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The charged forms of π–conjugated chromophores are relevant in the field of organic electronics as charge carriers in optoelectronic devices, but also as energy storage substrates in organic batteries. In this context, intramolecular reorganization energy plays an important role in controlling material efficiency. In this work, we investigate how the diradical character influences the reorganization energies of holes and electrons by considering a library of diradicaloid chromophores. We determine the reorganization energies with the four-point adiabatic potential method using quantum–chemical calculations at density functional theory (DFT) level. To assess the role of diradical character, we compare the results obtained, assuming both closed-shell and open-shell representations of the neutral species. The study shows how the diradical character impacts the geometrical and electronic structure of neutral species, which in turn control the magnitude of reorganization energies for both charge carriers. Based on computed geometries of neutral and charged species, we propose a simple scheme to rationalize the small, computed reorganization energies for both n-type and p-type charge transport. The study is supplemented with the calculation of intermolecular electronic couplings governing charge transport for selected diradicals, further supporting the ambipolar character of the investigated diradicals. [ABSTRACT FROM AUTHOR]

We report clear room temperature ambipolar transport in ambient-air processed methylammonium lead iodide (MAPbI3) thin-film transistors (TFTs) with aluminum oxide gate-insulators and indium-zinc-oxide source/drain electrodes. The high ionicity of the MAPbI3 leads to p-type and n-type self-doping, and depending on the applied bias we show that simultaneous or selective transport of electrons and/or holes is possible in a single MAPbI3 TFT. The electron transport (n-type), however, is slightly more pronounced than the hole transport (p-type), and the respective channel resistances range from 5–11 and 44–55 MΩ/μm. Both p-type and n-type TFTs show good on-state characteristics for low driving voltages. It is also shown here that the on-state current of the n-type and p-type TFTs is highest in the slightly PbI2-rich and MAI-rich films, respectively, suggesting controllable n-type or p-type transport by varying precursor ratio. [ABSTRACT FROM AUTHOR]