Charge Transport and Carrier-Phonon Interactions in Soft Lattice Metal Halide Perovskites

Non-technical Description Metal halide perovskites are a unique class of “soft” semiconductors that have attracted enormous interest. They can be solution processed at relatively low temperatures and have shown promise for optoelectronic devices such as solar cells, light emitting diodes and radiation detectors. However, understanding charge transport in these materials remains elusive. Studies of charge transport are complicated by ion movement and the difficulty in forming high-quality electrical contacts. Furthermore, perovskites can degrade during processing or when depositing metal contacts on top of them. This results in excessive contact resistance and limits device performance. By physically laminating electrodes onto perovskite films, the team will avoid such degradation and be able to perform reliable electrical studies. They will combine studies of photocurrent and capacitance on temperature and light intensity with direct structural analysis. They will also vary contacts and use doping to further tailor the carrier density and explore unique phenomena in these materials. This systematic study will unravel the intriguing properties of perovskites and develop critical insights needed to design more efficient devices. The relevant research activities also offer valuable educational opportunities to students for training next generation of workforce in relevant technologies. Technical Description This project exploits a unique van der Waals integration strategy to create atomically clean contacts with greatly reduced contact resistance for a systematic electrical transport study of metal halide perovskites (MHPs). By physically laminating the prefabricated atomically flat thin film metal electrodes onto the perovskite thin films without directly exposing the perovskites to any lithography or deposition steps, this approach can effectively avoid the associated material degradations to achieve greatly reduced contact resistance for reliable electrical transport studies. The project will probe charge transport and photocarrier induced local lattice distortion, the associated phase transition, and their impact on the carrier dynamics and fundamental transport properties: including temperature- and illumination-dependent photo-conductance and photo-capacitance studies to probe carrier-phonon interactions, and their impact on the carrier recombination and transport properties; direct structural analysis to investigate the atomic structural change associated with the carrier generation under different illumination or temperature; developing different contacts or selective doping strategies to probe both electron and hole transport characteristics; using the optimized device fabrication and measurement protocols to probe the carrier-phonon interactions and ferroelectricity in low-dimensional MHPs and other related materials; and further tailoring the carrier density through a combination of chemical doping, electrical static doping and photodoping to probe carrier-phonon or carrier-carrier interactions and explore possible emergent phenomena. These research activities help develop a critical understanding of the fundamental photophysical, electrical transport properties, and the intriguing carrier-phonon interactions in this unique class of materials, which will not aim engineering improved photovoltaics or light-emitting diodes, but also help unlock new technological potentials from MHPs. This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.