Thermally activated delayed fluorescence(TADF)polymeric materials based on through-space charge transfer(TSCT)have emerged as a highly studied topic in recent years.However,the construction of TSCT TADF materials via ...Thermally activated delayed fluorescence(TADF)polymeric materials based on through-space charge transfer(TSCT)have emerged as a highly studied topic in recent years.However,the construction of TSCT TADF materials via a supramolecular approach is still a big challenge.In this work,we report the noncovalent synthesis of TSCT TADF materials using a cyclic peptide-based bottle-brushed supramolecular polymer as a scaffold.By bringing the TSCT donor and acceptor in close proximity in space using the supramolecular scaffold,distinctive TADF emission in both solution and solid states could be achieved.Furthermore,the TADF system could be utilized as a sensitizer to coassemble with fluorescence acceptors to build thermally assisted fluorescence systems,resulting in color-tunable delayed fluorescence with high efficiency and color purity.Our findings provide a facile yet effective approach to designing and fabricating TSCT TADF materials,which might hold great potential for applications in the fields of organic light-emitting diode,bioimaging,and sensing.展开更多
Electronic coupling between individual building blocks plays an essential role in charge transport through molecular materials and devices.However,the investigation of the transmission mechanism in charge transport vi...Electronic coupling between individual building blocks plays an essential role in charge transport through molecular materials and devices.However,the investigation of the transmission mechanism in charge transport via intramolecular coupling remains challenging.Herein,we demonstrate the transition of the intramolecular through-bond and through-space coupling in a single-molecule junction with a family of diketopyrrolopyrrole(DPP)derivative by varying intramolecular donor–acceptor(D–A)interactions.The transition is accomplished by regulating D–A interactions by inserting different aromatic rings inside,leading to two orders of magnitude difference of the single-molecule conductance.The flicker noise analysis demonstrates that the conductance difference arises from the control of the contribution between through-bond and through-space coupling.These findings are further supported by the calculation that the intramolecular coupling among molecular building blocks correlates with the D–A interaction,providing a promising way to regulate the contribution between through-bond and through-space coupling in the charge transport through molecular materials and devices.展开更多
基金The National Natural Science Foundation of China(grant no.22101124)Shenzhen Science and Technology Program(grant nos.20220815163454004 and JCYJ20210324105009025)+1 种基金Natural Science Foundation of Guangdong Province of China(grant no.2022A1515011394)Shenzhen Nobel Prize Scientists Laboratory Project(grant no.C17783101)are acknowledged for the financial support.
文摘Thermally activated delayed fluorescence(TADF)polymeric materials based on through-space charge transfer(TSCT)have emerged as a highly studied topic in recent years.However,the construction of TSCT TADF materials via a supramolecular approach is still a big challenge.In this work,we report the noncovalent synthesis of TSCT TADF materials using a cyclic peptide-based bottle-brushed supramolecular polymer as a scaffold.By bringing the TSCT donor and acceptor in close proximity in space using the supramolecular scaffold,distinctive TADF emission in both solution and solid states could be achieved.Furthermore,the TADF system could be utilized as a sensitizer to coassemble with fluorescence acceptors to build thermally assisted fluorescence systems,resulting in color-tunable delayed fluorescence with high efficiency and color purity.Our findings provide a facile yet effective approach to designing and fabricating TSCT TADF materials,which might hold great potential for applications in the fields of organic light-emitting diode,bioimaging,and sensing.
基金supported by Natural Science Foundation of China(nos.21722305,21673195,21703188,51733004,and 51525303)the National Key R&D Program of China(nos.2017YFA0204902 and 2017YFA0204903)+1 种基金the Beijing National Laboratory for Molecular Sciences(no.BNLMS202005)the China Postdoctoral Science Foundation(no.2017M622060).
文摘Electronic coupling between individual building blocks plays an essential role in charge transport through molecular materials and devices.However,the investigation of the transmission mechanism in charge transport via intramolecular coupling remains challenging.Herein,we demonstrate the transition of the intramolecular through-bond and through-space coupling in a single-molecule junction with a family of diketopyrrolopyrrole(DPP)derivative by varying intramolecular donor–acceptor(D–A)interactions.The transition is accomplished by regulating D–A interactions by inserting different aromatic rings inside,leading to two orders of magnitude difference of the single-molecule conductance.The flicker noise analysis demonstrates that the conductance difference arises from the control of the contribution between through-bond and through-space coupling.These findings are further supported by the calculation that the intramolecular coupling among molecular building blocks correlates with the D–A interaction,providing a promising way to regulate the contribution between through-bond and through-space coupling in the charge transport through molecular materials and devices.
基金supported by the National Natural Science Foundation of China(22275097,61875090,21772095,and 91833306)the Key Giant Project of Jiangsu Educational Committee(19KJA180005)+5 种基金the Fifth 333 Project of Jiangsu Province of China(BRA2019080)the 1311 Talents Program of Nanjing University of Posts and Telecommunicationsthe Natural Science Foundation of Jiangsu Higher Education Institutions(22KJB150030)the Scientific Starting Fund from Nanjing University of Posts and Telecommunications(NUPTSF)(NY219160)the Natural Science Foundation of Nanjing University of Posts and Telecommunications(NY221092 and NY222148)the Open Research Fund of State Key Laboratory of Organic Electronics and Information Displays。
