Directing Energy Transfer in Halide Perovskite–Chromophore Hybrid Assemblies

DuBose, Jeffrey T.; Kamat, Prashant V.

doi:10.1021/jacs.1c09867

Directing Energy Transfer in Halide Perovskite–Chromophore Hybrid Assemblies

Journal Article · Tue Nov 02 00:00:00 EDT 2021 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.1c09867· OSTI ID:1830686

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Univ. of Notre Dame, IN (United States); Univ of Notre Dame
Univ. of Notre Dame, IN (United States)

Directing the flow of energy and the nature of the excited states that are produced in nanocrystal–chromophore hybrid assemblies is crucial for realizing their photocatalytic and optoelectronic applications. Using a combination of steady-state and time-resolved absorption and photoluminescence (PL) experiments, we have probed the excited-state interactions in the CsPbBr₃–Rhodamine B (RhB) hybrid assembly. PL studies reveal quenching of the CsPbBr₃ emission with a concomitant enhancement of the fluorescence of RhB, indicating a singlet-energy-transfer mechanism. Transient absorption spectroscopy shows that this energy transfer occurs on the ~200 ps time scale. To understand whether the energy transfer occurs through a Förster or Dexter mechanism, we leveraged facile halide-exchange reactions to tune the optical properties of the donor CsPbBr₃ by alloying with chloride. This allowed us to tune the spectral overlap between the donor CsPb(Br_1–xCl_x)₃ emission and acceptor RhB absorption. For CsPbBr₃-RhB, the rate constant for energy transfer (k_ET) agrees well with Förster theory, whereas alloying with chloride to produce chloride-rich CsPb(Br_1–xCl_x)₃ favors a Dexter mechanism. These results highlight the importance of optimizing both the donor and acceptor properties to design light-harvesting assemblies that employ energy transfer. Furthermore, the ease of tuning optical properties through halide exchange of the nanocrystal donor provides a unique platform for studying and tailoring excited-state interactions in perovskite–chromophore assemblies.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Notre Dame, IN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FC02-04ER15533

OSTI ID:: 1830686

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 45 Vol. 143; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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