Correlated electron-hole mechanism for molecular doping in organic semiconductors

Jing Li (1) , Gabriele d'Avino (1) , Anton Pershin (2) , Denis Jacquemin (3) , Ivan Duchemin (4) , David Beljonne (2) , Xavier Blase (1)

1 NEEL - TMC - Théorie de la Matière Condensée
2 Fonds de la Recherche Scientifique [FNRS]
3 UN - Université de Nantes
4 LSIM - Laboratory of Atomistic Simulation

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 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.

Domaines: Matière Condensée [cond-mat]; Science des matériaux [cond-mat.mtrl-sci]

Jing Li, Gabriele d'Avino, Anton Pershin, Denis Jacquemin, Ivan Duchemin, et al.. Correlated electron-hole mechanism for molecular doping in organic semiconductors. Physical Review Materials, 2017, 1 (2), pp.025602. ⟨10.1103/PhysRevMaterials.1.025602⟩. ⟨hal-01625561⟩