approach shows promise for the precise tuning of the layer thickness and doping concentration, and offers a scalable approach for creating high-quality SiV layers in diamond, advancing their integration into nanophotonic cavities for quantum technologies.

DOI
10.1088/1361-6528/adee9e

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Abstract Silicon-vacancy (SiV) centers in diamond are promising for quantum photonics due to their narrow zero-phonon line and excellent photonic properties. Here, we demonstrate controlled growth of delta-doped SiV layers in nanocrystalline diamond films by a single-step microwave plasma chemical vapor deposition growth process. By manipulating nitrogen flow during growth, we achieved a uniform layer of SiVs in diamond while maintaining consistent microstructural properties throughout the film. While a correlation between microstructural change and doping density is observed, optical emission spectroscopy analysis reveals that the mechanism between the two processes is different. Atom probe tomography confirms the uniform distribution of silicon atoms in the diamond matrix, even at concentrations as high as 3.6 × 1021 cm−3. The approach shows promise for the precise tuning of the layer thickness and doping concentration, and offers a scalable approach for creating high-quality SiV layers in diamond, advancing their integration into nanophotonic cavities for quantum technologies.
Progress in controlling diamond synthesis has made it possible to produce very pure crystals and to incorporate and control atomic impurities and carbon vacancies in the crystal lattice. The appropriate impurity-vacancy combinations can give rise to special defects known as color centers, such as the nitrogen-vacancy (NV) or the silicon-vacancy (SiV), which exhibit exceptional quantum properties with spins that are optically addressable. The use of diamond containing color centers has paved the way for the development of innovative quantum technologies, such as very high-resolution magnetometry and quantum information processing. Nevertheless, the development of quantum sensors at the nanometric scale remains one of the most interesting challenges. In this context, the development of a reliable nanoparticle synthesis technique that allows the desired defects to be incorporated and their quantum optical properties to be modulated is crucial. In this seminar, an efficient and recent method to produce diamond nanoparticles containing NV, SiV and germanium-vacancy (GeV) centers is proposed through direct plasma assisted chemical vapour deposition (CVD) growth. This technique allows good control of both nanoparticle growth processes and color centers formation. The optimization of the CVD nanodiamond growth process is presented, showing the impact of different plasma parameters and gas phasecomposition on nanoparticle crystallinity, size and shape. Morphological characterizations reveal the production of small (around 100 nm) and well faceted nanodiamond particles. In addition, the SiV and GeV color centers incorporation can be tuned within this material by varying the gas phase composition which emphasizes the high flexibility of the CVD growth technique. Finally, the quantum properties of the incorporated color centers have been successfully investigated under extreme pressure conditions (up to ~ 180 GPa) showing a monotonic blue shift of their optical zero-phonon line. Since their luminescence remains stable, SiV and GeV centers emerge as high-pressure nanosensors.
Silicon-vacancy (SiV – ) color center in diamond is of high interest for applications in nanophotonics and quantum information technologies, as a single photon emitter with excellent spectral properties. To obtain spectrally identical SiV – emitters, we doped homoepitaxial diamond films in situ with 28 Si, 29 Si, and 30 Si isotopes using isotopically enriched (>99.9%) silane SiH 4 gas added in H 2 –CH 4 mixtures in the course of the microwave plasma-assisted chemical vapor deposition process. Zero-phonon line components as narrow as ∼4.8 GHz were measured in both absorption and luminescence spectra for the monoisotopic SiV – ensembles with a concentration of a few parts per billion. We determined with high accuracy the Si isotopic energy shift of SiV – zero-phonon line. The SiV – emission intensity is shown to be easily controlled by the doped epifilm thickness. Also, we identified and characterized the localized single photon SiV – sources. The developed doping process opens a way to produce the SiV – emitter ensembles with energy confined in an extremely narrow range.
We demonstrate the coupling of single color centers in diamond to plasmonic and dielectric photonic structures to realize novel nanophotonic devices. Nanometer spatial control in the creation of single color centers in diamond is achieved by implantation of nitrogen atoms through high-aspect-ratio channels in a mica mask. Enhanced broadband single-photon emission is demonstrated by coupling nitrogen-vacancy centers to plasmonic resonators, such as metallic nanoantennas. Improved photon-collection efficiency and directed emission is demonstrated by solid immersion lenses and micropillar cavities. Thereafter, the coupling of diamond nanocrystals to the guided modes of micropillar resonators is discussed along with experimental results. Finally, we present a gas-phase-doping approach to incorporate color centers based on nickel and tungsten, in situ into diamond using microwave-plasma-enhanced chemical vapor deposition. The fabrication of silicon-vacancy centers in nanodiamonds by microwave-plasma-enhanced chemical vapor deposition is discussed in addition.
Arrays of identical and individually addressable qubits lay the foundation for the creation of scalable quantum hardware such as quantum processors and repeaters. Silicon vacancy centers in diamond (SiV) offer excellent physical properties such as low inhomogeneous broadening, fast photon emission, and a large Debye-Waller factor, while the possibility for all-optical ultrafast manipulation and techniques to extend the spin coherence times make them very promising candidates for qubits. Here, we have developed arrays of nanopillars containing single SiV centers with high yield, and we demonstrate ultrafast all-optical complete coherent control of the state of a single SiV center. The high quality of the chemical vapor deposition (CVD) grown SiV centers provides excellent spectral stability, which allows us to coherently manipulate and quasi-resonantly read out the state of individual SiV centers on picosecond timescales using ultrafast optical pulses. This work opens new opportunities towards the creation of a scalable on-chip diamond platform for quantum information processing and scalable nanophotonics applications.
Arrays of identical and individually addressable qubits lay the foundation for the creation of scalable quantum hardware such as quantum processors and repeaters. Silicon-vacancy (SiV) centers in diamond offer excellent physical properties such as low inhomogeneous broadening, fast photon emission, and a large Debye–Waller factor. The possibility for all-optical ultrafast manipulation and techniques to extend the spin coherence times makes them promising candidates for qubits. Here, we have developed arrays of nanopillars containing single (SiV) centers with high yield, and we demonstrate ultrafast all-optical complete coherent control of the excited state population of a single SiV center at the optical transition frequency. The high quality of the chemical vapor deposition (CVD) grown SiV centers provides excellent spectral stability, which allows us to coherently manipulate and quasi-resonantly read out the excited state population of individual SiV centers on picosecond timescales using ultrafast optical pulses. Furthermore, this work opens new opportunities to create a scalable on-chip diamond platform for quantum information processing and scalable nanophotonics applications.
We introduce a process for the fabrication of high-quality, spatially isolated nano-diamonds on iridium via microwave-plasma-assisted chemical vapour deposition (CVD) growth. We perform spectroscopy of single silicon-vacancy (SiV) centres produced during the growth of the nano-diamonds. The colour centres exhibit extraordinary narrow zero-phonon-lines down to 0.7 nm at room temperature. Single photon count rates up to 4.8 Mcps at saturation make these SiV centres the brightest diamond-based single photon sources to date. We measure for the first time the fine structure of a single SiV centre, thus confirming the atomic composition of the investigated colour centres.