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physica status solidi (a)

Charge‐Assisted Engineering of Color Centers in Diamond

Tobias Lühmann, Jan Meijer, Sébastien Pezzagna

Published Jan 15, 2021• 32 citations
Publisher

Abstract

Owing to its unique optical and spin properties, the nitrogen‐vacancy (NV) center holds the promise of a diamond‐based room‐temperature scalable quantum computer, but the numerous technical and physical issues are not yet overcome, especially the poor N to NV conversion. The NV and other color centers are, however, successfully used as multitasking quantum sensors, and open new routes in quantum sensing technologies. Most recently, several breakthroughs and demonstrations were achieved, shedding a new light on the feasibility of a NV‐based quantum computer. Herein, the recently developed method of charge‐assisted single defect engineering is reviewed. With a controlled charging of the involved species, it modifies the diffusion or kinetics of defect formation and acts as a catalyzer of the NV creation while hindering the formation of competing and perturbing defects such as divacancies or NVH. Very high NV creation yields up to 75% are obtained and the method is suitable to other impurity‐vacancy defects. Furthermore, it has positive consequences on the charge state stability and coherence time of the NV centers, which is as well discussed. Together with the possibility to nowadays deterministically implant single ions, this powerful method brings the scalability of NV qubits closer.

DOI
10.1002/pssa.202000614

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Coulomb-driven single defect engineering for scalable qubits and spin sensors in diamond

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Abstract Qubits based on colour centres in diamond became a prominent system for solid-state quantum information processing and sensing. But the deterministic creation of qubits and the control of their environment are still critical issues, preventing the development of a room-temperature quantum computer. We report on the high creation yield of NV centres of 75% (a tenfold enhancement) by charge-assisted defect engineering, together with an improvement of their spin coherence. The method strongly favours the formation and negative charge state of the NV centres with respect to intrinsic diamond, while it hinders the formation of competing and perturbing defects such as di-vacancies or NVH complexes. We evidence spectrally the charge state tuning of the implantation-induced vacancies from V0 to V−, key element of this Coulomb-driven engineering. The generality of the method is demonstrated using several donors (phosphorous, oxygen and sulphur) and applying it to other centres (SnV and MgV) in diamond.

Nature Communications•Oct 31, 2019•130 citations

Charge‐Assisted Engineering of Color Centers in Diamond

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Charge-Assisted Engineering The recently developed method of charge-assisted single defect engineering brings the full scalability of solid-state qubits or quantum sensors closer. Applied to colour centres in diamond (NV, SnV, MgV,…), it enables a strong enhancement of their creation yield and of their properties such as charge-state stability or spin coherence times. More details can be found in article number 2000614 by Sébastien Pezzagna and co-workers.

