Computational Method for Evaluating the Thermoelectric Power Factor for Organic Materials Modeled by the Holstein Model: A Time-Dependent Density Matrix Renormalization Group Formalism.

Abstract

Organic/polymeric materials are of emerging importance for thermoelectric conversion. The soft nature of these materials implies strong electron-phonon coupling, often leading to carrier localization. This poses great challenges for the conventional Boltzmann transport description based on relaxation time approximation and band structure calculations. In this work, combining the Kubo formula with the finite-temperature time-dependent density matrix renormalization group (FT-TD-DMRG) in the grand canonical ensemble, we developed a nearly exact algorithm to calculate the thermoelectric power factor PF = α2 σ, where α is the Seebeck coefficient and σ is the electrical conductivity, and apply the algorithm to Holstein Hamiltonian with electron-phonon coupling to model organic materials. Our algorithm can provide a unified description covering the weak coupling limit described by the bandlike Boltzmann transport to the strong coupling hopping limit.