Controllable Singlet-Triplet Energy Splitting of Graphene Quantum Dots through Oxidation: From Phosphorescence to TADF

Advanced Materials
Minsu ParkSeokwoo Jeon

Abstract

Long-lived afterglow emissions, such as room-temperature phosphorescence (RTP) and thermally activated delayed fluorescence (TADF), are beneficial in the fields of displays, bioimaging, and data security. However, it is challenging to realize a single material that simultaneously exhibits both RTP and TADF properties with their relative strengths varied in a controlled manner. Herein, a new design approach is reported to control singlet-triplet energy splitting (∆EST ) in graphene quantum dots (GQD)/graphene oxide quantum dots (GOQDs) by varying the ratio of oxygenated carbon to sp2 carbon (γOC ). It is demonstrated that ∆EST decreases from 0.365 to 0.123 eV as γOC increases from 4.63% to 59.6%, which in turn induces a dramatic transition from RTP to TADF. Matrix-assisted stabilization of triplet excited states provides ultralong lifetimes to both RTP and TADF. Embedded in boron oxynitride, the low oxidized (4.63%) GQD exhibits an RTP lifetime (τTavg ) of 783 ms, and the highly oxidized (59.6%) GOQD exhibits a TADF lifetime (τDFavg ) of 125 ms. Furthermore, the long-lived RTP and TADF materials enable the first demonstration of anticounterfeiting and multilevel information security using GQD. These results will open up a new ap...Continue Reading

References

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May 7, 2016·Advanced Materials·Hyewon YoonSeokwoo Jeon
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Oct 14, 2017·Physical Chemistry Chemical Physics : PCCP·Shinaj K RajagopalMahesh Hariharan
Apr 11, 2018·ACS Applied Materials & Interfaces·Weon-Sik ChaeSeokwoo Jeon

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Citations

Aug 6, 2021·The Journal of Physical Chemistry Letters·Jingkun YuSiyu Lu
Dec 31, 2020·ACS Central Science·Junjun LiuBai Yang
Oct 4, 2021·Comprehensive Reviews in Food Science and Food Safety·Arumugam Selva SharmaQuansheng Chen
Jan 13, 2022·Macromolecular Rapid Communications·Yixuan WangXiaolin Xie

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