Phonon-limited electron mobility in Si, GaAs, and GaP with exact treatment of dynamical quadrupoles

Brunin, Guillaume; Miranda, Henrique; Giantomassi, Matteo; Royo, Miquel; Stengel, Massimiliano; Verstraete, Matthieu J.; Gonze, Xavier; Rignanese, Gian‐Marco; Hautier, Geoffroy

doi:10.1103/physrevb.102.094308

Cited by 67 publications

(101 citation statements)

References 87 publications

(184 reference statements)

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“…[14,15]. For lightly doped semiconductors, the current state of the art is the full wave vector dependent solution of Boltzmann's equation [16][17][18], using an electron-phonon coupling (EPC) scattering kernel calculated from first principles and making an effective relaxation time approximation: Each electron state has a single averaged scattering time, in the mean field of all other electrons in equilibrium. This approach has only started to be applied to transport in metals recently [19][20][21], in part because most metal Fermi surfaces are much larger than the pockets found in lightly doped semiconductors.…”

Section: Introductionmentioning

confidence: 99%

Thermoelectric properties of elemental metals from first-principles electron-phonon coupling

Gennaro

Verstraete

2020

Phys. Rev. B

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The Seebeck coefficient is one of the key ingredients in thermoelectric properties, and it is often calculated based simply on the electronic band structure, within the frame of Boltzmann's transport theory and the constant relaxation time approximation. Despite the simplicity and popularity of this approximation, its validity is not fully justified even in lightly doped semiconductors, and it breaks down completely in metals. On the other hand, more sophisticated first-principles approaches are available but require the computation of the full electronphonon coupling. Here, we demonstrate with several simple (alkali and noble) metals viz., Li, Na, K, Cu, Ag, Au, and Pt, that the variational approach based on ab initio couplings can reproduce experimental Seebeck coefficients quantitatively, whereas the constant relaxation time approximation yields significant quantitative discrepancies and often fails to predict the correct sign. Calculations of the electrical resistivity of these metals via the variational approach are also reported.

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Section: Introductionmentioning

confidence: 99%

Thermoelectric properties of elemental metals from first-principles electron-phonon coupling

Gennaro

Verstraete

2020

Phys. Rev. B

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“…Note added.-Recently, we became aware of a related work by another group that reaches similar conclusions about the importance of the dynamical quadrupole term to obtain an accurate physical description of e-ph interactions [25,26].…”

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confidence: 84%

“…Yet, DFPT is too costly to use directly on the ultrafine Brillouin zone grids needed to compute e-ph relaxation times and charge transport using the BTE. The current approach relies on Fourier interpolation techniques to capture the short-range e-ph interactions [23][24][25][26] while adding the dipole Fröhlich term in reciprocal space for polar materials. Deriving and computing the Fröhlich interaction [27,28] has been a first step toward implementing Vogl's modern e-ph theory in firstprinciples calculations and correctly capturing the longrange e-ph contributions.…”

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confidence: 99%

Piezoelectric Electron-Phonon Interaction from Ab Initio Dynamical Quadrupoles: Impact on Charge Transport in Wurtzite GaN

et al. 2020

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First-principles calculations of e-ph interactions are becoming a pillar of electronic structure theory. However, the current approach is incomplete. The piezoelectric (PE) e-ph interaction, a long-range scattering mechanism due to acoustic phonons in noncentrosymmetric polar materials, is not accurately described at present. Current calculations include short-range e-ph interactions (obtained by interpolation) and the dipolelike Frölich long-range coupling in polar materials, but lack important quadrupole effects for acoustic modes and PE materials. Here we derive and compute the long-range e-ph interaction due to dynamical quadrupoles, and apply this framework to investigate e-ph interactions and the carrier mobility in the PE material wurtzite GaN. We show that the quadrupole contribution is essential to obtain accurate e-ph matrix elements for acoustic modes and to compute PE scattering. Our work resolves the outstanding problem of correctly computing e-ph interactions for acoustic modes from first principles, and enables studies of e-ph coupling and charge transport in PE materials.

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“…Recent work has applied this approach to compute the transport behavior of large numbers of materials, including 48,000 semiconductors in the Materials Project database by Ricci et al 27 , 809 sulfides by Miyata et al 28 , and 75 potential thermoelectric candidates by Xing et al 29 ; however, the unphysical treatment of electron scattering and the reliance on an empirical tuning parameter often results in significant errors. (iii) Finally, the fully first principles approach to calculating the electron-phonon interaction based on density functional perturbation theory (DFPT) combined with Wannier interpolation can now yield highly accurate electron lifetimes and have demonstrated remarkable agreement to experimental measurements of electron mobility and conductivity [30][31][32][33][34][35] . The calculation of the scattering matrix elements needed to obtain electron lifetimes is highly computationally demanding, even when approximations are made.…”

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confidence: 99%

Efficient calculation of carrier scattering rates from first principles

et al. 2021

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The electronic transport behaviour of materials determines their suitability for technological applications. We develop a computationally efficient method for calculating carrier scattering rates of solid-state semiconductors and insulators from first principles inputs. The present method extends existing polar and non-polar electron-phonon coupling, ionized impurity, and piezoelectric scattering mechanisms formulated for isotropic band structures to support highly anisotropic materials. We test the formalism by calculating the electronic transport properties of 23 semiconductors, including the large 48 atom CH3NH3PbI3 hybrid perovskite, and comparing the results against experimental measurements and more detailed scattering simulations. The Spearman rank coefficient of mobility against experiment (rs = 0.93) improves significantly on results obtained using a constant relaxation time approximation (rs = 0.52). We find our approach offers similar accuracy to state-of-the art methods at approximately 1/500th the computational cost, thus enabling its use in high-throughput computational workflows for the accurate screening of carrier mobilities, lifetimes, and thermoelectric power.

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Phonon-limited electron mobility in Si, GaAs, and GaP with exact treatment of dynamical quadrupoles

Cited by 67 publications

References 87 publications

Thermoelectric properties of elemental metals from first-principles electron-phonon coupling

Thermoelectric properties of elemental metals from first-principles electron-phonon coupling

Piezoelectric Electron-Phonon Interaction from Ab Initio Dynamical Quadrupoles: Impact on Charge Transport in Wurtzite GaN

Efficient calculation of carrier scattering rates from first principles

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