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arXiv:1807.04028 · Optica

Laser writing of individual nitrogen-vacancy defects in diamond with near-unity yield

Yu-Chen Chen, Benjamin Griffiths, Laiyi Weng, Shannon S. Nicley, Shazeaa N. Ishmael, Yashna Lekhai, Sam Johnson, Colin J. Stephen, Ben L. Green, Gavin W. Morley, Mark E. Newton, Martin J. Booth, Patrick S. Salter, Jason M. Smith

Published May 10, 2019• 167 citations
arXivHTMLPDF

Abstract

Atomic defects in wide band gap materials show great promise for development of a new generation of quantum information technologies, but have been hampered by the inability to produce and engineer the defects in a controlled way. The nitrogen-vacancy (NV) color center in diamond is one of the foremost candidates, with single defects allowing optical addressing of electron spin and nuclear spin degrees of freedom with potential for applications in advanced sensing and computing. Here we demonstrate a method for the deterministic writing of individual NV centers at selected locations with high positioning accuracy using laser processing with online fluorescence feedback. This method provides a new tool for the fabrication of engineered materials and devices for quantum technologies and offers insight into the diffusion dynamics of point defects in solids.

DOI
10.1364/optica.6.000662

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Colour centre defects in diamond are promising candidates for many quantum technologies because they act as isolated two level systems in the solid-state that can be controlled and read-out through photonics [1][2][3]. Realisation of these technologies requires the placement of many highly coherent centres in a regular array with high positional accuracy and high fabrication yield [4]. Previous fabrication techniques have lacked the ability to produce high yields with high positional accuracy without causing irreparable damage to the lattice which reduced the quality of the spin and optical properties [5]. Ultra-fast laser writing has been shown to produce highly coherent nitrogen vacancy (NV) colour centres within the diamond lattice with positional accuracies of order hundreds of nanometers and a stochastic yield. In this case, the yield and positional accuracy is held back by the need to thermally anneal the diamond within a furnace to convert laser generated defects into colour centres; a fabrication step in which there is little to no control over individual site [6]. In this thesis, the ultra-fast pulsed laser writing technique is broached in detail from both a theoretical and experimental standpoint. The theory behind the highly non-linear light-matter interactions is studied and a hypothesis is developed for the energy transfer between photo-excited carriers and the lattice via the non-radiative recombination of self-trapped multi-excitonic states [7]. In addition, this thesis presents an expansion on the laser writing of colour centres through broaching the generation of different colour centres that have some preferential properties over the NV [8], and the development of a new engineering technique involving a local laser anneal [9]. The yield of generated centres is increased from stochastic to deterministic by replacing the global thermal anneal with the local laser anneal in combination with a fluorescence feedback mechanism. In addition, the use of the laser to locally anneal generated centres leads to a factor of five improvement in the positional accuracy due to the highly non-linear interaction of the laser with the material. These results culminate in a key step forward in the development of a large scale quantum device and improved understanding of the highly dynamical processes that occur upon femtosecond laser interaction with a wide bandgap material.

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Abstract We report the deterministic writing of single nitrogen-vacancy defects in commercially available high purity diamond using only laser processing. The positioning accuracy of the single defects is around 250 nm and about 20% of the written defects display near transform-limited optical transitions at a temperature of 5 K. The results represent a significant step towards defect-engineered devices using colour centres as coherent spin-photon interfaces for quantum technologies, and shed light on the physical mechanism for laser-induced vacancy diffusion in diamond.

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Control over the charge states of color centers in solids is necessary to fully utilize them in quantum technologies. However, the microscopic charge dynamics of deep defects in wide-band-gap semiconductors are complex, and much remains unknown. We utilize a single-shot charge-state readout of an individual nitrogen-vacancy (NV) center to probe the charge dynamics of the surrounding defects in diamond. We show that the NV center charge state can be converted through the capture of holes produced by optical illumination of defects many micrometers away. With this method, we study the optical charge conversion of silicon-vacancy (SiV) centers and provide evidence that the dark state of the SiV center under optical illumination is SiV 2– . These measurements illustrate that charge carrier generation, transport, and capture are important considerations in the design and implementation of quantum devices with color centers and provide a novel way to probe and control charge dynamics in diamond.

