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

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    Type
    Article
    Authors
    Proppe, Andrew H. cc
    Walters, Grant W. cc
    Alsalloum, Abdullah Yousef cc
    Zhumekenov, Ayan A. cc
    Mosconi, Edoardo
    Kelley, Shana O. cc
    De Angelis, Filippo cc
    Adamska, Lyudmyla cc
    Umari, Paolo
    Bakr, Osman cc
    Sargent, E. cc
    KAUST Department
    Division 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
    Date
    2020-01-14
    Online Publication Date
    2020-01-14
    Print Publication Date
    2020-02-06
    Embargo End Date
    2021-01-14
    Submitted Date
    2019-11-12
    Permanent link to this record
    http://hdl.handle.net/10754/661070
    
    Metadata
    Show full item record
    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
    Citation
    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.9b03349
    Sponsors
    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)
    Journal
    The Journal of Physical Chemistry Letters
    DOI
    10.1021/acs.jpclett.9b03349
    Additional Links
    https://pubs.acs.org/doi/10.1021/acs.jpclett.9b03349
    ae974a485f413a2113503eed53cd6c53
    10.1021/acs.jpclett.9b03349
    Scopus Count
    Collections
    Articles; Physical Science and Engineering (PSE) Division; Material Science and Engineering Program; KAUST Catalysis Center (KCC)

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