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Sub-10 nm Precision Engineering of Solid-State Defects via Nanoscale Aperture Array Mask

MetadataDetails
Publication Date2022-02-08
JournalNano Letters
AuthorsTae-Yeon Hwang, Jung‐Hyun Lee, Seung-Woo Jeon, Yong‐Su Kim, Young‐Wook Cho
InstitutionsKorea University of Science and Technology, Korea Institute of Science and Technology
Citations9
AnalysisFull AI Review Included

Technical Documentation & Analysis: Precision NV Center Engineering

Section titled “Technical Documentation & Analysis: Precision NV Center Engineering”

This research demonstrates a breakthrough in the deterministic positioning of Nitrogen Vacancy (NV) centers in diamond, a critical step toward scalable solid-state quantum systems.

  • Precision Achievement: Sub-10 nm precision engineering of NV centers using a novel Nanoscale Aperture Array (NAA) mask combined with Electron Beam Lithography (EBL).
  • Record Mask Dimensions: Achieved the smallest reported single aperture mask opening area (28 nmÂČ) and the closest center-to-center width (~10 nm) for ion implantation.
  • Material Foundation: Utilized high-purity Single Crystal Diamond (SCD) substrates ([N] < 5 ppb, [B] < 1 ppb) to minimize intrinsic defects.
  • Qubit Confinement: Successfully confined clusters of up to three NV spins within a 30 nm diameter EBL hole spot, verified by g(2) and ODMR measurements.
  • Strong Coupling Potential: The 10 nm separation distance is suitable for realizing strong spin-spin magnetic dipolar coupling on timescales shorter than the spin coherence time (T2,Hahn).
  • Future MPCVD Requirement: The study identifies the need for subsequent diamond layer re-growth via Microwave Plasma Chemical Vapor Deposition (MPCVD) to eliminate surface defects and enhance the spin coherence time (T2,Hahn), a core 6CCVD capability.
ParameterValueUnitContext
Diamond Purity (Nitrogen)< 5ppbSubstrate intrinsic concentration
Diamond Purity (Boron)< 1ppbSubstrate intrinsic concentration
NAA Aperture Size (da)5.87 ± 0.82nmOptimized mean aperture diameter
Aperture-to-Aperture Distance10.7nmCenter-to-center separation
NAA Aspect Ratio10N/ARatio of thickness to aperture size
NAA Thickness55nmAl-Si thin film thickness
EBL Secondary Mask Diameter~30nmCircular hole pattern used for confinement
Ion Implantation Species14N+N/ANitrogen ions
Ion Implantation Energy10keVUsed for all samples
Ion Implantation Dose4 x 1013/cmÂČTarget dose
Projected Range (SRIM)30.1nmPenetration depth of 10 keV ions
Longitudinal Straggle (SRIM)15.3nmDepth variation
Smallest Mask Opening Area28nmÂČAchieved in this work (Table 1)
Achieved NV-NV Coupling Distance~10nmModerate coupling regime
Average Single NV T2,Hahn4.5”sLimited by shallow implantation/surface noise
Target T2,Hahn for Strong Coupling~20”sRequired for 10 nm separation
High-Temperature Annealing 1800°C8 hours (NV generation)
High-Temperature Annealing 21100°C2 hours (NV generation)
Surface Annealing450°C4 hours (O2 termination for T2,Hahn improvement)

The deterministic placement of NV centers relied on a multi-step nanofabrication process using high-purity SCD:

  1. Diamond Cleaning: Substrates were cleaned via tri-acid boiling (sulfuric, perchloric, nitric acid) for >1 hour at 170 °C.
  2. Al-Si Thin Film Deposition: A 55 nm thick, phase-separated eutectic Al-Si thin film was deposited directly onto the diamond surface using RF sputtering.
    • Parameters: Ar working pressure 0.3 mTorr, substrate temperature 100 °C, RF power 150W, deposition rate 15.8 nm/min.
  3. NAA Formation: Selective etching of Al nanowires was performed by immersing the samples in 5% phosphoric acid overnight, leaving the NAAs layer composed of amorphous silicon oxide.
  4. Secondary Masking (EBL): A secondary EBL mask (ZEP520a, ~200 nm thick) with circular hole patterns (~30 nm diameter) was applied to isolate small clusters of NAAs.
  5. Nitrogen Ion Implantation: 14N+ ions were implanted at 10 keV energy and a dose of 4 x 1013/cmÂČ through the double-layered NAA/EBL mask.
  6. NV Generation Annealing: Samples were annealed sequentially at 800 °C (8h) and 1100 °C (2h).
  7. Surface Termination: An additional O2 annealing process was performed at 450 °C (4h) to induce oxygen termination for improved shallow NV spin coherence.
  8. Characterization: Optical (PL, g(2)) and spin (ODMR, Hahn-echo T2,Hahn) measurements were performed using a home-built confocal microscope at room temperature.

