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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
InstitutionsHanyang University, Korea University of Science and Technology
Citations9
AnalysisFull AI Review Included

This research details a breakthrough method for engineering solid-state defects (Nitrogen Vacancy, NV centers) in diamond with sub-10 nm precision, crucial for scalable quantum systems.

  • Core Innovation: A double-layered mask system combining Nanoscale Aperture Arrays (NAAs) and Electron Beam Lithography (EBL) is used for highly precise 14N+ ion implantation.
  • Precision Record: The technique achieved the smallest reported single aperture mask opening area (28 nm2) and the closest center-to-center spin separation (approximately 10 nm).
  • NAA Characteristics: The NAAs, derived from phase-separated eutectic Al-Si, exhibit a high aspect ratio (10) and an inherently uniform triangular lattice geometry, ensuring high scalability.
  • Cluster Confinement: The method successfully confined small clusters of up to three NV spins within a 30 nm diameter EBL hole spot, verified by g(2) and ODMR measurements.
  • Coupling Potential: The close proximity (~10 nm) achieved suggests the potential for strong NV-NV dipolar coupling, a prerequisite for realizing scalable quantum registers.
  • Scalability: The NAA-EBL double-layer mask is robust for fabricating a large number of uniform, closely separated quantum nodes in a wide area.
ParameterValueUnitContext
NV Positioning Precision (Area)28nm2Smallest single aperture mask opening area achieved.
Aperture Size (da)5.87 ± 0.82nmMean aperture size of optimized NAAs.
Aperture-to-Aperture Distance10.7nmCenter-to-center separation of NAAs.
NAA Aspect Ratio10RatioHigh aspect ratio achieved via Al-Si phase separation.
NAA Mask Thickness55nmSufficient to block 10 keV ions.
EBL Secondary Mask Diameter~30 (Measured 32.23)nmConfining cluster size (Sample A).
Ion Species14N+IonImplanted nitrogen source.
Implantation Energy10keVStandard energy used for all samples.
Implantation Dose4 x 1013ions/cm2Total dose applied.
SRIM Projected Range (10 keV)30.1nmCalculated projected range of 14N+ ions.
Single NV Coherence Time (T2,Hahn)4.5”sAverage measured T2,Hahn for single NVs.
Maximum Single NV T2,Hahn>16”s10% of measured single NVs exceeded this value.
Strong Coupling Separation Target~10nmRequired separation for strong NV-NV dipolar coupling.
Confined NV CountUp to 3NVsConfirmed within a single 30 nm EBL spot.

The fabrication relies on a phase-separation technique combined with standard lithography and ion implantation:

  1. Diamond Cleaning: High-purity diamond substrate cleaned by tri-acid boiling (sulfuric, perchloric, nitric acid) for >1 h at 170 °C.
  2. Al-Si Thin Film Deposition: A 55 nm thick eutectic Al-Si phase-separated thin film deposited via RF sputtering (Ar pressure 0.3 mTorr, substrate temperature 100 °C, RF power 150W).
  3. NAA Formation (Selective Etching): Aluminum nanowires selectively etched by immersion in 5% phosphoric acid, leaving the NAA layer composed of amorphous silicon oxide with a mean aperture size of 5.87 nm.
  4. Secondary Mask Patterning: A secondary EBL mask (ZEP520a) with circular holes (~30 nm diameter, 200 nm thickness) applied onto the NAAs to define implantation spots.
  5. Ion Implantation: 14N+ ions implanted through the NAA-EBL double-layer mask at 10 keV with a dose of 4 x 1013/cm2.
  6. NV Generation (Annealing): Samples annealed sequentially at 800 °C for 8 h and 1100 °C for 2 h to generate NV centers.
  7. Surface Treatment: Additional O2 annealing performed at 450 °C for 4 h to induce oxygen termination, improving the spin coherence time of shallow NV centers.
  8. Measurement: Optical and spin properties verified using home-built confocal microscopy, second-order autocorrelation function (g(2)), and Optically Detected Magnetic Resonance (ODMR).

This high-precision defect engineering technique is foundational for developing next-generation quantum technologies:

  • Scalable Quantum Computing: Enables the fabrication of uniform, strongly coupled quasi-2D spin clusters, essential for constructing scalable solid-state qubit registers and quantum processors.
  • High-Resolution Quantum Sensing: Facilitates the creation of dense, uniform arrays of NV spin sensors, significantly improving the spatial resolution and sensitivity of magnetic field imaging and other quantum sensing applications.
  • Quantum Simulation Platforms: Provides a robust method for engineering strongly interacting electronic spin ensembles, serving as ideal platforms for studying complex quantum phenomena and many-body physics.
  • Advanced Qubit Manufacturing: Offers a highly robust and scalable tool for deterministic positioning of solid-state defects, overcoming yield and uniformity challenges associated with previous nanoimplantation methods (e.g., AFM tip or single-layer EBL masks).
  • Shallow NV Enhancement: The technique, when combined with post-processing methods like epitaxial overgrowth or microwave-assisted chemical vapor deposition (CVD), can lead to shallow NV centers with enhanced spin properties and longer coherence times.
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.