Spectrally Resolved Ultrafast Exciton Transfer in Mixed Perovskite Quantum Wells

Proppe, Andrew H.; Elkins, Madeline H.; Voznyy, Oleksandr; Pensack, Ryan D.; Zapata, Felipe; Besteiro, Lucas V.; Quan, Li Na; Quintero-Bermudez, Rafael; Todorovic, Petar; Kelley, Shana O.; Govorov, Alexander O.; Gray, Stephen K.; Infante, Ivan; Sargent, Edward H.; Scholes, Gregory D.

doi:10.1021/acs.jpclett.9b00018

Title: Spectrally Resolved Ultrafast Exciton Transfer in Mixed Perovskite Quantum Wells

Journal Article · 10 January 2019 · Journal of Physical Chemistry Letters

DOI: https://doi.org/10.1021/acs.jpclett.9b00018 · OSTI ID:1557832

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Univ. of Toronto, ON (Canada)
Princeton Univ., NJ (United States)
Netherlands eScience Center, Amsterdam (Netherlands)
Univ. of Electronic Science and Technology of China, Chengdu (China); Univ. of Quebec (Canada)
Ohio Univ., Athens, OH (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Vrije Univ., Amsterdam (Netherlands)

Solution-processed perovskite quantum wells have been utilized to fabricate increasingly efficient and stable optoelectronic devices. Little is known about the dynamics of photogenerated excitons in perovskite quantum wells within the first few hundred femtoseconds-a crucial time scale on which energy and charge transfer processes may compete. In this work we use ultrafast transient absorption and two-dimensional electronic spectroscopy to clarify the movement of excitons and charges in reduced-dimensional perovskite solids. We report excitonic funneling from strongly to weakly confined perovskite quantum wells within 150 fs, facilitated by strong spectral overlap and orientational alignment among neighboring wells. This energy transfer happens on time scales orders of magnitude faster than charge transfer, which we find to occur instead over 10s to 100s of picoseconds. Simulations of both Forster-type interwell exciton transfer and free carrier charge transfer are in agreement with these experimental results, with theoretical exciton transfer calculated to occur in 100s of femtoseconds.

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Research Organization:: Argonne National Laboratory (ANL), Lemont, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division; Natural Sciences and Engineering Research Council of Canada (NSERC); Netherlands Organisation for Scientific Research (NWO); Canadian Institute for Advanced Research (CIFAR)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1557832

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 3 Vol. 10; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
carrier dynamics
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Title: Spectrally Resolved Ultrafast Exciton Transfer in Mixed Perovskite Quantum Wells

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