physica status solidi (a)•Mar 1, 2021•5 citations

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Silicon has turned from a niche laboratory-scale material into the backbone of modern electronics. Diamond functionalized with color centers could follow a similar path and grow from proof-of-concepts experiments to application-oriented quantum technologies. Quantum sensing, communication, and information processing with color centers has been proven to work in scientific experiments and enhanced sensitivities as well as novel functionalities have been reported. While the first generation of diamond quantum devices relied on color centers formed uncontrolled in natural diamond with a high statistical variation in composition and crystallinity, the situation has changed nowadays. With the emergence of high purity monocrystals and the option for isotopic purification of the carbon matrix, technological progress in materials science on the atomic-scale enabled tailoring the spin properties in diamond. But, since many color centers typically require vacancies to combine with impurities in the carbon lattice via diffusion, the generation of color centers underlies a statistical process providing only little control on the center's final position in the crystal lattice. The negatively charged nitrogen-vacancy (NV$^-$) center is the most studied optically active defect in diamond and exhibits remarkable spin properties and sensing capabilities, even on the nanoscale and at room temperature. The spin properties of NV$^-$ centers close to the surface (1\,nm - 30\,nm) have been thoroughly studied and the deeper the spins are located in diamond the less decoherence from surface defects is observed. Creating NV$^-$ centers at the surface by nitrogen ion implantation and burying them beneath a thin diamond layer via chemical vapor deposition (CVD) of diamond is reported to enhance the coherence times significantly. By separating the color center generation from controlling the resulting depth by an additional diamond layer, narrow depth profiles can be achieved by reducing the ion energy during implantation. Although the coherence properties improve, many of the implanted NV$^-$ center are reported to vanish in the hydrogen-rich plasma of growth CVD chambers. The mechanism responsible for the instability of NV$^-$ centers towards the plasma remains unclear, though. One hypothesis is the formation of nitrogen-vacancy-hydrogen centers from diffusing hydrogen and implanted NV$^-$ centers but is has not been proven, yet. Here, we demonstrate the fabrication of depth confined NV$^-$ centers by combining low energy (1\,keV - 5\,keV) ion implantation and CVD overgrowth. By increasing the thickness of the overgrown layer (6\,nm - 100\,nm) the influence of surface noise is shown to decrease leading to bulk-like coherence properties of up to $450\,\upmu$s (Hahn-echo) and $T_2^*$ dephasing times around $20\,\upmu$s. Monitoring the NV$^-$ density as a function of the overgrowth time, we analyze the kinetics of the passivation in case of implanting ion doses of 10$^{11}$ $^{15}$N $^{+}$/cm$^2$ and 10$^{12}$ $^{15}$N $^{+}$/cm$^2$. The passivation turns out to occur faster for lower doses offering insights into sub-surface hydrogen diffusion in diamond. Analyzing the spin bath before and after overgrowth reveals a drastic reduction in paramagnetic spins after the CVD process but no NVH$^-$ is found around the surviving NV$^-$ centers. Checking the chemical composition in overgrown implantation sites with secondary-ion-mass-specrometry (SIMS), however, confirms significant amounts of hydrogen in the $^{15}$N-implanted layers. Since the concentration found for hydrogen exceeds the one for nitrogen by far, we suggest that diffusing hydrogen interacts also with vacancies forming probably mostly diamagnetic defects. In the last part of this dissertation, NV$^-$ centers are generated with sub-nanometer precision below a thin $^{13}$C-enriched layer for quantum simulation. For fabricating the spin architecture starting from a $^{12}$C base layer, we overgrow implanted nitrogen with a $^{13}$C layer and bury the spins beneath a 30\,nm-thick $^{12}$C capping layer. By measuring the coupling strength between the electron and nuclear spins, we deduce a NV$^-$ placement accuracy reaching below one nanometer with respect to the $^{13}$C-layer. Regarding the spin properties of the electron spins, no reduction in $T_2$ is observed despite of the proximity to the dense $^{13}$C-bath. As a consequence, the overgrowth of NV$^-$ centers is demonstrated as a bottom-up approach to produce buried spin architectures with sharp isotopic transitions and efficient $^{13}$C-NV$^-$ coupling. Together with the potential for bulk-like coherence properties the synergy of implantation and overgrowth is a powerful tool to fabricate reproducible quantum systems with tailored properties and high depth confinement.

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Recent progress in hybrid diamond photonics for quantum information processing and sensing

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Point defects in diamond, particularly nitrogen-vacancy (NV) centers, have emerged as powerful tools for a broad range of quantum technologies. These defects are promising candidates for quantum information science, serving as deterministic single-photon sources and solid-state quantum memories. They have also been employed as nanoscale quantum sensors to detect various physical quantities, including magnetic fields, electric fields, and temperature, owing to their long spin coherence time at room temperature. Development of these diamond-based quantum technologies has been rapidly boosted by a recent quantum leap in nanofabrication technologies for high-quality single-crystal diamond. Incorporating these color centers into diamond nanostructures with mature integrated photonics provides a promising route to build scalable and practical systems for quantum applications. This review discusses recent progress and challenges in the hybrid integration of diamond color centers on cutting-edge photonic platforms. Nitrogen-vacancy centers in diamond have emerged as powerful tools for a broad range of quantum technologies. This review discusses recent progress and challenges in the hybrid integration of diamond color centers on cutting-edge photonic platforms.

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Abstract Negatively charged nitrogen‐vacancy (NV − ) centers in diamond are appealing for quantum sensing applications due to their environmental sensitivity and long coherence times. Precise and scalable shallow color center creation is essential yet challenging for technological quantum applications. This is due to the involvement of several lengthy processes, such as ion implantation and thermal annealing of the samples. The latter process can be addressed by application of an alternative activation technique that bypasses the high‐temperature annealing. For this, nitrogen‐implanted regions on a diamond substrate are exposed to continuous‐wave 405 nm laser radiation. The illumination leads to local activation of NV − centers with photoluminescence yield saturation for regions activated with laser power at around 800 µW. For low implantation doses, single NV − centers are created with corresponding mean T 2 coherence time value around 71 µs. The NV − creation yield for the lower implantation doses match conventional creation methods, while higher doses show reduced yield values. However, the coherent properties are comparable to NV − centers within annealed samples. This shows that the activated NV − centers are well‐suited for advanced applications in quantum sensing and related technologies.

