The influence of Structural Dynamics in Two-Dimensional Hybrid Organic-Inorganic Perovskites on their Photoluminescence Efficiency – Neutron scattering analysis
arxiv(2024)
摘要
Two-dimensional hybrid organic-inorganic perovskites (HOIPs) have emerged as
promising materials for light-emitting diode applications. In this study, by
using time-of-flight neutron spectroscopy we identified and quantitatively
separated the lattice vibrational and molecular rotational dynamics of two
perovskites, butylammonium lead iodide (BA)_2PbI_4 and
phenethyl-ammonium lead iodide (PEA)_2PbI_4. By examining
the corresponding temperature dependence, we found that the lattice vibrations,
as evidenced by neutron spectra, are consistent with the lattice dynamics
obtained from Raman scattering. We revealed that the rotational dynamics of
organic molecules in these materials tend to suppress their photoluminescence
quantum yield while the vibrational dynamics did not show predominant
correlations with their optoelectronic properties. This study proposes that the
rotational motions of the polarized molecules could significantly interrupt the
exciton binding energy potential, cause the exciton dissociations, enhance the
non-radiative recombination rates, and hence reduce the photoluminescence
yield. These findings provide a deeper understanding of the fundamental
interactions in 2D HOIPs and may guide the design of more efficient
light-emitting materials for advanced technological applications.
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