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Ultrathin boron-doped diamond – surface-wave-plasma synthesis of semi-conductive nanocrystalline boron-doped diamond layers at low temperature

MetadataDetails
Publication Date2025-01-01
JournalMaterials Advances
AuthorsP. Ashcheulov, Davydova M, A Taylor, P. Hubík, A. Kovalenko
InstitutionsFraunhofer Institute for Applied Solid State Physics
AnalysisFull AI Review Included

The research details the successful synthesis and characterization of ultrathin, semi-conductive Boron-Doped Diamond (BDD) layers using a cost-effective, low-temperature Surface-Wave-Plasma (SWP) technique.

  • Low-Temperature Synthesis: BDD layers were fabricated at a substrate temperature of only 500 °C (±20 °C), significantly lower than conventional CVD methods (700-1000 °C), enabling compatibility with a wider range of substrate materials.
  • Ultrathin and Smooth Films: Achieved highly uniform, nanocrystalline BDD layers with thicknesses averaging ~150 nm (range 124-167 nm) and exceptional smoothness (RMS roughness 6-8 nm).
  • Tunable Electrical Properties: Electrical resistivity was systematically controlled by optimizing the gas-phase B/C ratio and CO2 concentration, yielding semi-conductive films tunable across five orders of magnitude (1.85 Ω cm up to 303,500 Ω cm).
  • Gas Chemistry Optimization: Increasing CO2 concentration (0.1% to 2%) was shown to improve diamond quality (higher sp3 content) but simultaneously decreased boron incorporation and increased electrical resistivity.
  • Electrochemical Performance: The resulting Si/BDD electrodes demonstrated a wide electrochemical stability window of ~2.5-3.0 V in aqueous electrolytes, comparable to much thicker microcrystalline BDD electrodes.
  • Cost-Effectiveness: The ultrathin nature supports reduced fabrication time and energy consumption, positioning SWP-synthesized BDD as a viable, cost-efficient alternative to thick microcrystalline films.
ParameterValueUnitContext
Synthesis MethodMW-LA-PECVDN/ASurface-Wave-Plasma (SWP)
Substrate Temperature500 ± 20°CUnassisted configuration
Growth Duration6hoursFixed for all samples
Layer Thickness Range124 - 167nmUltrathin nanocrystalline BDD
Average Growth Rate< 30nm h-1Low rate due to low temperature
RMS Roughness Range6 - 8nmMeasured via AFM
Microwave Power2 x 3kWTotal power input
Process Pressure0.25mbarFixed operating pressure
H2 Concentration94 - 96%Primary carrier gas
CH4 Concentration4%Carbon source
CO2 Concentration Range0.1 - 2%Used for quality and resistivity tuning
B/C Ratio (Gas Phase)60 - 60,000ppmDiborane (B2H6) precursor
Electrical Resistivity Range1.85 - 303,500Ω cmSemi-conductive range
Boron Concentration (Solid)6.07 x 1019 - 7.1 x 1020at. cm-3Assessed via GDOES
Electrochemical Window2.5 - 3.0VMeasured in 1 M KCl electrolyte
Diamond Raman Peak1322 - 1331cm-1Confirms successful sp3 synthesis

The ultrathin nanocrystalline BDD layers were fabricated using a custom-built Microwave Plasma Enhanced CVD reactor with Linear Antenna delivery (MW-LA-PECVD).

  1. Substrate Preparation:
    • Substrates used included high-temperature glass, quartz, and conductive p-type Si (<0.005 Ω cm resistivity).
    • Si substrates underwent HF acid treatment to remove the native SiO2 layer.
    • All substrates were seeded using nanodiamond dispersion (NanoAmando) via spin coating.
  2. Gas Admixture:
    • The primary gas mixture was H2/CH4/B2H6/CO2.
    • H2 (94-96%) and CH4 (4%) were fixed.
    • B/C ratios were varied widely (60, 600, 6000, 60000 ppm) using 7500 ppm B2H6 in H2.
    • CO2 concentration was systematically varied (0.1%, 0.5%, 1%, 1.5%, 2%) to optimize electrical properties and quality.
  3. Deposition Process:
    • The reactor operated at 0.25 mbar pressure and 2 x 3 kW microwave power.
    • Synthesis was performed in an unassisted configuration, achieving a low substrate surface temperature of 500 °C (±20 °C) via plasma heating.
    • All growth cycles were fixed at 6 hours duration.
  4. Characterization Techniques:
    • Thickness/Morphology: Cross-section and top-view Scanning Electron Microscopy (SEM). Image processing was used for statistical grain size distribution analysis.
    • Roughness: Atomic Force Microscopy (AFM) in Peak Force Tapping mode.
    • Quality/Structure: Raman Spectroscopy (488 nm laser) to confirm sp3 diamond bonding and non-diamond content.
    • Boron Concentration: Glow Discharge Optical Emission Spectroscopy (GDOES) depth profiling.
    • Electrical Resistivity: Differential van der Pauw (vdP) method using evaporated Ti/Au contacts.
    • Electrochemistry: Cyclic Voltammetry (CV) using a three-electrode setup (Ag/AgCl reference, Pt counter) in 1 M KCl with Fe(CN)63-/4- redox marker.

The synthesis of ultrathin, semi-conductive BDD layers at low temperatures using SWP MW-LA-PECVD offers significant advantages for applications requiring high chemical stability, optical transparency, and tunable electrical characteristics.

Industry/ApplicationKey Benefit of Ultrathin SWP-BDD
Electrochemistry & SensingWide potential window (~3.0 V) and high stability; tunable semi-conductive properties are beneficial for specific processes (e.g., CO2 reduction, pharmaceutical degradation).
Electro-Optical DevicesUltrathin nature (~150 nm) provides high optical transparency; smooth surface (RMS 6-8 nm) minimizes light scattering.
Flexible ElectronicsReduced thickness enables a certain degree of mechanical flexibility, suitable for integration into soft or portable devices.
Gas SensingHigh chemical stability and tunable electrical characteristics are critical for robust and selective gas sensor fabrication.
Substrate VersatilityLow synthesis temperature (500 °C) allows BDD coating onto temperature-sensitive materials (e.g., certain glasses or metals) that cannot withstand conventional CVD temperatures (800-1100 °C).
Cost-Effective ManufacturingSWP technique is scalable for large areas (wafer-size) and the ultrathin films reduce material usage and fabrication time, lowering overall production costs.
View Original Abstract

Ultrathin boron-doped diamond layers, synthesized at 500 °C, provide a cost-effective, energy-efficient material with moderate semi-conductive properties for advanced functional uses.