Skip to content

Structural and Functional Properties of Si and Related Semiconducting Materials Processed by High-Pressure Torsion

MetadataDetails
Publication Date2023-03-30
JournalMATERIALS TRANSACTIONS
AuthorsYoshifumi Ikoma
InstitutionsMaterials Science & Engineering, Kyushu University
Citations15
AnalysisFull AI Review Included
Section titled “Structural and Functional Properties of Si and Related Semiconducting Materials Processed by High-Pressure Torsion”

This research utilizes High-Pressure Torsion (HPT) to induce severe plastic deformation (SPD) in Si and Si0.5Ge0.5, achieving novel metastable phases and significantly altered functional properties suitable for advanced devices.

  • Metastable Phase Formation: HPT successfully induced the strain-driven phase transformation sequence Si-I → Si-II → Si-III/XII in Si at a nominal pressure of 6 GPa.
  • Si-IV Synthesis: In-situ synchrotron XRD confirmed that annealing HPT-processed Si up to 473 K resulted in the formation of the hexagonal-diamond Si-IV phase from Si-III/XII.
  • Electrical Enhancement: Resistivity of Si decreased significantly (from ~0.2 Ωm to ~7 x 10-3 Ωm) with increasing shear strain, attributed to the formation of semimetallic Si-III.
  • Thermal Management: Thermal conductivity (Îș) of Si was drastically reduced from the bulk value (~140 W m-1K-1) to approximately 3 W m-1K-1, primarily due to grain refinement.
  • SiGe Alloy Discovery: HPT processing of Si0.5Ge0.5 formed the metastable bc8-Si0.5Ge0.5 phase, which exhibits semimetallic properties, analogous to Si-III.
  • Optical Properties: A weak, broad photoluminescence (PL) peak appeared in the visible light region after annealing, indicating the presence of Si-I nanograins exhibiting quantum confinement effects.
ParameterValueUnitContext
HPT Nominal Pressure (Si)6, 24GPaUsed for 10 mm and 5 mm diameter disks, respectively.
HPT Rotational Speed1rpmStandard processing speed for all HPT experiments.
Minimum Thermal Conductivity (Si)~3W m-1K-1Achieved after HPT processing (N ≄ 50), representing a 98% reduction from bulk Si (~140 W m-1K-1).
Minimum Resistivity (Si)~7 x 10-3ΩmAchieved at N=100 rotations, indicating semimetallic behavior due to Si-III formation.
Si-III Bandgap30meVPotential for narrow gap semiconductor applications.
Si-XII Bandgap0.24eVPotential for narrow gap semiconductor applications.
Si-IV Formation Temperature473KMaximum annealing temperature observed for Si-IV formation via in-situ synchrotron XRD.
bc8-Si0.5Ge0.5 Lattice Constant0.678nmMetastable phase formed in HPT-processed Si0.5Ge0.5.
Si-I Crystallite Size (N ≄ 50)<10nmEstimated average size for Si-I, Si-III, and Si-XII phases after HPT.
Si-I Volume Fraction (N=100, 6 GPa)~0.5N/ARemaining diamond-cubic phase after maximum deformation.
  1. Material Preparation: Single-crystal Si(100) wafers and bulk Si0.5Ge0.5 crystals (grown by the Traveling Liquidus-Zone, TLZ, method) were cut into disks (5 or 10 mm diameter).
  2. High-Pressure Torsion (HPT): Samples were processed at room temperature using a tungsten carbide lower anvil with a 0.25 mm deep cavity. Nominal pressures were 6 GPa or 24 GPa, applied at 1 rpm rotational speed for up to 100 rotations (N).
  3. In-situ Synchrotron XRD: Phase transformations during annealing were monitored using high-energy XRD (61.4 keV) at SPring-8 (BL04B1). Samples were annealed up to 473 K to observe the formation of Si-IV.
  4. Microstructural Characterization: High-Resolution Transmission Electron Microscopy (HRTEM) was used on ex-situ annealed samples (473 K for 2 h) to confirm the presence of Si-I and Si-IV nanograins.
  5. Electrical Property Measurement: Electrical resistivity was determined using a standard four-probe method.
  6. Thermal Property Measurement: Thermal diffusivity (α) was measured via the laser flash method. Thermal conductivity (Îș) was calculated using the formula Îș = αΔρ, where c (heat capacity) was fixed at 0.71 J g-1K-1.
  7. Optical Property Measurement: Photoluminescence (PL) spectra were collected at room temperature using a 488 nm laser to detect quantum confinement effects from Si nanograins.
  • Narrow Gap Semiconductor Devices: Utilizing the metastable Si-III (30 meV bandgap) and Si-XII (0.24 eV bandgap) phases for infrared detection, low-power electronics, and specialized sensors where conventional Si is unsuitable.
  • High-Efficiency Photovoltaics (Solar Cells): Leveraging Si-I nanograins for quantum confinement effects (visible light PL) and the potential light-absorbing properties of Si-IV (0.95 eV indirect bandgap) to enhance solar energy conversion efficiency, potentially utilizing Multiple Exciton Generation (MEG).
  • Advanced Thermoelectrics: The extreme reduction in thermal conductivity (Îș ~3 W m-1K-1) in HPT-processed Si and SiGe alloys is critical for improving the figure of merit (ZT) in thermoelectric generators, enabling efficient waste heat recovery.
  • Novel Semimetallic Components: Utilizing the semimetallic nature of Si-III and bc8-Si0.5Ge0.5 for specialized interconnects or electronic components requiring high carrier mobility or unique electrical interfaces.
  • Bulk Metastable Material Production: HPT enables the synthesis of these high-pressure metastable phases in bulk form (millimeter to centimeter scale), facilitating industrial scaling compared to traditional diamond anvil cell methods.
View Original Abstract

We report on high-pressure torsion (HPT) processing of Si and related semiconducting materials, and discuss their phase transformations and electrical, thermal, and optical properties. In-situ synchrotron x-ray diffraction revealed that the metastable bc8-structure Si-III and r8-structure Si-XII in the HPT-processed Si samples gradually disappeared and hexagonal-diamond Si-IV appeared during annealing up to 473 K. The formation of Si-III/XII in the samples processed at a nominal pressure of 6 GPa indicated the strain-induced phase transformation from diamond-cubic Si-I to a high-pressure tetragonal Si-II phase during HPT processing, and a following phase transformation from Si-II to Si-III/XII upon decompression. The resistivity decreased with increasing the number of anvil rotations due to the formation of semimetallic Si-III. The thermal conductivity of Si was reduced to ∌3 W m−1K−1 after HPT processing. A weak and broad photoluminescence peak associated with Si-I nanograins appeared in the visible light region after annealing. Metastable bc8-Si0.5Ge0.5 with a semimetallic property was formed by HPT processing of a traveling-liquidus-zone-grown Si0.5Ge0.5 crystal. These results indicate that the application of HPT processing to Si and related semiconductors paves the way to novel devices utilizing nanograins and metastable phases.