Non-monotonic pressure dependence of the thermal conductivity of boron arsenide

Abstract

Recent experiments demonstrate that boron arsenide (BAs) is a showcase material to study the role of higher-order four-phonon interactions in affecting heat conduction in semiconductors. Here we use first-principles calculations to identify a phenomenon in BAs and a related material - boron antimonide, that has never been predicted or experimentally observed for any other material: competing responses of three-phonon and four-phonon interactions to pressure rise cause a non-monotonic pressure dependence of thermal conductivity, κ, which first increases similar to most materials and then decreases. The resulting peak in κ shows a strong temperature dependence from rapid strengthening of four-phonon interactions relative to three-phonon processes with temperature. Our results reveal pressure as a knob to tune the interplay between the competing phonon scattering mechanisms in BAs and similar compounds, and provide clear experimental guidelines for observation in a readily accessible measurement regime.

High-pressure phases of boron arsenide with potential high thermal conductivity

“…Fig. 5 shows the calculated κ nat and κ pure as a function of pressure for zb-and 2H-BAs at 300 K. The calculated κ nat and κ pure for zb-BAs decreases with pressure, which is in good agreement with the previous theoretical calculation with three-phonon scattering 65,66 . The calculated thermal conductivity for 2H-BAs also decreases under pressure but decreases a little.…”

“…Thus, the thermal conductivity usually increases under pressure. Recently, the thermal conductivities as a function of pressure for many materials have been studied [64][65][66][67][68][69] . For example, under pressure, κ for diamond, BN, MgO and AlN increase, while κ for HgTe, BeTe and BSb decrease and CdTe and ZnTe remain constant.…”

“…However, the 3 rd anharmonic interaction increases with pressure for zb-and 2H-BAs, which will lead to the decrease in κ. In addition, the influence of the three-phonon scattering phase space between acoustic phonons 65 , acoustic and optic phonons as well as optic phonons on thermal conductivity are also studied. However, the increase in 3 rd anharmonic interaction under pressure is the dominated parameter for the negative pressure dependent thermal conductivity for zb-and 2H-BAs.…”

Ultrahigh thermal conductivity in isotope-enriched cubic boron nitride

“…To understand the high thermal conductivity and large isotope effect we observed in cBN, we employed the unified ab initio theory we developed for phonon-mediated thermal transport in solids (22,32,33). Briefly, we obtained the required phonon properties and anharmonic interatomic force constants within the density functional theory framework (Quantum ESPRESSO), and acquired the thermal conductivity by solving the Peierls-Boltzmann equation (PBE) for phonon transport including three-and four-phonon scattering, phononisotope, and phonon-impurity scattering.…”

Pressure‐Dependent Behavior of Defect‐Modulated Band Structure in Boron Arsenide

“…One interesting feature is that the 11 B Raman peak splits into two peaks starting from ≈4 GPa and this split increases with pressure, eventually reaches 7.1 cm −1 at 19.4 GPa. This phenomenon, according to the first‐principles calculations by Ravichandran et al., comes from the LO/TO phonon splitting, [ 22 ] as a result of different hardening rates between the LO and TO phonons at high pressure. According to the calculations, LO/TO splitting already exists at ambient condition.…”