期刊
FRONTIERS IN CHEMISTRY
卷 9, 期 -, 页码 -出版社
FRONTIERS MEDIA SA
DOI: 10.3389/fchem.2021.810304
关键词
pure organic room-temperature phosphorescence; discrete molecule; thianthrene; ratiometric optical oxygen sensing; polymer film; folding geometry; spin-orbit coupling
资金
- National Natural Science Foundation of China [51873077, 91833304, 52073117, 52103209]
- National Key Research and Development Program of China [2020YFA0714603]
- China Postdoctoral Science Foundation [2018M641767]
In this work, two new pure organic discrete-molecule room-temperature phosphorescence (RTP) materials were synthesized, which show dual emission of fluorescence and RTP through a mechanism of folding-induced spin-orbit coupling enhancement. These materials can be used for optical oxygen sensing at low oxygen concentrations with high sensitivity.
In this work, two thianthrene (TA) derivatives, 1-phenylthianthrene (TA1P) and 2-phenylthianthrene (TA2P), were synthesized with single-phenyl modification for pure organic discrete-molecule room-temperature phosphorescence (RTP). They both show the dual emission of fluorescence and RTP in amorphous polymer matrix after deoxygenation, as a result of a new mechanism of folding-induced spin-orbit coupling (SOC) enhancement. Compared with TA1P, TA2P exhibits a higher RTP efficiency and a larger spectral separation between fluorescence and RTP, which is ascribed to the substituent effect of TA at the 2-position. With decreasing oxygen concentration from 1.61% to 0%, the discrete-molecule TA2P shows an about 18-fold increase in RTP intensity and an almost constant fluorescence intensity, which can make TA2P as a self-reference ratiometric optical oxygen sensing probe at low oxygen concentrations. The oxygen quenching constant (K-SV) of TA2P is estimated as high as 10.22 KPa-1 for polymethyl methacrylate (PMMA)-doped film, and even reach up to 111.86 KPa-1 for Zeonex(R)-doped film, which demonstrates a very high sensitivity in oxygen sensing and detection. This work provides a new idea to design pure organic discrete-molecule RTP materials with high efficiency, and TA derivatives show a potential to be applied in quantitative detection of oxygen as a new-generation optical oxygen-sensing material.
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