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Electrical transport measurements for superconducting sulfur hydrides using boron-doped diamond electrodes on beveled diamond anvil

MetadataDetails
Publication Date2020-10-02
JournalSuperconductor Science and Technology
AuthorsRyo Matsumoto, Mari Einaga, Shintaro Adachi, Sayaka Yamamoto, Tetsuo Irifune
InstitutionsEhime University, Osaka University
Citations12
AnalysisFull AI Review Included

This research details the successful fabrication and application of a novel Diamond Anvil Cell (DAC) designed for stable, in-situ electrical transport measurements of high-pressure materials, specifically superconducting sulfur hydrides.

  • Core Innovation: Boron-Doped Diamond (BDD) micro-electrodes and an Undoped Diamond (UDD) insulating layer were epitaxially grown directly onto the culet surface of a beveled diamond anvil.
  • Performance: The developed DAC achieved stable electrical transport measurements up to 192 GPa, significantly extending the pressure range and stability compared to conventional electrode insertion methods.
  • Synthesis Pathway: Sulfur hydride (H2S) was synthesized into superconducting phases using a low-temperature (200 K), rapid high-pressure (120 GPa) compression pathway.
  • Superconductivity Observed: A clear two-step superconducting transition with zero resistance was observed under high pressure.
  • Phase Identification: The higher transition temperature (Tc1, ~30 K class) is suggested to correspond to C2/c HS2, while the lower Tc phase (Tc2, ~15 K class) corresponds to elemental sulfur.
  • Critical Field: The Tc1 phase exhibited a high upper critical field Hc2(0) of 53.0 T at 154 GPa, demonstrating robust superconducting properties.
ParameterValueUnitContext
Maximum Pressure Achieved192GPaLimit of measurement before anvil failure
Initial Compression Pressure120GPaPressure achieved after rapid squeeze
High Tc Phase (Tc1) Onset~35KEstimated onset at 154 GPa
Low Tc Phase (Tc2) Onset15KObserved at 120 GPa
Upper Critical Field Hc2(0) (Tc1)53.0TExtrapolated value at 154 GPa
Upper Critical Field Hc2(0) (Tc2)28.2TExtrapolated value at 154 GPa
Coherence Length Ο(0) (Tc1)2.5nmCalculated using Ginzburg-Landau formula
Coherence Length Ο(0) (Tc2)3.4nmCalculated using Ginzburg-Landau formula
Sample Space Dimensions15 x 20”mArea surrounded by UDD insulation
BDD Boron/Carbon Ratio2500ppmTuned using C3H9B gas during MPCVD
BDD Growth Pressure (MPCVD)70TorrTotal gas pressure during BDD deposition
BDD Microwave Power500WPower used during BDD deposition
UDD Growth Pressure (MPCVD)35TorrTotal gas pressure during UDD deposition
UDD Microwave Power350WPower used during UDD deposition
Metal Mask Annealing450°C1h duration in Ar gas-flow

The experiment involved two main stages: BDD/UDD fabrication on the anvil, and high-pressure synthesis/measurement.

  1. Lithography: Electron Beam Lithography (EBL) was used on the beveled diamond anvil to define the shape of the micro-electrodes.
  2. Mask Deposition: A Ti/Au thin film metal mask was deposited via a lift-off process.
  3. Adhesion Enhancement: The mask was annealed at 450 °C for 1 hour under Ar gas-flow to form a TiC intermediate layer, ensuring strong adhesion between the diamond and the metal.
  4. BDD Growth: Epitaxial BDD was selectively grown onto the uncovered diamond surface using Hydrogen-Induced Microwave-Assisted Plasma Chemical Vapor Deposition (MPCVD).
    • Source Gases: CH4 (carbon source) and C3H9B (boron dopant, 2500 ppm B/C ratio).
    • Conditions: 70 Torr total pressure, 300 sccm total gas flow, 500 W microwave power.
  5. Cleaning: The metal mask and graphite impurities were removed using a wet etching mixture of HNO3 and H2SO4 at 400 °C for 30 minutes.
  6. UDD Insulation: An Undoped Diamond (UDD) insulating layer was deposited around the BDD electrodes using similar MPCVD processes.
    • Conditions: 35 Torr total pressure, 400 sccm total gas flow (H2 and CH4), 350 W microwave power.
  1. Gasket Preparation: A composite gasket was used, featuring a cubic boron nitride (cBN) center part and a rhenium (Re) outer plate. A 30 ”m sample chamber hole was fabricated in the cBN using Focused Ion Beam (FIB).
  2. Low-Temperature Filling: The DAC was cooled by dipping in liquid nitrogen, and the temperature was monitored (~200 K). H2S gas was introduced, solidified, and then changed to a liquid state around 200 K.
  3. Rapid Compression: The DAC screw was rapidly squeezed while the temperature was held around 200 K, quickly increasing the pressure up to 120 GPa (low-temperature, high-pressure pathway).
  4. Annealing and Measurement: The sample underwent room temperature annealing (resistance dropped from 77 kΩ to 38 Ω over 26 hours). Electrical resistance was measured using a standard four-probe method (PPMS/Quantum Design).
  5. Post-Compression Treatment: To further promote chemical reactions, the sample was annealed in an oven (up to 100 °C) and subsequently heated using an IR laser (1080 nm, 10-20 W).
  6. Characterization: Crystal structure was evaluated in-situ using Synchrotron X-ray Diffraction (XRD).

The development of stable, integrated BDD micro-electrodes on beveled diamond anvils is a significant advancement for extreme environment research and sensing technology.

Industry/FieldRelevance of Technology
High-Pressure PhysicsEnables stable, repeatable in-situ electrical measurements (resistivity, Tc, Hc2) up to multi-megabar pressures, crucial for discovering novel materials (e.g., room-temperature superconductors).
Diamond ElectronicsDemonstrates advanced fabrication techniques (EBL, MPCVD) for creating complex, integrated BDD/UDD micro-structures on non-planar (beveled) diamond surfaces.
Extreme Environment SensingBDD electrodes are chemically inert and mechanically robust, making them ideal for sensors (pressure, temperature, electrochemical) operating under extreme conditions (high pressure, high temperature, corrosive media).
Hydrogen EconomyDirectly supports the design and characterization of functional materials like hydrogen-storage alloys and hydrogen-rich superconductors.
Quantum Materials DiscoveryProvides a reliable platform for synthesizing and characterizing new high-Tc superconductors and other exotic quantum phases under pressure.
6ccvd.com RelevanceExpertise in high-quality CVD diamond growth (BDD and UDD) is essential for fabricating these integrated anvil components, particularly the precise control over doping (2500 ppm B/C) and epitaxial growth required for micro-electrodes.
View Original Abstract

Abstract A diamond anvil cell (DAC) has become an effective tool for investigating physical phenomena that occur at extremely high pressure, such as high-transition temperature superconductivity. Electrical transport measurements, which are used to characterize one of the most important properties of superconducting materials, are difficult to perform using conventional DACs. The available sample space in conventional DACs is very small and there is an added risk of electrode deformation under extreme operating conditions. To overcome these limitations, we herein report the fabrication of a boron-doped diamond microelectrode and undoped diamond insulation on a beveled culet surface of a diamond anvil. Using the newly developed DAC, we have performed in-situ electrical transport measurements on sulfur hydride H 2 S, which is a well-known precursor of the pressure-induced, high-transition temperature superconducting sulfur hydride, H 3 S. These measurements conducted under high pressures up to 192 GPa, indicated the presence of a multi-step superconducting transition, which we have attributed to elemental sulfur and possibly HS 2 .