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Materials for Quantum Technology

Deterministic laser-writing of nitrogen-vacancy centres in high purity diamond

Andrew R Kirkpatrick, Zhin Mai, Colin J. Stephen, Gareth Siôn Jones, Gavin W. Morley, Martin J. Booth, Patrick S. Salter, Jason M. Smith

Published Nov 5, 2025• 1 citation
Publisher

Abstract

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.

DOI
10.1088/2633-4356/ae1c14

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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.
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.
In this work, we demonstrate two developments, in device and material engineering respectively, towards an efficient spin-photon device using colour centres in diamond for scalable quantum computing networks: firstly, we report the emission enhancement of the coherent zero-phonon-line transistion of an nitrogen vacancy centre in a diamond membrane on coupling to a tunable open-cavity; secondly, we present a new method for deterministic writing of NV arrays in bulk diamond with a 96% yield of single defects, a 50 nm positional accuracy in the image plane, and NV electron spin coherence (T2) times of up to 170 microseconds.
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.
Quantum emitters, such as the negatively charged nitrogen-vacancy center in diamond, are attractive for quantum technologies, such as nano-sensing, quantum information processing, and as a non-classical light source. However, it is still challenging to position individual emitters in photonic structures while preserving the spin coherence properties of the defect. In this paper, we investigate single and ensemble waveguide-integrated nitrogen-vacancy centers in diamond fabricated by femtosecond laser writing followed by thermal annealing. Their spin coherence properties are systematically investigated and are shown to be comparable to native nitrogen-vacancy centers in diamond. This method paves the way for the fabrication of coherent spins integrated within photonic devices.