Correlated electron-hole mechanism for molecular doping in organic semiconductors

Abstract

The electronic and optical properties of the paradigmatic F4TCNQ-doped pentacene in the low-doping limit are investigated by a combination of state-of-the-art many-body \emph{ab initio} methods accounting for environmental screening effects, and a carefully parametrized model Hamiltonian. We demonstrate that while the acceptor level lies very deep in the gap, the inclusion of electron-hole interactions strongly stabilizes dopant-semiconductor charge transfer states and, together with spin statistics and structural relaxation effects, rationalize the possibility for room-temperature dopant ionization. Our findings reconcile available experimental data, shedding light on the partial vs. full charge transfer scenario discussed in the literature, and question the relevance of the standard classification in shallow or deep impurity levels prevailing for inorganic semiconductors.

Keywords: Organic semiconductors, Molecular doping, Approximation methods for many-body systems, GW formalism, Bethe-Salpeter equation

References in corpus (2)

• First-principles GW calculations for fullerenes, porphyrins, phtalocyanine, and other molecules of interest for organic photovoltaic applications
• Quasi-Particle Self-Consistent $GW$ for Molecules

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• Microscopic Insight into the Electronic Structure of BCF-Doped Oligothiophenes from \textit{Ab initio} Many-Body Theory