Transition Dipole Moments of n = 1, 2, and 3 Perovskite Quantum Wells from the Optical Stark Effect and Many-Body Perturbation Theory

Andrew H. Proppe, Grant W. Walters, Abdullah Yousef Alsalloum, Ayan A. Zhumekenov, Edoardo Mosconi, Shana O. Kelley, Filippo De Angelis, Lyudmyla Adamska, Paolo Umari, Osman Bakr, E. Sargent

Research output: Contribution to journalArticlepeer-review

24 Scopus citations

Abstract

Metal halide perovskite quantum wells (PQWs) are quantum and dielectrically confined materials exhibiting strongly bound excitons. The exciton transition dipole moment dictates absorption strength and influences interwell coupling in dipole-mediated energy transfer, a process that influences the performance of PQW optoelectronic devices. Here we use transient reflectance spectroscopy with circularly polarized laser pulses to investigate the optical Stark effect in dimensionally pure single crystals of n = 1, 2, and 3 Ruddlesden-Popper PQWs. From these measurements, we extract in-plane transition dipole moments of 11.1 (±0.4), 9.6 (±0.6) and 13.0 (±0.8) D for n = 1, 2 and 3, respectively. We corroborate our experimental results with density functional and many-body perturbation theory calculations, finding that the nature of band edge orbitals and exciton wave function delocalization depends on the PQW
Original languageEnglish (US)
Pages (from-to)716-723
Number of pages8
JournalThe Journal of Physical Chemistry Letters
Volume11
Issue number3
DOIs
StatePublished - Jan 15 2020

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: This publication is based on work supported by the United States Department of the Navy, Office of Naval Research (Grant Award No.: N00014-17-1-2524). A. H. P. and G. W. W. acknowledge support from the Natural Sciences and Engineering Research Council of Canada (NSERC). E.M. and F.D.A acknowledge European Union’s Horizon 2020 research and innovation programme under Grant Agreement No. 764047 of the ESPRESSO project. The Ministero dell’Istruzione dell’Università e della Ricerca (MIUR) and Università degli Studi di Perugia are acknowledged for financial support through the program “Dipartimenti di Eccellenza 2018-2022” (Grant AMIS). L.A. and P.U. acknowledge PRACE (Project ID 20171633963) for awarding access to Marconi at CINECA, Italy.

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