4.8 Article

Excitonic Effects in Methylammonium Lead Halide Perovskites

Journal

JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 9, Issue 10, Pages 2595-2603

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.8b00526

Keywords

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Funding

  1. Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, Office of Science within the U.S. Department of Energy [DE-AC36-08G028308]
  2. LDRD project

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The exciton binding energy in methylammonium lead iodide (MAPbI(3)) is about 10 meV, around 1/3 of the available thermal energy (k(B)T similar to 26 meV) at room temperature. Thus, exciton populations are not stable at room temperature at moderate photoexcited carrier densities. However, excitonic resonances dominate the absorption onset. Furthermore, these resonances determine the transient absorbance and transient reflectance spectra. The exciton binding energy is a reflection of the Coulomb interaction energy between photoexcited electrons and holes. As such, it serves as a marker for the strength of electron/hole interactions and impacts a variety of phenomena, such as, absorption, radiative recombination, and Auger recombination. In this Perspective, we discuss the role of excitons and excitonic resonances in the optical properties of lead-halide perovskite semiconductors. Finally, we discuss how the strong light-matter interactions induce an optical stark effect splitting the doubly spin degenerate ground exciton states and are easily observed at room temperature.

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