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

Abstract

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.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [4]; ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [5];  [6]; ORCiD logo [7]; ORCiD logo [1]; ORCiD logo [2]
  1. Univ. of Toronto, ON (Canada)
  2. Princeton Univ., NJ (United States)
  3. Netherlands eScience Center, Amsterdam (Netherlands)
  4. Univ. of Electronic Science and Technology of China, Chengdu (China); Univ. of Quebec (Canada)
  5. Ohio Univ., Athens, OH (United States)
  6. Argonne National Lab. (ANL), Lemont, IL (United States)
  7. Vrije Univ., Amsterdam (Netherlands)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Lemont, IL (United States)
Sponsoring Org.:
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)
OSTI Identifier:
1557832
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 10; Journal Issue: 3; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; carrier dynamics; dynamics; energy transfer; layered perovskite; metal halide perovskite; two-dimensional electronic spectroscopy

Citation Formats

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., and Scholes, Gregory D. Spectrally Resolved Ultrafast Exciton Transfer in Mixed Perovskite Quantum Wells. United States: N. p., 2019. Web. doi:10.1021/acs.jpclett.9b00018.
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. Spectrally Resolved Ultrafast Exciton Transfer in Mixed Perovskite Quantum Wells. United States. doi:10.1021/acs.jpclett.9b00018.
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., and Scholes, Gregory D. Thu . "Spectrally Resolved Ultrafast Exciton Transfer in Mixed Perovskite Quantum Wells". United States. doi:10.1021/acs.jpclett.9b00018.
@article{osti_1557832,
title = {Spectrally Resolved Ultrafast Exciton Transfer in Mixed Perovskite Quantum Wells},
author = {Proppe, Andrew H. and Elkins, Madeline H. and Voznyy, Oleksandr and Pensack, Ryan D. and Zapata, Felipe and Besteiro, Lucas V. and Quan, Li Na and Quintero-Bermudez, Rafael and Todorovic, Petar and Kelley, Shana O. and Govorov, Alexander O. and Gray, Stephen K. and Infante, Ivan and Sargent, Edward H. and Scholes, Gregory D.},
abstractNote = {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.},
doi = {10.1021/acs.jpclett.9b00018},
journal = {Journal of Physical Chemistry Letters},
number = 3,
volume = 10,
place = {United States},
year = {2019},
month = {1}
}

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