A rotating organic cation and a dynamically disordered soft inorganic cage are the hallmark features of organic-inorganic lead-halide perovskites. Understanding the interplay between these two subsystems is a challenging problem, but it is this coupling that is widely conjectured to be responsible for the unique behavior of photocarriers in these materials. In this work, we use the fact that the polarizability of the organic cation strongly depends on the ambient electrostatic environment to put the molecule forward as a sensitive probe of the local crystal fields inside the lattice cell. We measure the average polarizability of the C/N–H bond stretching mode by means of infrared spectroscopy, which allows us to deduce the character of the motion of the cation molecule, find the magnitude of the local crystal field, and place an estimate on the strength of the hydrogen bond between the hydrogen and halide atoms. Our results pave the way for understanding electric fields in lead-halide perovskites using infrared bond spectroscopy.
Cesium lead halide perovskite materials have recently attracted attention in view of their optical and electronic properties which make them excellent candidates for potential applications in lasers, light emitting diodes and photodetectors. In this work, we provide the experimental and theoretical evidence for sequential photon absorption/re-emission in CsPbBr3 perovskite microwires. Using two-photon excitation, we recorded PL lifetimes and emission spectra as a function of the lateral distance between PL excitation and collection positions along the microwire, with separations exceeding 100 µm. As the propagation length increases, the PL spectrum develops a new emission peak that is red-shifted by 20 nm from the main emission and is accompanied by the appearance of the well-resolved rise times in the PL kinetics. We undertake quantitative modeling that accounts for bimolecular recombination and photon recycling within the microwire waveguide, and find that it is sufficient to account for the observed decay modifications. The model relies on a high radiative efficiency in CsPbBr3 perovskite microwires to explain the photon recycling observed. Such findings provide crucial information about the potential impact of photon recycling and waveguide trapping on optoelectronic properties of cesium lead halide perovskite materials
Access to the requested content is limited to institutions that have purchased or subscribe to SPIE eBooks.
You are receiving this notice because your organization may not have SPIE eBooks access.*
*Shibboleth/Open Athens users─please
sign in
to access your institution's subscriptions.
To obtain this item, you may purchase the complete book in print or electronic format on
SPIE.org.
INSTITUTIONAL Select your institution to access the SPIE Digital Library.
PERSONAL Sign in with your SPIE account to access your personal subscriptions or to use specific features such as save to my library, sign up for alerts, save searches, etc.