Photoinduced Radical Emission in a Coassembly System

Li, Yiran; Baryshnikov, Glib; Xu, Chenchen; Ågren, Hans; Zhu, Liangliang; Yi, Tao; Zhao, Yanli; Wu, Hongwei

doi:10.1002/anie.202110405

Cited by 53 publications

(81 citation statements)

References 63 publications

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“…Theoretical calculations and experimental results suggest that the shortwavelength emission in the current radicals can be attributed to anti-Kasha's rule behavior, in which the emission originates from the relatively high excited states (D 3 /D 2 ) to D 0 (Fig. 1b) [19][20][21][22][23][24] . This kind of radical is advantageous because they have a wide bandgap, and they exhibit blue-shifted absorption and emission.…”

Section: Introductionmentioning

confidence: 91%

A Platform for Blue-Luminescent Carbon-Centered Radicals

Li¹,

Wang²,

Chen³

et al. 2022

Preprint

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Organic radicals, which have unique doublet spin-configuration, provide an alternative method to overcome the efficiency limitation of organic light-emitting diodes (OLEDs) based on conventional fluorescent organic mole-cules. Further, they have made great breakthroughs in deep-red and near-infrared OLEDs. However, it is diffi-cult to extend their fluorescence into a short-wavelength region because of the natural narrow bandgap of the organic radicals. Herein, we significantly expand the scope of luminescent radicals by showing a new platform of carbon-centered radicals derived from N-heterocyclic carbenes that produce blue to green emissions (444–529 nm). Time-dependent density functional theory calculations and experimental investigations disclose that the fluorescence originates from the high-energy excited states to the ground state, demonstrating an anti-Kasha behavior. The present work provides an efficient and modular approach toward a library of carbon-centered radicals that feature anti-Kasha's rule emission, rendering them as potential new emitters in the short-wavelength region.

show abstract

Section: Introductionmentioning

confidence: 91%

A Platform for Blue-Luminescent Carbon-Centered Radicals

Li¹,

Wang²,

Chen³

et al. 2022

Preprint

View full text Add to dashboard Cite

show abstract

“…Theoretical calculations and experimental results suggest that the short-wavelength emission in the current radicals can be attributed to anti-Kasha's rule behavior, in which the emission originates from the relatively high excited states (D 3 /D 2 ) to D 0 (Fig. 1b) [19][20][21][22][23][24] . This kind of radical is advantageous because they have a wide bandgap, and they exhibit blue-shifted absorption and emission.…”

mentioning

confidence: 90%

A platform for blue-luminescent carbon-centered radicals

Wang

Chen

et al. 2022

Nat Commun

View full text Add to dashboard Cite

Organic radicals, which have unique doublet spin-configuration, provide an alternative method to overcome the efficiency limitation of organic light-emitting diodes (OLEDs) based on conventional fluorescent organic molecules. Further, they have made great breakthroughs in deep-red and near-infrared OLEDs. However, it is difficult to extend their fluorescence into a short-wavelength region because of the natural narrow bandgap of the organic radicals. Herein, we significantly expand the scope of luminescent radicals by showing a new platform of carbon-centered radicals derived from N-heterocyclic carbenes that produce blue to green emissions (444–529 nm). Time-dependent density functional theory calculations and experimental investigations disclose that the fluorescence originates from the high-energy excited states to the ground state, demonstrating an anti-Kasha behavior. The present work provides an efficient and modular approach toward a library of carbon-centered radicals that feature anti-Kasha’s rule emission, rendering them as potential new emitters in the short-wavelength region.

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“…[1][2][3][4][5] Due to the unique magnetic, electronic, and optical properties, organic radicals play important roles in molecular magnets, [6] electronic devices, [7][8][9] catalysis, [10][11][12][13] photochemistry. [14][15][16][17][18][19] In particular, radicalcontaining frameworks (RCFs), such as radicals incorporated in covalent organic frameworks (COFs) and metal organic frameworks (MOFs), have emerged as promising functional materials in gas adsorption, [20] photoluminescence, [21] photothermal therapy, [22][23][24][25] catalysis, [26,27] and magnetism. [28,29] However, organic radicals are not easily existing stable due to their unpaired valence electron, to further constructing them into ordered frame structure may face more difficult challenges, such as designing radical containing ligands, keeping organic radicals stable during synthesis, avoiding electrostatic repulsion of the organic radicals.…”

Section: Introductionmentioning

confidence: 99%

Chaotropic Effect Stabilized Radical‐Containing Supramolecular Organic Frameworks for Photothermal Therapy

Chen

Shen

et al. 2022

Small

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Radical‐containing frameworks (RCFs) have emerged as promising functional materials in various fields due to the combination of the highly ordered frame structure and the fascinating property of organic radicals. Here, the first example of radical‐containing supramolecular organic frameworks (SOFs) fabricated by the chaotropic effect between closo‐dodecaborate cluster (B12H122−) and 2,4,6‐tri(4‐pyridyl)‐1,3,5‐triazine (TPT3+) is presented. The SOFs can be easily synthesized by stirring the B12H122− and the TPT3+ in aqueous solution through self‐assembly. Upon 435 nm light irradiation, the SOFs exhibits photochromic behavior from slight yellow (SOF‐1) to dark purple (SOF‐2). Electron paramagnetic resonance spectroscopy also reveals that stable radicals are generated in situ after light irradiation. Powder X‐ray diffraction demonstrates the SOFs maintain their structural stabilities upon light irradiation. More interestingly, the radical‐containing SOFs exhibit efficient photothermal effect under 660 nm light irradiation, which can be applied as photothermal agent for antibacterial application both in vitro and in vivo. This work highlights the construction of RCFs through supramolecular self‐assembly, which may arouse applications in energy, catalysis, photoluminescence, and biomedical fields.

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Photoinduced Radical Emission in a Coassembly System

Cited by 53 publications

References 63 publications

A Platform for Blue-Luminescent Carbon-Centered Radicals

A Platform for Blue-Luminescent Carbon-Centered Radicals

A platform for blue-luminescent carbon-centered radicals

Chaotropic Effect Stabilized Radical‐Containing Supramolecular Organic Frameworks for Photothermal Therapy

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