Mechanistic Understanding and Rational Design of Quantum Dot/Mediator Interfaces for Efficient Photon Upconversion

Xu, Zihao; Huang, Zhiyuan; Jin, Tao; Lian, Tianquan; Tang, Ming L.

doi:10.1021/acs.accounts.0c00526

Title: Mechanistic Understanding and Rational Design of Quantum Dot/Mediator Interfaces for Efficient Photon Upconversion

Journal Article · Tue Nov 03 00:00:00 EST 2020 · Accounts of Chemical Research

DOI:https://doi.org/10.1021/acs.accounts.0c00526· OSTI ID:1773894

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^[2]; Jin, Tao ^[1];

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Emory Univ., Atlanta, GA (United States)
Univ. of California, Riverside, CA (United States)

The semiconductor-nanocrystal-sensitized, three-component upconversion system has made great strides over the past 5 years. The three components (i.e., triplet photosensitizer, mediator, and emitter) each play critical roles in determining the input and output photon energy and overall quantum efficiency (QE). The nanocrystal photosensitizer converts the absorbed photon into singlet excitons and then triplet excitons via intersystem crossing. The mediator accepts the triplet exciton via either direct Dexter-type triplet energy transfer (TET) or sequential charge transfer (CT) while extending the exciton lifetime. Through a second triplet energy-transfer step from the mediator to the emitter, the latter is populated in its lowest excited triplet state. Triplet–triplet annihilation (TTA) between two triplet emitters generates the emitter in its bright singlet state, which then emits the upconverted photon. Quantum dots (QD) have a tunable band gap, large extinction coefficient, and small singlet–triplet energy losses compared to metal–ligand charge-transfer complexes. This high triplet exciton yield makes QDs good candidates for photosensitizers. In terms of driving triplet energy transfer, the triplet energy of the mediator should be slightly lower than the triplet exciton energy of the QD sensitizer for a downhill energy landscape with minimal energy loss. The same energy cascade is also required for the transfer from the mediator to the emitter. Lastly, the triplet energy of the emitter must be slightly larger than one-half of its singlet energy to ensure that TTA is exothermic. Optimization of the sensitizer, mediator, and emitter will lead to an increase in the anti-Stokes shift and the total quantum efficiency. Evaluating each individual step’s efficiency and kinetics is necessary for the understanding of the limiting factors in existing systems.

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Research Organization:: Univ. of California, Riverside, CA (United States)

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

Grant/Contract Number:: SC0018969; SC0008798

OSTI ID:: 1773894

Journal Information:: Accounts of Chemical Research, Vol. 54, Issue 1; ISSN 0001-4842

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Quantum dots
Charge transfer
Luminescence
Energy transfer
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Title: Mechanistic Understanding and Rational Design of Quantum Dot/Mediator Interfaces for Efficient Photon Upconversion

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