arXiv:2106.05405•Nano Letters•Aug 2, 2021•20 citations
Atomic defects in wide band gap materials show great promise for development of a new generation of quantum information technologies, but have been hampered by the inability to produce and engineer the defects in a controlled way. The nitrogen-vacancy (NV) color center in diamond is one of the foremost candidates, with single defects allowing optical addressing of electron spin and nuclear spin degrees of freedom with potential for applications in advanced sensing and computing. Here we demonstrate a method for the deterministic writing of individual NV centers at selected locations with high positioning accuracy using laser processing with online fluorescence feedback. This method provides a new tool for the fabrication of engineered materials and devices for quantum technologies and offers insight into the diffusion dynamics of point defects in solids.
Colour centre defects in diamond are promising candidates for many quantum technologies because they act as isolated two level systems in the solid-state that can be controlled and read-out through photonics [1][2][3]. Realisation of these technologies requires the placement of many highly coherent centres in a regular array with high positional accuracy and high fabrication yield [4]. Previous fabrication techniques have lacked the ability to produce high yields with high positional accuracy without causing irreparable damage to the lattice which reduced the quality of the spin and optical properties [5]. Ultra-fast laser writing has been shown to produce highly coherent nitrogen vacancy (NV) colour centres within the diamond lattice with positional accuracies of order hundreds of nanometers and a stochastic yield. In this case, the yield and positional accuracy is held back by the need to thermally anneal the diamond within a furnace to convert laser generated defects into colour centres; a fabrication step in which there is little to no control over individual site [6]. In this thesis, the ultra-fast pulsed laser writing technique is broached in detail from both a theoretical and experimental standpoint. The theory behind the highly non-linear light-matter interactions is studied and a hypothesis is developed for the energy transfer between photo-excited carriers and the lattice via the non-radiative recombination of self-trapped multi-excitonic states [7]. In addition, this thesis presents an expansion on the laser writing of colour centres through broaching the generation of different colour centres that have some preferential properties over the NV [8], and the development of a new engineering technique involving a local laser anneal [9]. The yield of generated centres is increased from stochastic to deterministic by replacing the global thermal anneal with the local laser anneal in combination with a fluorescence feedback mechanism. In addition, the use of the laser to locally anneal generated centres leads to a factor of five improvement in the positional accuracy due to the highly non-linear interaction of the laser with the material. These results culminate in a key step forward in the development of a large scale quantum device and improved understanding of the highly dynamical processes that occur upon femtosecond laser interaction with a wide bandgap material.
Abstract We report the deterministic writing of single nitrogen-vacancy defects in commercially available high purity diamond using only laser processing. The positioning accuracy of the single defects is around 250 nm and about 20% of the written defects display near transform-limited optical transitions at a temperature of 5 K. The results represent a significant step towards defect-engineered devices using colour centres as coherent spin-photon interfaces for quantum technologies, and shed light on the physical mechanism for laser-induced vacancy diffusion in diamond.
Diamond's nitrogen vacancy (NV) center is an optically active defect with long spin coherence times, showing great potential for both efficient nanoscale magnetometry and quantum information processing schemes. Recently, both the formation of buried 3D optical waveguides and high-quality single NVs in diamond were demonstrated using the versatile femtosecond laser-writing technique. However, until now, combining these technologies has been an outstanding challenge. In this Letter, we fabricate laser-written photonic waveguides in quantum grade diamond which are aligned to within micron resolution to single laser-written NVs, enabling an integrated platform providing deterministically positioned waveguide-coupled NVs. This fabrication technology opens the way toward on-chip optical routing of single photons between NVs and optically integrated spin-based sensing.
Introduction Nitrogen-vacancy (NV) centers in diamond are widely recognized as highly promising solid-state quantum sensors due to their long room temperature coherence times and atomic-scale size, which enable exceptional sensitivity and nanoscale spatial resolution under ambient conditions. Ultrafast laser writing has demonstrated the deterministic spatial control of individual NV− centers, however, the resulting random orientation of the defect axis limits the magnetic field sensitivity and signal contrast. Methods We developed an all-optical approach for reorienting laser-written NV− centers to lie along a specific crystallographic axis using femtosecond laser annealing. The orientation is determined by polarization analysis, and the annealing and subsequent polarization analysis are repeated until the desired orientation is observed. Results Our method achieves deterministic alignment of NV− centers along the optical axis in (111)-oriented diamond substrates and allows selection between two observable orientation classes in (100)-oriented substrates. The reorientation preserves spatial ordering while producing uniform orientation across arrays of NV− centers. Discussion This approach enables scalable fabrication of orientation-controlled NV− arrays, and paves the way for scalable, high performance quantum devices based on orientation-controlled NV− centers.
Nitrogen-vacancy (NV) color centers in diamond have emerged as a focal point in quantum technology research due to their exceptional optical and electronic spin properties. This discovery not only expands our understanding of the material properties of diamond but also paves the way for practical applications in quantum technology. As a solid-state spin quantum system characterized by long electron spin coherence times and stable performance, NV color centers offer distinct advantages in quantum information processing. Recent advancements have enabled the fabrication of high-quality NV color centers with controllable concentration and spatial positioning through techniques such as in situ doping, ion implantation, and hybrid approaches. These technological breakthroughs have significantly enhanced the efficiency of NV center fabrication, thereby establishing a robust foundation for their widespread application in quantum sensing and quantum information technologies. This review provides a compre­hensive introduction to the structure and fundamental properties of NV color centers in diamond, an in-depth analysis of recent progress in their fabrication techniques, and a critical discussion of their current applications in quantum science and technology. Additionally, the challenges, open questions, and future research directions in NV color center studies are addressed.
Control over the charge states of color centers in solids is necessary to fully utilize them in quantum technologies. However, the microscopic charge dynamics of deep defects in wide-band-gap semiconductors are complex, and much remains unknown. We utilize a single-shot charge-state readout of an individual nitrogen-vacancy (NV) center to probe the charge dynamics of the surrounding defects in diamond. We show that the NV center charge state can be converted through the capture of holes produced by optical illumination of defects many micrometers away. With this method, we study the optical charge conversion of silicon-vacancy (SiV) centers and provide evidence that the dark state of the SiV center under optical illumination is SiV 2– . These measurements illustrate that charge carrier generation, transport, and capture are important considerations in the design and implementation of quantum devices with color centers and provide a novel way to probe and control charge dynamics in diamond.