• 文献标题:   Controllable Singlet-Triplet Energy Splitting of Graphene Quantum Dots through Oxidation: From Phosphorescence to TADF
  • 文献类型:   Article
  • 作  者:   PARK M, KIM HS, YOON H, KIM J, LEE S, YOO S, JEON S
  • 作者关键词:   anticounterfeiting, graphene quantum dot, phosphorescence, singlettriplet energy splitting, thermally activated delayed fluorescence
  • 出版物名称:   ADVANCED MATERIALS
  • ISSN:   0935-9648 EI 1521-4095
  • 通讯作者地址:   Korea Adv Inst Sci Technol
  • 被引频次:   2
  • DOI:   10.1002/adma.202000936
  • 出版年:   2020

▎ 摘  要

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 ( increment E-ST) in graphene quantum dots (GQD)/graphene oxide quantum dots (GOQDs) by varying the ratio of oxygenated carbon to sp(2)carbon (gamma(OC)). It is demonstrated that increment E(ST)decreases from 0.365 to 0.123 eV as gamma(OC)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 (tau(T)(avg)) of 783 ms, and the highly oxidized (59.6%) GOQD exhibits a TADF lifetime (tau(DF)(avg)) 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 approach to the engineering of singlet-triplet splitting in GQD for controlled realization of smart multimodal afterglow materials.