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Applied Physics Letters

Enhancing the spin properties of shallow implanted nitrogen vacancy centers in diamond by epitaxial overgrowth

T. Staudacher, Florestan Ziem, Lutz Häussler, Rainer Stöhr, S. Steinert, Friedemann Reinhard, Jochen Scharpf, A. Denisenko, Jörg Wrachtrup

Published Nov 19, 2012• 59 citations
Publisher

Abstract

Scaling of diamond defect center based quantum registers relies on the ability to position nitrogen vacancy (NV) centers with high spatial resolution. Using ion implantation, shallow (<10 nm) NVs can be placed with accuracy below 20 nm, but generally show reduced spin properties compared to bulk NVs. We demonstrate the enhancement of spin properties for shallow implanted NVs using a diamond overgrowth technique. An increase of coherence times up to an order of magnitude (T2 = 250 μs) was achieved, ms decoherence times were realized using dynamical decoupling. This marks a further step towards achieving strong coupling among defects positioned with nm precision.

DOI
10.1063/1.4767144

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The negatively charged nitrogen-vacancy ([Formula: see text]) center shows excellent spin properties and sensing capabilities on the nanoscale even at room temperature. Shallow implanted [Formula: see text] centers can effectively be protected from surface noise by chemical vapor deposition (CVD) diamond overgrowth, i.e. burying them homogeneously deeper in the crystal. However, the origin of the substantial losses in [Formula: see text] centers after overgrowth remains an open question. Here, we use shallow [Formula: see text] centers to exclude surface etching and identify the passivation reaction of NV to NVH centers during the growth as the most likely reason. Indirect overgrowth featuring low energy (2.5-5 keV) nitrogen ion implantation and CVD diamond growth before the essential annealing step reduces this passivation phenomenon significantly. Furthermore, we find higher nitrogen doses to slow down the NV-NVH conversion kinetics, which gives insight into the sub-surface diffusion of hydrogen in diamond during growth. Finally, nano sensors fabricated by indirect overgrowth combine tremendously enhanced [Formula: see text] and [Formula: see text] times with an outstanding degree of depth-confinement which is not possible by implanting with higher energies alone. Our results improve the understanding of CVD diamond overgrowth and pave the way towards reliable and advanced engineering of shallow [Formula: see text] centers for future quantum sensing devices.

