Ab initio optimization of phonon drag effect for lower-temperature thermoelectric energy conversion

Abstract

While the thermoelectric figure of merit zT above 300K has seen significant improvement recently, the progress at lower temperatures has been slow, mainly limited by the relatively low Seebeck coefficient and high thermal conductivity. Here we report, for the first time, success in first-principles computation of the phonon drag effect - a coupling phenomenon between electrons and non-equilibrium phonons - in heavily doped region and its optimization to enhance the Seebeck coefficient while reducing the phonon thermal conductivity by nanostructuring. Our simulation quantitatively identifies the major phonons contributing to the phonon drag, which are spectrally distinct from those carrying heat, and further reveals that while the phonon drag is reduced in heavily-doped samples, a significant contribution to Seebeck coefficient still exists. An ideal phonon filter is proposed to enhance zT of silicon at room temperature by a factor of 20 to around 0.25, and the enhancement can reach 70 times at 100K. This work opens up a new venue towards better thermoelectrics by harnessing non-equilibrium phonons.

References in corpus (6)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Maximally localized Wannier functions: Theory and applications
• Significant reduction of lattice thermal conductivity by electron-phonon interaction in silicon with high carrier concentrations: a first-principles study
• The role of lighter and heavier embedded nanoparticles on the thermal conductivity of SiGe alloys
• Thermoelectric transport properties of silicon: Towards an ab initio approach
• Unified picture for the colossal thermopower compound FeSb${}_2$

Cited by in corpus (26)

• Towards predictive many-body calculations of phonon-limited carrier mobilities in semiconductors
• First-principles mode-by-mode analysis for electron-phonon scattering channels and mean free path spectra in GaAs
• First-principles dynamics of electrons and phonons
• Thermoelectricity in correlated narrow-gap semiconductors
• Electron-phonon drag enhancement of transport properties from fully coupled \textit{ab initio} Boltzmann formalism
• Magneto-transport phenomena in p-doped diamond from first principles
• Coupled transport of phonons and carriers in semiconductors: A case study of n-doped GaAs
• Significant Phonon Drag Effect in Wide Bandgap GaN and AlN
• Acoustic Deformation Potentials of $n$-Type PbTe from First Principles
• Optical and thermal characterization of a group-III nitride semiconductor membrane by microphotoluminescence spectroscopy and Raman thermometry
• Leveraging Electron-Phonon Interaction to Enhance Thermoelectric Power Factor in Graphene-Like Semimetals
• Peak thermoelectric power factor of holey silicon films
• Nonlinear Hall effect from long-lived valley-polarizing relaxons
• Advances in the optimization of silicon-based thermoelectrics: a theory perspective
• Elasto-Dynamical Induced Spin and Charge Pumping in Bulk Heavy Metals
• Theory of Phason Drag Effect on Thermoelectricity
• SrPd, a candidate material with extremely large magnetoresistance
• Vibronics of multi-material nanopillared membranes and impact on the thermal conductivity
• Descriptors of intrinsic hydrodynamic thermal transport: screening a phonon database in a machine learning approach
• Impact of Electron-Phonon Interaction on Thermal Transport: A Review
• Modulation of Semiconductor Superlattice Thermopower Through Symmetry and Strain
• Theory of Seebeck ratchet in noncentrosymmetric electron-phonon coupled system
• Prototypical many-body signatures in transport properties of semiconductors
• Origin of anomalous temperature dependence of Nernst effect in narrow-gap semiconductors
• The elphbolt ab initio solver for the coupled electron-phonon Boltzmann transport equations
• Spatially Mapping Phonon Drag in Ultrascaled 5-nm Silicon Nanowire Field-Effect Transistor Based on a Quantum Hydrodynamic Formalism