Proceedings of MATSUS Fall 2024 Conference (MATSUSFall24)
DOI: https://doi.org/10.29363/nanoge.matsusfall.2024.167
Publication date: 28th August 2024
Metal halide perovskites have attracted much attention for use in several optoelectronic applications, including photovoltaics and light emission. Due to their superior stability and bright photoluminescence, quasi-2D or layered perovskites such as the Ruddlesden-Popper perovskite phenylethylammonium lead iodide (PEAPbI4) have been a popular choice for many applications. However, these materials typically have exciton binding energies of 100s of meV that can thus greatly alter optoelectronic properties due to a large population of excitons present at ambient temperatures [1]. Using both transient and steady-state spectroscopic methods, we have investigated the excitonic properties of quasi-2D perovskites including PEAPbI4 and thiophenemethylammonium (ThMAPbI4). In PEAPbI4, we separate contributions from free charge-carriers and excitons and observe ultrafast cooling of free charges followed by slower recombination of both excitons and a minority concentration of free charges [2]. In ThMAPbI4, we investigate the temperature-dependent properties from room temperature to 77 K and characterize emission from a defect-bound exciton at low temperatures [3]. Together, these studies highlight the relationship between structure and optoelectronic properties of these materials.
A common strategy for circumventing the poor transport properties of quasi-2D perovskites is to form heterostructures with 3D perovskites, where quasi-2D materials are incorporated into 3D perovskite thin films as either a mixture or a capping layer. Using a combination of visible transient absorption spectroscopy (TAS) and optical pump/THz probe spectroscopy (OPTP), we have evaluated device-relevant 3D perovskite thin films which have been treated with phenylethylammonium salts in order to preferentially form RP phases at the surface of the films [4]. In all cases, we find that the surface is a complex mixture of 2D and 3D components. In addition to observing that the charge-carrier dynamics are sensitive to the film preparation method, we distinguish between bulk and surface passivation effects and query charge transfer between RP and 3D species.
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