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Onoda Shinobu

A nitrogen vacancy (NV) center, which is a luminescent point defect based on substitutional nitrogen and neighbouring vacancy, is the most studied color centers in diamond. NV center is known as a solidstate spin quantum bit (qubit) at room temperature. NV-qubit is widely utilized for quantum sensors and quantum information processing, etc. In this talk, the recent progress of color center fabrication by electron irradiation and ion implantation will be discussed.

•Sep 4, 2023•0 citations
Owing to its unique optical and spin properties, the nitrogen‐vacancy (NV) center holds the promise of a diamond‐based room‐temperature scalable quantum computer, but the numerous technical and physical issues are not yet overcome, especially the poor N to NV conversion. The NV and other color centers are, however, successfully used as multitasking quantum sensors, and open new routes in quantum sensing technologies. Most recently, several breakthroughs and demonstrations were achieved, shedding a new light on the feasibility of a NV‐based quantum computer. Herein, the recently developed method of charge‐assisted single defect engineering is reviewed. With a controlled charging of the involved species, it modifies the diffusion or kinetics of defect formation and acts as a catalyzer of the NV creation while hindering the formation of competing and perturbing defects such as divacancies or NVH. Very high NV creation yields up to 75% are obtained and the method is suitable to other impurity‐vacancy defects. Furthermore, it has positive consequences on the charge state stability and coherence time of the NV centers, which is as well discussed. Together with the possibility to nowadays deterministically implant single ions, this powerful method brings the scalability of NV qubits closer.
Abstract Qubits based on colour centres in diamond became a prominent system for solid-state quantum information processing and sensing. But the deterministic creation of qubits and the control of their environment are still critical issues, preventing the development of a room-temperature quantum computer. We report on the high creation yield of NV centres of 75% (a tenfold enhancement) by charge-assisted defect engineering, together with an improvement of their spin coherence. The method strongly favours the formation and negative charge state of the NV centres with respect to intrinsic diamond, while it hinders the formation of competing and perturbing defects such as di-vacancies or NVH complexes. We evidence spectrally the charge state tuning of the implantation-induced vacancies from V0 to V−, key element of this Coulomb-driven engineering. The generality of the method is demonstrated using several donors (phosphorous, oxygen and sulphur) and applying it to other centres (SnV and MgV) in diamond.
Silicon has turned from a niche laboratory-scale material into the backbone of modern electronics. Diamond functionalized with color centers could follow a similar path and grow from proof-of-concepts experiments to application-oriented quantum technologies. Quantum sensing, communication, and information processing with color centers has been proven to work in scientific experiments and enhanced sensitivities as well as novel functionalities have been reported. While the first generation of diamond quantum devices relied on color centers formed uncontrolled in natural diamond with a high statistical variation in composition and crystallinity, the situation has changed nowadays. With the emergence of high purity monocrystals and the option for isotopic purification of the carbon matrix, technological progress in materials science on the atomic-scale enabled tailoring the spin properties in diamond. But, since many color centers typically require vacancies to combine with impurities in the carbon lattice via diffusion, the generation of color centers underlies a statistical process providing only little control on the center's final position in the crystal lattice. The negatively charged nitrogen-vacancy (NV−^-−) center is the most studied optically active defect in diamond and exhibits remarkable spin properties and sensing capabilities, even on the nanoscale and at room temperature. The spin properties of NV−^-− centers close to the surface (1\,nm - 30\,nm) have been thoroughly studied and the deeper the spins are located in diamond the less decoherence from surface defects is observed. Creating NV−^-− centers at the surface by nitrogen ion implantation and burying them beneath a thin diamond layer via chemical vapor deposition (CVD) of diamond is reported to enhance the coherence times significantly. By separating the color center generation from controlling the resulting depth by an additional diamond layer, narrow depth profiles can be achieved by reducing the ion energy during implantation. Although the coherence properties improve, many of the implanted NV−^-− center are reported to vanish in the hydrogen-rich plasma of growth CVD chambers. The mechanism responsible for the instability of NV−^-− centers towards the plasma remains unclear, though. One