Transition Dipole Moments of n = 1, 2, and 3 Perovskite Quantum Wells from the Optical Stark Effect and Many-Body Perturbation Theory
AuthorsProppe, Andrew H.
Walters, Grant W.
Alsalloum, Abdullah Yousef
Zhumekenov, Ayan A.
Kelley, Shana O.
De Angelis, Filippo
KAUST DepartmentDivision of Physical Science and Engineering, King Abdullah University of Science and Technology, Thuwal 23955-6900, Kingdom of Saudi Arabia
Functional Nanomaterials Lab (FuNL)
KAUST Catalysis Center (KCC)
Material Science and Engineering Program
Physical Science and Engineering (PSE) Division
Online Publication Date2020-01-14
Print Publication Date2020-02-06
Embargo End Date2021-01-14
Permanent link to this recordhttp://hdl.handle.net/10754/661070
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AbstractMetal 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
CitationProppe, A. H., Walters, G. W., Alsalloum, A. Y., Zhumekenov, A. A., Mosconi, E., Kelley, S. O., … Sargent, E. H. (2020). Transition Dipole Moments of n = 1, 2, and 3 Perovskite Quantum Wells from the Optical Stark Effect and Many-Body Perturbation Theory. The Journal of Physical Chemistry Letters, 716–723. doi:10.1021/acs.jpclett.9b03349
SponsorsThis 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.
PublisherAmerican Chemical Society (ACS)