First-principles calculations of charge carrier transport

Drift and Hall carrier mobilities in bulk and 2D semiconductors are fundamental properties in semiconductor devices and govern their switching frequency, photoconductive grain, and transport in solar cells and light-emitting diodes. Recent advances in electron-phonon calculations have enabled the study of these properties with predictive accuracy and without resorting to empirical parameters [1].

In this talk, we review the various approaches and approximations starting from the Kadanoff–Baym equation of motion and with a focus on the iterative Boltzmann transport equation (BTE) and the Kubo formalism.

For the BTE, we present drift and Hall mobility results for bulk [2] and monolayers [3], showing the importance of long-range electrostatics.

Importantly, we discuss guidelines for robust, accurate, reproducible and efficient calculations [4].

We will then show the limits of the state-of-the art methods and show the importance of self-consistency for the electron lifetimes [5] and spectral functions [6].

These recent developments culminated in the development of a self-consistent Kubo (scKubo) transport method [7], a rung above the BTE theory as it includes non-perturbative effects through a first-order vertex correction.

We will present and discuss fully ab-initio scKubo results in AlN and SrVO3 [6].

[1] S. Poncé, W. Li, S. Reichardt, and F. Giustino, Rep. Prog. Phys. 83, 036501 (2020)

[2] S. Poncé, F. Macheda, E.R. Margine, N. Marzari, N. Bonini, and F. Giustino, Phys. Rev. Research 3, 043022 (2021)

[3] S. Poncé, M. Royo, M. Gibertini, N. Marzari, and M. Stengel, Phys. Rev. Lett. 130, 166301 (2023)

[4] J. Zhou, S. Poncé, and J.C. Charlier, Phys. Rev. B 110, 125304 (2024)

[5] J.M. Lihm, S. Poncé, and C.H. Park, Phys. Rev. B 110, L121106 (2024)

[6] J.M. Lihm and S. Poncé, to be submitted (2024)

[7] T. Holstein, Annals of Physics 29, 410 (1964)