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High thermal conductivity driven by the unusual phonon relaxation time platform in 2D monolayer boron arsenide

MetadataDetails
Publication Date2020-01-01
JournalRSC Advances
AuthorsYanxiao Hu, Dengfeng Li, Yan Yin, Shichang Li, Hangbo Zhou
InstitutionsChongqing University of Posts and Telecommunications, A*STAR Graduate Academy
Citations24
AnalysisFull AI Review Included

This study investigates the diffusive thermal transport properties of two-dimensional (2D) monolayer honeycomb Boron Arsenide (h-BAs) using first-principles calculations and the Boltzmann Transport Equation (BTE).

  • High Thermal Conductivity (TC): Monolayer h-BAs exhibits an ultra-high TC of 181 W m-1 K-1 at 300 K, positioning it as a leading thermally conductive 2D semiconductor.
  • Dominant Heat Carriers: Unlike graphene and h-BN, where out-of-plane acoustic (ZA) phonons dominate TC, h-BAs heat transport is primarily driven by in-plane acoustic (IA) modes (76% contribution).
  • Unique Relaxation Platform: The high TC is attributed to an unusual frequency-independent “platform” region observed in the relaxation time of IA phonons, extending relaxation times up to 102 ps.
  • Scattering Suppression Mechanism: This platform results from the suppression of key three-phonon scattering channels (specifically ZA + ZA → IA) due to the extremely flat dispersion of the ZA phonon branch in h-BAs.
  • Comparative Advantage: h-BAs TC is approximately one order of magnitude higher than that of h-GaN (16 W m-1 K-1), despite similar mass densities, highlighting the critical role of phonon spectrum differences.
  • Physical Insight: The low TC of h-GaN is linked to a downward trend in its out-of-plane optical (ZO) branch, which increases the phase space for ZA + IA → ZO scattering, a mechanism suppressed in h-BAs.
ParameterValueUnitContext
Thermal Conductivity (h-BAs)181W m-1 K-1Iterative BTE solution at 300 K
Thermal Conductivity (h-GaN)16W m-1 K-1Iterative BTE solution at 300 K
IA Mode Contribution (h-BAs)76%Percentage of total TC at 300 K
ZA Mode Contribution (h-BAs)23%Percentage of total TC at 300 K
TC Ratio (h-BAs / h-GaN)>10-Comparison at 300 K
Lattice Constant (h-BAs)3.39AOptimized structure
LO-TO Frequency Gap0.31THzSplitting at Gamma (Γ) point
Maximum ZA Frequency1.81THzIndicates weak out-of-plane vibration
LA Group Velocity (Long-wave)9.3 x 103m s-1Longitudinal Acoustic branch limit
Born Effective Charge (B, in-plane)1.744eZ*(B)xx
Born Effective Charge (B, out-of-plane)-0.051eZ*(B)zz (Indicates minimal charge transfer)
Dielectric Constant (In-plane)4.678-Δxx
Dielectric Constant (Out-of-plane)1.162-Δzz

The thermal properties were determined using computational physics methods based on Density Functional Theory (DFT) and the phonon Boltzmann Transport Equation (BTE).

  1. DFT Calculation: Performed using the Vienna Ab initio Simulation Package (VASP) employing the Generalized Gradient Approximation (GGA) functional (PBE).
  2. Structural Optimization: The structure was fully relaxed with a kinetic energy cutoff of 550 eV. Relaxation continued until the interatomic force was less than 10-5 eV A-1.
  3. Electronic Convergence: Energy convergence criteria were set to 10-7 eV, utilizing a Γ-centered k-mesh of 21 x 21 x 1 for Brillouin Zone (BZ) sampling.
  4. Phonon BTE Solution: The ShengBTE code was used to solve the BTE, calculating thermal conductivity under both the Relaxation Time Approximation (RTA) and iterative methods.
  5. Interatomic Force Constants (IFCs): Both 2nd and 3rd order IFCs were calculated via the finite displacement method.
    • Supercells used: 7 x 7 x 1 (for 2nd IFCs) and 3 x 3 x 1 (for 3rd IFCs).
    • Interactions were considered up to the 7th nearest neighbors (cutoff distance 0.68 nm).
  6. Scattering Calculation: A dense 101 x 101 x 1 q-mesh was used for accurate phonon-phonon scattering calculations.
  7. Long-Range Correction: Born effective charges and dielectric constants were calculated using Density Functional Perturbation Theory (DFPT) to correct the dynamical matrix for long-range electrostatic interactions.
  8. Isotope Inclusion: Natural isotopic abundances for Boron (10B and 11B) and Arsenic (75As) were included in the scattering rate calculations.

The exceptional thermal conductivity of h-BAs, combined with its semiconductor properties (reported band gap of 1.18 eV), makes it highly promising for thermal management in advanced microelectronic and optoelectronic systems.

  • Thermal Management in Integrated Circuits (ICs): Utilizing h-BAs as an ultra-efficient 2D heat spreader or substrate layer to dissipate localized heat in highly miniaturized, high-power density electronic devices.
  • High-Frequency and Power Electronics: Application in Gallium Nitride (GaN) or Silicon Carbide (SiC) based power devices where thermal bottlenecks limit performance and reliability. h-BAs could serve as a superior thermal interface material (TIM) or buffer layer.
  • Optoelectronics and Lasers: Use in short-wavelength optoelectronic devices (e.g., UV LEDs or lasers) where localized heating is critical. The high TC ensures stable operating temperatures and extended device lifespan.
  • Advanced Semiconductor Architectures: Integration into heterostructures or van der Waals stacks where both high carrier mobility and excellent thermal dissipation are required simultaneously.
  • Thermal Interface Materials (TIMs): Development of h-BAs nanoflakes or films for use in high-performance TIMs, replacing conventional materials like graphene or h-BN in demanding thermal applications.
View Original Abstract

The cubic boron arsenide (BAs) crystal has received extensive research attention because of its ultra-high thermal conductivity comparable to that of diamond.