This research highlights the critical need for ultra-high purity diamond and advanced surface engineering techniques, both of which are core competencies of 6CCVD. Our MPCVD capabilities are essential for replicating and extending this work toward truly scalable quantum systems.

Research Requirement6CCVD SolutionMaterial Specification
High-Purity SubstrateOptical Grade SCDUltra-low [N] (< 5 ppb) and [B] (< 1 ppb) for minimal background noise and long intrinsic coherence times.
Scalability & UniformityLarge Format SCD PlatesCustom dimensions up to 125mm (PCD equivalent) and large SCD plates, enabling high-throughput fabrication of quantum nodes.
T2,Hahn ImprovementHigh-Quality SCD OvergrowthMPCVD epitaxial re-growth (0.1 ”m to 500 ”m thickness) to bury shallow NV centers, eliminating surface-related noise and achieving target T2,Hahn (> 20 ”s).
Masking/Etching CompatibilityCustom Thickness SubstratesSCD substrates up to 10mm thick, polished to Ra < 1 nm, ensuring optimal surface quality for subsequent nanofabrication steps (sputtering, EBL, etching).

The NAA-EBL double-layer mask technique requires precise control over thin film deposition and subsequent processing. 6CCVD offers comprehensive support for these advanced requirements:

  • Custom Thickness Control: We provide SCD wafers with thickness control from 0.1 ”m to 500 ”m, allowing researchers to precisely tune the depth of the implanted NV layer relative to the surface noise, a key factor in T2,Hahn optimization.
  • Integrated Metalization Services: While this paper focused on Al-Si masks, future quantum device architectures often require integrated microwave delivery structures (e.g., coplanar waveguides). 6CCVD offers in-house metalization capabilities including Au, Pt, Pd, Ti, W, and Cu deposition, crucial for delivering microwave signals for ODMR and spin manipulation.
  • Advanced Polishing: The success of thin film deposition (like the 55 nm Al-Si layer) relies on an atomically smooth surface. 6CCVD guarantees SCD polishing to Ra < 1 nm, ensuring uniform mask adhesion and high-fidelity pattern transfer.

The low average T2,Hahn (4.5 ”s) observed in this study is a common challenge for shallow NV implantation. The paper correctly identifies MPCVD diamond re-growth as the solution to eliminate surface defect noise and increase coherence time (p. 13).

6CCVD’s in-house PhD team specializes in optimizing MPCVD recipes for quantum applications. We can assist researchers in designing the optimal epitaxial overgrowth layer (thickness, purity, growth rate) required for similar Scalable Qubit System projects, ensuring the buried NV centers achieve the target coherence time of 20 ”s or greater necessary for strong dipolar coupling.

For custom specifications or material consultation, visit 6ccvd.com or contact our engineering team directly.

View Original Abstract

Engineering a strongly interacting uniform qubit cluster would be a major step toward realizing a scalable quantum system for quantum sensing and a node-based qubit register. For a solid-state system that uses a defect as a qubit, various methods to precisely position defects have been developed, yet the large-scale fabrication of qubits within the strong coupling regime at room temperature continues to be a challenge. In this work, we generate nitrogen vacancy (NV) color centers in diamond with sub-10 nm scale precision using a combination of nanoscale aperture arrays (NAAs) with a high aspect ratio of 10 and a secondary E-beam hole pattern used as an ion-blocking mask. We perform optical and spin measurements on a cluster of NV spins and statistically investigate the effect of the NAAs during an ion-implantation process. We discuss how this technique is effective for constructing a scalable system.