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Investigation of the inherent field-driven charge transport behaviour of three-dimensional lead halide perovskites has largely remained challenging, owing to undesirable ionic migration effects near room temperature and dipolar disorder instabilities prevalent specifically in methylammonium-and-lead-based high-performing three-dimensional perovskite compositions. Here, we address both these challenges and demonstrate that field-effect transistors based on methylammonium-free, mixed metal (Pb/Sn) perovskite compositions do not suffer from ion migration effects as notably as their pure-Pb counterparts and reliably exhibit hysteresis-free p-type transport with a mobility reaching 5.4 cm2 V-1 s-1. The reduced ion migration is visualized through photoluminescence microscopy under bias and is manifested as an activated temperature dependence of the field-effect mobility with a low activation energy (~48 meV) consistent with the presence of the shallow defects present in these materials. An understanding of the long-range electronic charge transport in these inherently doped mixed metal halide perovskites will contribute immensely towards high-performance optoelectronic devices.

In spintronics, pure spin currents play a key role in transmitting, processing and storing information. A pure spin current is a flow of electron spin angular momentum without a simultaneous flow of charge current. It can be carried by conduction electrons or magnons and has been studied in many inorganic metals, semiconductors and insulators, but not yet in organic semiconductors. Charge carriers in π-conjugated organic materials are localized spin-1/2 polarons which move by hopping, but the mechanisms of their spin transport and relaxation are not well understood. Here we use ferromagnetic resonance spin pumping in a ferromagnet/conjugated polymer/nonmagnetic spin-sink trilayer to demonstrate the ability of polarons to carry pure spin currents over hundreds of nanometres with long spin relaxation times of up to a millisecond and to exhibit Hanle precession. By systematically comparing charge and spin transport on the same trilayer we show that spin-orbit coupling mediates spin relaxation at room temperature.

Many of the remarkable electrical and optical properties of organic semiconductors are governed by the interaction of electronic excitations with intra- and intermolecular vibrational modes. However, in specific systems this interaction is not understood in detail at a molecular level and this has been due, at least in part, to the lack of easy-to-use and widely available experimental probes of the structural dynamics. Here we demonstrate that thermal diffuse scattering in electron diffraction patterns from organic semiconductors, such as 6,13-bistriisopropyl-silylethynyl pentacene, allows the dominant lattice vibrational modes to be probed directly. The amplitude and direction of the dominant molecular motions were determined by comparison of the diffuse scattering with simulations and molecular dynamics calculations. Our widely applicable approach enables a much deeper understanding of the structural dynamics in a broad range of organic semiconductors.