Interfacial Trap‐Assisted Triplet Generation in Lead Halide Perovskite Sensitized Solid‐State Upconversion

Photon upconversion via triplet–triplet annihilation (TTA) has promise for overcoming the Shockley–Queisser limit for single-junction solar cells by allowing the utilization of sub-bandgap photons. Recently, bulk perovskites have been employed as sensitizers in solid-state upconversion devices to ci...

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Main Authors: Wang, Lili, Yoo, Jason J., Lin, Ting‐An, Perkinson, Collin F., Lu, Yongli, Baldo, Marc A., Bawendi, Moungi G.
Other Authors: Massachusetts Institute of Technology. Department of Chemistry
Format: Article
Language:English
Published: Wiley 2022
Online Access:https://hdl.handle.net/1721.1/140348
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author Wang, Lili
Yoo, Jason J.
Lin, Ting‐An
Perkinson, Collin F.
Lu, Yongli
Baldo, Marc A.
Bawendi, Moungi G.
author2 Massachusetts Institute of Technology. Department of Chemistry
author_facet Massachusetts Institute of Technology. Department of Chemistry
Wang, Lili
Yoo, Jason J.
Lin, Ting‐An
Perkinson, Collin F.
Lu, Yongli
Baldo, Marc A.
Bawendi, Moungi G.
author_sort Wang, Lili
collection MIT
description Photon upconversion via triplet–triplet annihilation (TTA) has promise for overcoming the Shockley–Queisser limit for single-junction solar cells by allowing the utilization of sub-bandgap photons. Recently, bulk perovskites have been employed as sensitizers in solid-state upconversion devices to circumvent poor exciton diffusion in previous nanocrystal (NC)-sensitized devices. However, an in-depth understanding of the underlying photophysics of perovskite-sensitized triplet generation is still lacking due to the difficulty of precisely controlling interfacial properties of fully solution-processed devices. In this study, interfacial properties of upconversion devices are adjusted by a mild surface solvent treatment, specifically altering perovskite surface properties without perturbing the bulk perovskite. Thermal evaporation of the annihilator precludes further solvent contamination. Counterintuitively, devices with more interfacial traps show brighter upconversion. Approximately an order of magnitude difference in upconversion brightness is observed across different interfacial solvent treatments. Sequential charge transfer and interfacial trap-assisted triplet sensitization are demonstrated by comparing upconversion performance, transient photoluminescence dynamics, and magnetic field dependence of the devices. Incomplete triplet conversion from transferred charges and consequent triplet-charge annihilation (TCA) are also observed. The observations highlight the importance of interfacial control and provide guidance for further design and optimization of upconversion devices using perovskites or other semiconductors as sensitizers.
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spelling mit-1721.1/1403482024-06-06T19:44:22Z Interfacial Trap‐Assisted Triplet Generation in Lead Halide Perovskite Sensitized Solid‐State Upconversion Wang, Lili Yoo, Jason J. Lin, Ting‐An Perkinson, Collin F. Lu, Yongli Baldo, Marc A. Bawendi, Moungi G. Massachusetts Institute of Technology. Department of Chemistry Massachusetts Institute of Technology. Department of Electrical Engineering and Computer Science Photon upconversion via triplet–triplet annihilation (TTA) has promise for overcoming the Shockley–Queisser limit for single-junction solar cells by allowing the utilization of sub-bandgap photons. Recently, bulk perovskites have been employed as sensitizers in solid-state upconversion devices to circumvent poor exciton diffusion in previous nanocrystal (NC)-sensitized devices. However, an in-depth understanding of the underlying photophysics of perovskite-sensitized triplet generation is still lacking due to the difficulty of precisely controlling interfacial properties of fully solution-processed devices. In this study, interfacial properties of upconversion devices are adjusted by a mild surface solvent treatment, specifically altering perovskite surface properties without perturbing the bulk perovskite. Thermal evaporation of the annihilator precludes further solvent contamination. Counterintuitively, devices with more interfacial traps show brighter upconversion. Approximately an order of magnitude difference in upconversion brightness is observed across different interfacial solvent treatments. Sequential charge transfer and interfacial trap-assisted triplet sensitization are demonstrated by comparing upconversion performance, transient photoluminescence dynamics, and magnetic field dependence of the devices. Incomplete triplet conversion from transferred charges and consequent triplet-charge annihilation (TCA) are also observed. The observations highlight the importance of interfacial control and provide guidance for further design and optimization of upconversion devices using perovskites or other semiconductors as sensitizers. 2022-02-15T13:47:58Z 2022-02-15T13:47:58Z 2021-05-28 Article http://purl.org/eprint/type/JournalArticle 0935-9648 1521-4095 https://hdl.handle.net/1721.1/140348 Wang, L., Yoo, J. J., Lin, T.-A., Perkinson, C. F., Lu, Y., Baldo, M. A., Bawendi, M. G., Interfacial Trap-Assisted Triplet Generation in Lead Halide Perovskite Sensitized Solid-State Upconversion. Adv. Mater. 2021, 33, 2100854 en http://dx.doi.org/10.1002/adma.202100854 Advanced Materials Creative Commons Attribution-Noncommercial-Share Alike http://creativecommons.org/licenses/by-nc-sa/4.0/ application/pdf Wiley Wiley
spellingShingle Wang, Lili
Yoo, Jason J.
Lin, Ting‐An
Perkinson, Collin F.
Lu, Yongli
Baldo, Marc A.
Bawendi, Moungi G.
Interfacial Trap‐Assisted Triplet Generation in Lead Halide Perovskite Sensitized Solid‐State Upconversion
title Interfacial Trap‐Assisted Triplet Generation in Lead Halide Perovskite Sensitized Solid‐State Upconversion
title_full Interfacial Trap‐Assisted Triplet Generation in Lead Halide Perovskite Sensitized Solid‐State Upconversion
title_fullStr Interfacial Trap‐Assisted Triplet Generation in Lead Halide Perovskite Sensitized Solid‐State Upconversion
title_full_unstemmed Interfacial Trap‐Assisted Triplet Generation in Lead Halide Perovskite Sensitized Solid‐State Upconversion
title_short Interfacial Trap‐Assisted Triplet Generation in Lead Halide Perovskite Sensitized Solid‐State Upconversion
title_sort interfacial trap assisted triplet generation in lead halide perovskite sensitized solid state upconversion
url https://hdl.handle.net/1721.1/140348
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