Disentangling Refractive Index Contributions in Transient Absorption Spectroscopy of Two-Dimensional Halide Perovskites
Xian Wei Chua, Yorrick Boeije, Taeheon Kang, Arjun Ashoka, Shabnum Maqbool, Akshay Rao, Samuel D. Stranks
TL;DR
This paper clarifies how refractive index changes affect the interpretation of transient absorption data in 2D halide perovskites.
Contribution
A Kramers–Kronig constrained analysis method is introduced to separate refractive index effects in TA spectroscopy.
Findings
Photoinduced changes in the dielectric function's real and imaginary parts are of similar magnitude.
Reflectivity effects do not significantly impact TA spectra or kinetics in 2D perovskites.
The method reconciles conflicting views in the literature on refractive index contributions.
Abstract
Two-dimensional (2D) halide perovskites are intensely researched for emerging light-emitting and -harvesting technologies due to their outstanding optoelectronic properties, strong quantum confinement, and enhanced ambient stability over their three-dimensional counterparts. A powerful technique for understanding their excited-state dynamics is transient absorption (TA) (pump–probe) spectroscopy. However, the interpretation can be complicated by simultaneous reflectivity changes arising from their high refractive index. Here, we adopt a Kramers–Kronig constrained variational analysis to disentangle these effects, as demonstrated for the prototypical Ruddlesden–Popper 2D perovskite phenylethylammonium lead iodide (PEA2PbI4). We show that photoinduced changes in the real and imaginary parts of the complex dielectric function can be of similar magnitude, but find that reflectivity effects…
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Taxonomy
TopicsPerovskite Materials and Applications · Chalcogenide Semiconductor Thin Films · Solid-state spectroscopy and crystallography