Scientific Reports•Dec 29, 2020•20 citations
Scaling of diamond defect center based quantum registers relies on the ability to position nitrogen vacancy (NV) centers with high spatial resolution. Using ion implantation, shallow (<10 nm) NVs can be placed with accuracy below 20 nm, but generally show reduced spin properties compared to bulk NVs. We demonstrate the enhancement of spin properties for shallow implanted NVs using a diamond overgrowth technique. An increase of coherence times up to an order of magnitude (T2 = 250 μs) was achieved, ms decoherence times were realized using dynamical decoupling. This marks a further step towards achieving strong coupling among defects positioned with nm precision.
The controlled scaling of diamond defect center based quantum registers relies on the ability to position NVs with high spatial resolution. Using ion implantation, shallow (< 10 nm) NVs can be placed with accuracy below 20nm, but generally show reduced spin properties compared to bulk NVs. We demonstrate the augmentation of spin properties for shallow implanted NV centers using an overgrowth technique. An increase of the coherence times up to an order of magnitude (T_2 = 250 μs) was achieved. Dynamic decoupling of defects spins achieves ms decoherence times. The study marks a further step towards achieving strong coupling among defects positioned with nm precision.
Efficient creation of shallow NV−^-− ensembles by high-angle ion implantation
Negatively charged nitrogen-vacancy (NV−^-−) centers located a few nanometers below the diamond surface are key quantum defects for nanoscale sensing of external spins. However, the creation of shallow NV−^-− centers with high yield remains a materials challenge. Here, we demonstrate that high-angle ion implantation enhances the creation efficiency of shallow NV−^-− centers. By implanting 15^{15}15N ions at angles exceeding 60∘^\circ∘, we achieve high NV−^-− yields approaching 10% with effective NV−^-− depths below 10 nm. These yields are significantly higher than those typically reported for shallow NV−^-− creation. The enhanced NV−^-− yield is consistent with an increased vacancy-to-nitrogen ratio in the near-surface region, which is expected to promote NV formation during annealing. The created NV−^-− ensembles show coherence properties comparable to those of single shallow NV−^-− centers at similar depths, and allow detection of nuclear spins in van der Waals materials attached to the diamond surface. Our results establish geometric control of ion implantation as a simple and broadly applicable approach to engineer shallow vacancy-related quantum defects.
The nanometer‐scale engineering of single nitrogen‐vacancy (NV) centres in diamond can be obtained by low‐energy (keV) nitrogen implantation with limited straggling. However, shallow NV centres (a few nanometres deep) generally have inferior overall properties than deeply implanted or deep native NV centres, due to the surface proximity. It has already been shown that the spin coherence time of shallow NVs is improved by overgrowth of a thin diamond layer. However the influence of the overgrowth on the survival, the optical properties and the charge state of the centres has not been studied in detail. In this article, we have overgrown three diamond samples (containing NV centres implanted at different depths) using different procedures. We show the successful overgrowth of a pattern of very shallow (2 nm) implanted NV centres using an optimised overgrowth process. Furthermore, the charge state of ensembles and single NV centres was found to be shifted from NV0 to NV− and stabilised in the negative charge state after overgrowth. The combination of low‐energy high‐resolution ion implantation and high‐purity chemical vapour deposition (CVD) overgrowth procedures opens the way towards the fabrication of scalable and efficient quantum devices based on single defects in diamond. Left: implanted pattern of very shallow NV centres (depth ∼2 nm) using a pierced AFM tip. Right: same pattern after CVD overgrowth of a 4 μm‐thick diamond layer.
We demonstrate three-dimensional localization of a single nitrogen-vacancy (NV) center in diamond by combining nitrogen doping during growth with a post-growth 12C implantation technique that facilitates vacancy formation in the crystal. We show that the NV density can be controlled by the implantation dose without necessitating increase of the nitrogen incorporation. By implanting a large 12C dose through nanoscale apertures, we can localize an individual NV center within a volume of (∼180 nm)3 at a deterministic position while repeatedly preserving a coherence time (T2) > 300 μs. This deterministic position control of coherent NV centers enables integration into NV-based nanostructures to realize scalable spin-sensing devices as well as coherent spin coupling mediated by photons and phonons.
Engineering shallow nitrogen-vacancy (NV) centers in diamond holds the key to unlocking new advances in nanoscale quantum sensing. We find that the creation of near-surface NVs through delta doping during diamond growth allows for tunable control over both NV depth confinement (with a twofold improvement relative to low-energy ion implantation) and NV density, ultimately resulting in highly-sensitive single defects and ensembles with coherence limited by NV-NV interactions. Additionally, we demonstrate the utility of our shallow delta-doped NVs by imaging magnetism in few-layer CrSBr, a two-dimensional magnet. We anticipate that the control afforded by near-surface delta doping will enable new developments in NV quantum sensing from nanoscale NMR to entanglement-enhanced metrology.
The negatively charged nitrogen-vacancy ([Formula: see text]) center shows excellent spin properties and sensing capabilities on the nanoscale even at room temperature. Shallow implanted [Formula: see text] centers can effectively be protected from surface noise by chemical vapor deposition (CVD) diamond overgrowth, i.e. burying them homogeneously deeper in the crystal. However, the origin of the substantial losses in [Formula: see text] centers after overgrowth remains an open question. Here, we use shallow [Formula: see text] centers to exclude surface etching and identify the passivation reaction of NV to NVH centers during the growth as the most likely reason. Indirect overgrowth featuring low energy (2.5-5 keV) nitrogen ion implantation and CVD diamond growth before the essential annealing step reduces this passivation phenomenon significantly. Furthermore, we find higher nitrogen doses to slow down the NV-NVH conversion kinetics, which gives insight into the sub-surface diffusion of hydrogen in diamond during growth. Finally, nano sensors fabricated by indirect overgrowth combine tremendously enhanced [Formula: see text] and [Formula: see text] times with an outstanding degree of depth-confinement which is not possible by implanting with higher energies alone. Our results improve the understanding of CVD diamond overgrowth and pave the way towards reliable and advanced engineering of shallow [Formula: see text] centers for future quantum sensing devices.