Transition Dipole Moments of n = 1, 2, and 3 Perovskite Quantum Wells from the Optical Stark Effect and Many-Body Perturbation Theory
Type
ArticleAuthors
Proppe, Andrew H.
Walters, Grant W.

Alsalloum, Abdullah Yousef

Zhumekenov, Ayan A.

Mosconi, Edoardo
Kelley, Shana O.

De Angelis, Filippo

Adamska, Lyudmyla

Umari, Paolo
Bakr, Osman

Sargent, E.

KAUST Department
Division of Physical Science and Engineering, King Abdullah University of Science and Technology, Thuwal 23955-6900, Kingdom of Saudi ArabiaFunctional Nanomaterials Lab (FuNL)
KAUST Catalysis Center (KCC)
Material Science and Engineering Program
Physical Science and Engineering (PSE) Division
Date
2020-01-14Online Publication Date
2020-01-14Print Publication Date
2020-02-06Embargo End Date
2021-01-14Submitted Date
2019-11-12Permanent link to this record
http://hdl.handle.net/10754/661070
Metadata
Show full item recordAbstract
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 PQWCitation
Proppe, 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.9b03349Sponsors
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.Publisher
American Chemical Society (ACS)Additional Links
https://pubs.acs.org/doi/10.1021/acs.jpclett.9b03349ae974a485f413a2113503eed53cd6c53
10.1021/acs.jpclett.9b03349