Lanthanide-doped inorganic nanoparticles turn molecular triplet excitons bright

Han, Sanyang; Deng, Renren; Gu, Qifei; Ni, Limeng; Huynh, Uyen; Zhang, Jiangbin; Yi, Zhigao; Zhao, Baodan; Tamura, Hiroyuki; Pershin, Anton; Xu, Hui; Huang, Zhiyuan; Ahmad, Shahab; Abdi-Jalebi, Mojtaba; Sadhanala, Aditya; Tang, Ming Lee; Bakulin, Artem A.; Beljonne, David; Liu, Xiaogang; Rao, Akshay

doi:10.1038/s41586-020-2932-2

Cited by 165 publications

(158 citation statements)

References 40 publications

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“…3b and Supplementary Fig. 15 ), 198 times faster than that obtained from pristine CPPOA (18.4 ns) 57 . Decay of the T 1 state has a constant 10.6 ns (Fig.…”

Section: Resultsmentioning

confidence: 82%

“…Cation-exchange reactions allow a large portion of lanthanide emitters to be exposed at nanoparticle surfaces, enabling direct bonding between surface emitters and capping molecules. Unlike the Tm 3+ -to-CPPOA energy transfer described above, we reasoned that strong exchange coupling dominates energy transfer between molecules and surface lanthanide emitters (e.g., Tb 3+ ) because their proximity results in fast triplet generation of molecules and efficient triplet energy transfer from molecules to lanthanide emitters 57 . To validate this hypothesis, we next performed ultrafast transient absorption spectroscopy to probe the photodynamics of excitation energy at the interface of CPPOA and Tb 3+ -exchanged multilayer nanoparticles.…”

Section: Resultsmentioning

confidence: 94%

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Photon upconversion through triplet exciton-mediated energy relay

Han

Zhang

et al. 2021

Nat Commun

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Exploration of upconversion luminescence from lanthanide emitters through energy migration has profound implications for fundamental research and technology development. However, energy migration-mediated upconversion requires stringent experimental conditions, such as high power excitation and special migratory ions in the host lattice, imposing selection constraints on lanthanide emitters. Here we demonstrate photon upconversion of diverse lanthanide emitters by harnessing triplet exciton-mediated energy relay. Compared with gadolinium-based systems, this energy relay is less dependent on excitation power and enhances the emission intensity of Tb3+ by 158-fold. Mechanistic investigations reveal that emission enhancement is attributable to strong coupling between lanthanides and surface molecules, which enables fast triplet generation (<100 ps) and subsequent near-unity triplet transfer efficiency from surface ligands to lanthanides. Moreover, the energy relay approach supports long-distance energy transfer and allows upconversion modulation in microstructures. These findings enhance fundamental understanding of energy transfer at molecule-nanoparticle interfaces and open exciting avenues for developing hybrid, high-performance optical materials.

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“…3b and Supplementary Fig. 15 ), 198 times faster than that obtained from pristine CPPOA (18.4 ns) 57 . Decay of the T 1 state has a constant 10.6 ns (Fig.…”

Section: Resultsmentioning

confidence: 82%

Section: Resultsmentioning

confidence: 94%

Photon upconversion through triplet exciton-mediated energy relay

Han

Zhang

et al. 2021

Nat Commun

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“…Functionalization of UCNPs with organic molecules or quantum dots has become a popular strategy to improving upconversion efficiency [105,106] . These photosensitizers exhibit broad absorption bands and extinction coefficients orders of magnitude higher than those of lanthanide sensitizers.…”

Section: Strategies For Enhancing Upconversion Luminescencementioning

confidence: 99%

Multiphoton Upconversion Materials for Photocatalysis and Environmental Remediation

Chan

et al. 2021

Chemistry An Asian Journal

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Solar‐driven photocatalysis holds great potential for energy conversion, environmental remediation, and sustainable chemistry. However, practical applications of conventional photocatalytic systems have been constrained by their insufficient ability to harvest solar radiation in the infrared spectrum. Lanthanide‐doped upconversion materials possess high photostability, tunable absorption, and the ability to convert low‐energy infrared radiation into high‐energy emission, making them attractive for infrared‐driven photocatalysis. This review highlights essential principles for rational design of efficient photocatalysts. Particular emphasis is placed on current state‐of‐the‐arts that offer enhanced upconversion luminescence efficiency. We also summarize recent advances in lanthanide‐doped upconversion materials for photocatalysis. We conclude with new challenges and prospects for future developments of infrared‐driven photocatalysts.

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“…1a), where the halogen atom effect matters. This work provides another vivid example of engineering of triplet excitons to realize unconventional photophysical properties in organic systems [8][9][10][11][12] .…”

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confidence: 99%