Exciton polaron formation and hot-carrier relaxation in rigid Dion–Jacobson-type two-dimensional perovskites

Biswas, Somnath; Zhao, Ruyan; Alowa, Fatimah; Zacharias, Marios; Sharifzadeh, Sahar; Coker, David F.; Seferos, Dwight S.; Scholes, Gregory D.

doi:10.1038/s41563-024-01895-z

Title: Exciton polaron formation and hot-carrier relaxation in rigid Dion–Jacobson-type two-dimensional perovskites

Journal Article · 15 May 2024 · Nature Materials

DOI: https://doi.org/10.1038/s41563-024-01895-z · OSTI ID:2540553

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Princeton Uiversity, NJ (United States)
University of Toronto, ON (Canada)
Boston University, MA (United States)
Université de Rennes (France)

The efficiency of two-dimensional Dion–Jacobson-type materials relies on the complex interplay between electronic and lattice dynamics; however, questions remain about the functional role of exciton–phonon interactions. Here we establish the robust polaronic nature of the excitons in these materials at room temperature by combining ultrafast spectroscopy and electronic structure calculations. We show that polaronic distortion is associated with low-frequency (30–60 cm^–1) lead iodide octahedral lattice motions. More importantly, we discover how targeted ligand modification of this two-dimensional perovskite structure manipulates exciton–phonon coupling, exciton polaron population and carrier cooling. At high excitation density, stronger exciton–phonon coupling increases the hot-carrier lifetime, forming a hot-phonon bottleneck. Furthermore, our study provides detailed insight into the exciton–phonon coupling and its role in carrier cooling in two-dimensional perovskites relevant for developing emerging hybrid semiconductor materials with tailored properties.

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Research Organization:: Boston University, MA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0015429; SC0018080; SC0020437; SC0023402

OSTI ID:: 2540553

Journal Information:: Nature Materials, Journal Name: Nature Materials Journal Issue: 7 Vol. 23; ISSN 1476-1122

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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