Longer Cations Increase Energetic Disorder in Excitonic 2D Hybrid Perovskites

The Journal of Physical Chemistry Letters
Daniel B StrausCherie R Kagan

Abstract

We synthesize and characterize derivatives of the two-dimensional hybrid perovskite (2DHP) phenethylammonium lead iodide ((PEA)2PbI4) in which the para H on the cation is replaced with F, Cl, CH3, or Br. These substitutions increase the length of the cation but leave the cross-sectional area unchanged, resulting in structurally similar PbI42- frameworks with increasing interlayer spacing. Longer cations result in broader, blue-shifted excitonic absorption spectra with reduced or eliminated structure, indicating greater energetic disorder. Photoluminescence spectra are largely invariant and insensitive to cation length, suggesting polaron formation stabilizes a structural and electronic minimum. Temperature-dependent line width analysis reveals excitons couple to a vibration on the organic framework that is weakly sensitive to these cation substitutions, and Raman spectra and electronic structure calculations support the presence of such a cationic mode. Despite carriers being confined to the inorganic framework, the length of the organic cation alters the optical and electronic properties of 2DHPs.

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Citations

Feb 9, 2021·The Journal of Physical Chemistry Letters·Mateusz DyksikPaulina Plochocka
Jun 17, 2021·Proceedings of the National Academy of Sciences of the United States of America·Li Na QuanPeidong Yang
Jul 7, 2021·ACS Applied Materials & Interfaces·Miriam KarpińskaPaulina Plochocka
Aug 19, 2021·The Journal of Physical Chemistry Letters·Wenbi Shcherbakov-WuWilliam A Tisdale
Jul 1, 2020·The Journal of Physical Chemistry Letters·Joanna M UrbanMichal Baranowski
Jan 7, 2020·The Journal of Physical Chemistry Letters·Ziren ZhouHua Gui Yang
Nov 13, 2020·The Journal of Physical Chemistry Letters·David FeldsteinErmin Malic
Jan 15, 2021·Journal of the American Chemical Society·Michael A HopeLyndon Emsley
Nov 4, 2021·Journal of the American Chemical Society·Qi SunShengye Jin
Nov 11, 2021·Science Advances·Mateusz DyksikPaulina Plochocka

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