Highly near-IR emissive ytterbium(<scp>iii</scp>) complexes with unprecedented quantum yields

Hu, Jiyun; Ning, Yingying; Meng, Yin‐Shan; Zhang, Jing; Wu, Zhongzhen; Gao, Song; Zhang, Junlong

doi:10.1039/c6sc05021b

Cited by 151 publications

(100 citation statements)

References 79 publications

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“…The efficiency of NIR OLEDs is currently limited by the low PLQY of lanthanide complexes, since the NIR transition could be deactivated even by C–H vibration. In recent years, some work demonstrated that the luminescence efficiency of NIR lanthanide complexes could be greatly improved by using deuterated and fluorinated ligands . This strategy even suits for the lanthanide which has scattered spectrum to enhance the emission efficiency of visible light .…”

Section: Conclusion and Prospectsmentioning

confidence: 99%

Review on the Electroluminescence Study of Lanthanide Complexes

Wang

Zhao

Chen

et al. 2019

Advanced Optical Materials

136

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Section: Conclusion and Prospectsmentioning

confidence: 99%

Review on the Electroluminescence Study of Lanthanide Complexes

Wang

Zhao

Chen

et al. 2019

Advanced Optical Materials

136

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“…4 Similarly, for an organic solar cell (OSC) k fl and k nr determine the exciton lifetime and thereby the probability that an exciton generates charge carriers. 5 These k nr 's are important in many other fields, including: phosphorescent OLEDs, [6][7][8] biomedical labeling, [9][10][11] photodynamic therapy, 12-14 laser dyes, [15][16][17] and luminescent solar concentrators. [18][19][20] In reality, the prediction of quantum yields (Φ) has been very difficult.…”

Section: Introductionmentioning

confidence: 99%

Toward Prediction of Nonradiative Decay Pathways in Organic Compounds I: The Case of Naphthalene Quantum Yields

2019

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Many emerging technologies depend on human's ability to control and manipulate the excited-state properties of molecular systems. These technologies include fluorescent labeling in biomedical imaging, light harvesting in photovoltaics, and electroluminescence in light-emitting devices. All of these systems suffer from non-radiative loss pathways that dissipate electronic energy as heat, which causes the overall system efficiency to be directly linked to quantum yield (Φ) of the molecular excited state. Unfortunately, Φ is very difficult to predict from first principles because the description of a slow non-radiative decay mechanism requires an accurate description of long-timescale excited-state quantum dynamics. In the present study, we introduce an efficient semiempirical method of calculating the fluorescence quantum yield (Φ fl) for molecular chromophores, which, based on machine learning, converts simple electronic energies computed using time-dependent density functional theory (TDDFT) into an estimate of Φ fl. As with all machine learning strategies, the algorithm needs to be trained on fluorescent dyes for which Φ fl 's are known, so as to provide a black-box method which can later predict Φ's for chemically similar chromophores that have not been studied experimentally. As a first illustration of how our proposed algorithm can be trained, we examine a family of 25 naphthalene derivatives. The simplest application of the energy gap law is found to be inadequate to explain the rates of internal conversion (IC) or intersystem crossing (ISC)-the electronic properties of at least one higher-lying electronic state (S n or T n) or one far-from-equilibrium geometry are typically needed to obtain accurate results. Indeed, the key descriptors turn out to be the transition state between the Franck-Condon minimum a distorted local minimum near an S 0 /S 1 conical intersection (which governs IC) and the magnitude of the spin-orbit coupling (which governs ISC). The resulting Φ fl 's are predicted with reasonable accuracy (± 22%), making our approach a promising ingredient for high-throughput screening and rational design of the molecular excited states with desired Φ's. We thus conclude that our model, while semi-empirical in nature, does in fact extract sound physical insight into the challenge of describing non-radiative relaxations.

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“…Organic dyes and complexes 9 have long been employed as sensitizing agents for Ln ion transitions, with photoluminescent quantum yields (PLQYs)of 75% being reported. 10 Though the absorption of the Ln ions is improved with these materials, they still do not offer a broad band absorption profile or the level of control that is necessary for achieving very high (>95%) PLQYs. Due to the lack of a protective shell in the materials, nonradiative quenching processes are present and can have a large impact on the PLQY of the material.…”

Section: Introductionmentioning

confidence: 99%

Broadband Sensitization of Lanthanide Emission with Indium Phosphide Quantum Dots for Visible to Near-Infrared Downshifting

et al. 2018

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Semiconductor quantum dot (QD)-sensitized lanthanide ions hold great promise in producing a broadly absorbing and sharply emitting luminophore, but their synthesis has proven to be difficult. We report the first synthesis of core/shell/shell InP/Ln YF/ShF (Ln = Yb, Nd; Sh = Lu, Y) nanocrystals that exhibit a broad visible absorption coupled to a sharp near-infrared emission. Additionally, this is the first report of Nd being coupled to a QD absorber. We characterize the system with a variety of electron microscopy and X-ray techniques that prove this unique structure. Optical measurements confirm the correlation of the Ln emission to the QD absorption, while the presence of a trap-state emission gives a clue as to the mechanism of energy transfer between the dot and the lanthanide.

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Highly near-IR emissive ytterbium(iii) complexes with unprecedented quantum yields

Abstract: We report a series of highly NIR emissive Yb complexes, in which the Yb is sandwiched between an octafluorinated porphyrinate antenna ligand and a deuterated Kläui ligand, and one of the complexes has an unprecedented quantum yield of 63%.

Cited by 151 publications

References 79 publications

Review on the Electroluminescence Study of Lanthanide Complexes

Review on the Electroluminescence Study of Lanthanide Complexes

Toward Prediction of Nonradiative Decay Pathways in Organic Compounds I: The Case of Naphthalene Quantum Yields

Broadband Sensitization of Lanthanide Emission with Indium Phosphide Quantum Dots for Visible to Near-Infrared Downshifting

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