Zhiwei Ding

Seeded growth of boron arsenide single crystals with high thermal conductivity

Materials with high thermal conductivities are crucial to effectively cooling high-power-density electronic and optoelectronic devices. Recently, zinc-blende boron arsenide (BAs) has been predicted to have a very high thermal conductivity of over 2000 W m−1 K−1 at room temperature by first-principles calculations, rendering it a close competitor for diamond which holds the highest thermal conductivity among bulk materials. Experimental demonstration, however, has proved extremely challenging, especially in the preparation of large high quality single crystals. Although BAs crystals have been previously grown by chemical vapor transport (CVT), the growth process relies on spontaneous nucleation and results in small crystals with multiple grains and various defects. Here, we report a controllable CVT synthesis of large single BAs crystals (400–600 μm) by using carefully selected tiny BAs single crystals as seeds. We have obtained BAs single crystals with a thermal conductivity of 351 ± 21 W m−1 K−1 at room ...

Ab initio study of electron mean free paths and thermoelectric properties of lead telluride

Last few years have witnessed significant enhancement of thermoelectric figure of merit of lead telluride (PbTe) via nanostructuring. Despite the experimental progress, current understanding of the electron transport in PbTe is based on either band structure calculation using first principles with constant relaxation time approximation or empirical models, both relying on adjustable parameters obtained by fitting experimental data. Here, we report parameter-free first-principles calculation of electron and phonon transport properties of PbTe, including mode-by-mode electron-phonon scattering analysis, leading to detailed information on electron mean free paths and the contributions of electrons and phonons with different mean free paths to thermoelectric transport properties in PbTe. Such information will help to rationalize the use and optimization of nanosctructures to achieve high thermoelectric figure of merit.

Unusual high thermal conductivity in boron arsenide bulk crystals

Moving the heat aside with BAs Thermal management becomes increasingly important as we decrease device size and increase computing power. Engineering materials with high thermal conductivity, such as boron arsenide (BAs), is hard because it is essential to avoid defects and impurities during synthesis, which would stop heat flow. Three different research groups have synthesized BAs with a thermal conductivity around 1000 watts per meter-kelvin: Kang et al., Li et al., and Tian et al. succeeded in synthesizing high-purity BAs with conductivities half that of diamond but more than double that of conventional metals (see the Perspective by Dames). The advance validates the search for high-thermal-conductivity materials and provides a new material that may be more easily integrated into semiconducting devices. Science, this issue p. 575, p. 579, p. 582; see also p. 549 Boron arsenide has an ultrahigh thermal conductivity, making it competitive with diamond for thermal management applications. Conventional theory predicts that ultrahigh lattice thermal conductivity can only occur in crystals composed of strongly bonded light elements, and that it is limited by anharmonic three-phonon processes. We report experimental evidence that departs from these long-held criteria. We measured a local room-temperature thermal conductivity exceeding 1000 watts per meter-kelvin and an average bulk value reaching 900 watts per meter-kelvin in bulk boron arsenide (BAs) crystals, where boron and arsenic are light and heavy elements, respectively. The high values are consistent with a proposal for phonon-band engineering and can only be explained by higher-order phonon processes. These findings yield insight into the physics of heat conduction in solids and show BAs to be the only known semiconductor with ultrahigh thermal conductivity.

Phonon Hydrodynamic Heat Conduction and Knudsen Minimum in Graphite

In the hydrodynamic regime, phonons drift with a nonzero collective velocity under a temperature gradient, reminiscent of viscous gas and fluid flow. The study of hydrodynamic phonon transport has spanned over half a century but has been mostly limited to cryogenic temperatures (∼1 K) and more recently to low-dimensional materials. Here, we identify graphite as a three-dimensional material that supports phonon hydrodynamics at significantly higher temperatures (∼100 K) based on first-principles calculations. In particular, by solving the Boltzmann equation for phonon transport in graphite ribbons, we predict that phonon Poiseuille flow and Knudsen minimum can be experimentally observed above liquid nitrogen temperature. Further, we reveal the microscopic origin of these intriguing phenomena in terms of the dependence of the effective boundary scattering rate on momentum-conserving phonon-phonon scattering processes and the collective motion of phonons. The significant hydrodynamic nature of phonon transport in graphite is attributed to its strong intralayer sp2 hybrid bonding and weak van der Waals interlayer interactions. More intriguingly, the reflection symmetry associated with a single graphene layer is broken in graphite, which opens up more momentum-conserving phonon-phonon scattering channels and results in stronger hydrodynamic features in graphite than graphene. As a boundary-sensitive transport regime, phonon hydrodynamics opens up new possibilities for thermal management and energy conversion.

Electron mean-free-path filtering in Dirac material for improved thermoelectric performance

Significance Using ab initio simulations, we uncover the electron mean-free-path (MFP) spectrum in Dirac material and specifically show how the thermoelectric efficiency can greatly benefit from a distinct, monotonically decreasing trend of electron MFPs arising from the linear energy-momentum dispersion implied by the Dirac band topology. In the past, it was generally assumed that for the nanostructuring approach to be effective, one should design nanostructures to have characteristic length larger than the electron MFP but smaller than the phonon MFP to reduce thermal conductivity. Our results show that enhancement in thermoelectric performance can be achieved in Dirac materials even when they are smaller than the electron MFP by selectively filtering out long-MFP electrons that are harmful to the Seebeck coefficient. Recent advancements in thermoelectric materials have largely benefited from various approaches, including band engineering and defect optimization, among which the nanostructuring technique presents a promising way to improve the thermoelectric figure of merit (zT) by means of reducing the characteristic length of the nanostructure, which relies on the belief that phonons’ mean free paths (MFPs) are typically much longer than electrons’. Pushing the nanostructure sizes down to the length scale dictated by electron MFPs, however, has hitherto been overlooked as it inevitably sacrifices electrical conduction. Here we report through ab initio simulations that Dirac material can overcome this limitation. The monotonically decreasing trend of the electron MFP allows filtering of long-MFP electrons that are detrimental to the Seebeck coefficient, leading to a dramatically enhanced power factor. Using SnTe as a material platform, we uncover this MFP filtering effect as arising from its unique nonparabolic Dirac band dispersion. Room-temperature zT can be enhanced by nearly a factor of 3 if one designs nanostructures with grain sizes of ∼10 nm. Our work broadens the scope of the nanostructuring approach for improving the thermoelectric performance, especially for materials with topologically nontrivial electronic dynamics.