4.8 Article

Exciton Polarons in Two-Dimensional Hybrid Metal-Halide Perovskites

Journal

JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 11, Issue 9, Pages 3173-3184

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.9b02342

Keywords

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Funding

  1. EU Horizon 2020 via Marie Sklodowska Curie Fellowship (Global) [705874]
  2. National Science Foundation
  3. Directorate for Mathematical and Physical Sciences, Division of Materials Research [1904293, 1838276]
  4. School of Chemistry and Biochemistry
  5. College of Science of Georgia Institute of Technology
  6. Marie Curie Actions (MSCA) [705874] Funding Source: Marie Curie Actions (MSCA)

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While polarons, charges bound to a lattice deformation induced by electron- phonon coupling, are primary photoexcitations in bulk metal-halide hybrid organic- inorganic perovskites (HOIPs), excitons, Coulomb-bound electron-hole pairs, are the stable quasi-particles in their two-dimensional (2D) analogues. However, are polaronic effects consequential for excitons in 2D-HOIPs? We argue that they are manifested intrinsically in the exciton spectral structure, which is composed of multiple nondegenerate resonances with constant interpeak energy spacing. We highlight population and dephasing dynamics that point to the apparently deterministic role of polaronic effects. We contend that an interplay of long-range and short-range exciton-lattice couplings gives rise to exciton polarons, which fundamentally establishes their effective mass and radius and, consequently, their quantum dynamics. Finally, we highlight opportunities for the community to develop the rigorous description of exciton polarons in 2D-HOIPs to advance their fundamental understanding as model systems for condensed-phase materials with strong lattice-mediated correlations.

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