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- Xing, Yi, et al.
(författare)
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Water molecular bridge-induced selective dual polarization in crystals for stable multi-emitters
- 2022
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Ingår i: Chemical Science. - : Royal Society of Chemistry. - 2041-6520 .- 2041-6539. ; 13:20, s. 6067-6073
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Tidskriftsartikel (refereegranskat)abstract
- In the solid state, the molecular polarization of donor-acceptor (D-A) molecules can be implemented in a simple way via the use of an external polarizing source (e.g., an electric field). However, internal chemical polarization approaches are less studied due to difficulties related to controlling the charge-separation orientation in the solid state. Herein, a series of D-A molecules with both a proton donor and an acceptor were designed. Water-based molecular bridges were then established in their crystal structures, which firmly and alternately connected the proton donor of one molecule and the acceptor of another via an intermolecular H-bond network. In this way, the selective dual polarization of a phenolic hydroxyl group and a pyridinyl group could be achieved, owing to the strengthening of the charge-separation orientation upon the simultaneous deprotonation and protonation of the D-A molecules. This effect led to a 3-5-fold amplification of the molecular dipole moment in the crystal form relative to the monomeric state. On this basis, multi-excitation and multi-emission characteristics were achieved in these charge-separated crystals, endowing them with the ability to visually detect the energy of a light source, covering a wide range of the UV-Vis spectral region. This work provides a practical chemical approach for developing intrinsically polarized systems that can exhibit stable but distinct molecular photophysical properties.
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2. |
- Ye, Danfeng, et al.
(författare)
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Deoxygenation-Promoted Aggregation-Induced TADF-RTP Dual Emission for High-Contrast Channel-Selectable Hypoxia Probing
- 2024
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Ingår i: The Journal of Physical Chemistry C. - : AMER CHEMICAL SOC. - 1932-7447 .- 1932-7455.
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Tidskriftsartikel (refereegranskat)abstract
- Thermally activated delayed fluorescence (TADF) and room-temperature phosphorescence (RTP) are two highly applicable emissive processes due to their time-resolved characteristics and their ability to respond to external stimuli. They have recently been integrated for comprehensive use in some solid-state luminogens; however, there remains a lack of molecular systems that can integrate them in the solution aggregated state, which considerably limits relevant biological applications. In this study, we present a molecular design enabling aggregation-induced TADF-RTP dual emission in the solution aggregated state, relying on the coexistence of T-1-to-S-1 and T-1-to-S-0 electronic processes in push-pull structures. This dual emission feature constitutes a broad spectral band with full width at half-maximum up to 175 nm, providing the ability to select different channels for biological detection and imaging. Moreover, deoxygenation is shown to promote molecular aggregation, leading to a significantly strengthened dual emission that enables a high-contrast hypoxia probing effect. These results not only reveal new photophysical mechanisms on organic molecules but also expand the detection functionality of luminescent materials in the biological field.
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