hypothesis is the formation of nitrogen-vacancy-hydrogen centers from diffusing hydrogen and implanted NV−^-− centers but is has not been proven, yet. Here, we demonstrate the fabrication of depth confined NV−^-− centers by combining low energy (1\,keV - 5\,keV) ion implantation and CVD overgrowth. By increasing the thickness of the overgrown layer (6\,nm - 100\,nm) the influence of surface noise is shown to decrease leading to bulk-like coherence properties of up to $450\,\upmu$s (Hahn-echo) and T2∗T_2^*T2∗​ dephasing times around $20\,\upmu$s. Monitoring the NV−^-− density as a function of the overgrowth time, we analyze the kinetics of the passivation in case of implanting ion doses of 1011^{11}11 15^{15}15N +^{+}+/cm2^22 and 1012^{12}12 15^{15}15N +^{+}+/cm2^22. The passivation turns out to occur faster for lower doses offering insights into sub-surface hydrogen diffusion in diamond. Analyzing the spin bath before and after overgrowth reveals a drastic reduction in paramagnetic spins after the CVD process but no NVH−^-− is found around the surviving NV−^-− centers. Checking the chemical composition in overgrown implantation sites with secondary-ion-mass-specrometry (SIMS), however, confirms significant amounts of hydrogen in the 15^{15}15N-implanted layers. Since the concentration found for hydrogen exceeds the one for nitrogen by far, we suggest that diffusing hydrogen interacts also with vacancies forming probably mostly diamagnetic defects. In the last part of this dissertation, NV−^-− centers are generated with sub-nanometer precision below a thin 13^{13}13C-enriched layer for quantum simulation. For fabricating the spin architecture starting from a 12^{12}12C base layer, we overgrow implanted nitrogen with a 13^{13}13C layer and bury the spins beneath a 30\,nm-thick 12^{12}12C capping layer. By measuring the coupling strength between the electron and nuclear spins, we deduce a NV−^-− placement accuracy reaching below one nanometer with respect to the 13^{13}13C-layer. Regarding the spin properties of the electron spins, no reduction in T2T_2T2​ is observed despite of the proximity to the dense 13^{13}13C-bath. As a consequence, the overgrowth of NV−^-− centers is demonstrated as a bottom-up approach to produce buried spin architectures with sharp isotopic transitions and efficient 13^{13}13C-NV−^-− coupling. Together with the potential for bulk-like coherence properties the synergy of implantation and overgrowth is a powerful tool to fabricate reproducible quantum systems with tailored properties and high depth confinement.
Point defects in diamond, particularly nitrogen-vacancy (NV) centers, have emerged as powerful tools for a broad range of quantum technologies. These defects are promising candidates for quantum information science, serving as deterministic single-photon sources and solid-state quantum memories. They have also been employed as nanoscale quantum sensors to detect various physical quantities, including magnetic fields, electric fields, and temperature, owing to their long spin coherence time at room temperature. Development of these diamond-based quantum technologies has been rapidly boosted by a recent quantum leap in nanofabrication technologies for high-quality single-crystal diamond. Incorporating these color centers into diamond nanostructures with mature integrated photonics provides a promising route to build scalable and practical systems for quantum applications. This review discusses recent progress and challenges in the hybrid integration of diamond color centers on cutting-edge photonic platforms. Nitrogen-vacancy centers in diamond have emerged as powerful tools for a broad range of quantum technologies. This review discusses recent progress and challenges in the hybrid integration of diamond color centers on cutting-edge photonic platforms.
Abstract Negatively charged nitrogen‐vacancy (NV − ) centers in diamond are appealing for quantum sensing applications due to their environmental sensitivity and long coherence times. Precise and scalable shallow color center creation is essential yet challenging for technological quantum applications. This is due to the involvement of several lengthy processes, such as ion implantation and thermal annealing of the samples. The latter process can be addressed by application of an alternative activation technique that bypasses the high‐temperature annealing. For this, nitrogen‐implanted regions on a diamond substrate are exposed to continuous‐wave 405 nm laser radiation. The illumination leads to local activation of NV − centers with photoluminescence yield saturation for regions activated with laser power at around 800 µW. For low implantation doses, single NV − centers are created with corresponding mean T 2 coherence time value around 71 µs. The NV − creation yield for the lower implantation doses match conventional creation methods, while higher doses show reduced yield values. However, the coherent properties are comparable to NV − centers within annealed samples. This shows that the activated NV − centers are well‐suited for advanced applications in quantum sensing and related technologies.