Currently,there is a strong drive to discover alternative materials that exhibit room-temperature phosphorescence(RTP)for displays,bioimaging,and data security.Ideally,these materials should be nontoxic,cheap,and poss...Currently,there is a strong drive to discover alternative materials that exhibit room-temperature phosphorescence(RTP)for displays,bioimaging,and data security.Ideally,these materials should be nontoxic,cheap,and possess controllable photoluminescent properties.Carbon dots(CDs)possess each of these characteristics,but to date,less attention has been paid to their RTP mechanism.Herein,we synthesized a series of CDs by self-crosslinking and carbonization of precursor.The resultant CDs were luminescent and exhibited a bright,micro-second afterglow lifetime.To increase the RTP,a second microwave processing step was used to coat the CDs with polyvinyl alcohol(PVA),polyacrylamide(PAM),or tetraethyl orthosilicate(TEOS),producing CDs@PVA,CDs@PAM,and CDs@TEOS composites.The core-shell structure acted to enhance crosslinking at the surface of the CDs to boost the RTP,creating abundant energy levels for intersystem crossover.In situ X-ray photoelectron spectroscopy verified electron transfer during luminescence.Finally,we present a design rule that can be used to tune the quantum yields and RTP lifetime of CDs,based on the effective stabilization of triplet excited states through the extent and strength of cross-linking.This simple strategy provides a flexible route for guiding the further development of CDs with tailored RTP properties for various applications.展开更多
Purely organic room-temperature phosphors,which have received extensive attention as emerging stateof-the-art luminescent materials in various fields,have a longer lifetime than fluorophores.The energy gap law and El-...Purely organic room-temperature phosphors,which have received extensive attention as emerging stateof-the-art luminescent materials in various fields,have a longer lifetime than fluorophores.The energy gap law and El-Sayed’s rule provide clear design principles for the development of organic room-temperature phosphorescence.Therefore,the incorporation of heteroatoms(such as sulfur and phosphorus)usually promotes the intersystem crossing rate and increases the 3(π,π*)configuration to realize long lifetimes.Furthermore,boron-containing phosphors not only display excellent phosphorescence properties but also expand El-Sayed’s rule without(n,π*)transitions.This review summarizes recent work on organic phosphorescence of heterocycles with boron,sulfur,and phosphorus heteroatoms and highlights the significance of the guidelines for constructing efficient phosphorescence molecules.This work is instrumental in further diversifying the pool of phosphorescent molecules and developing new and effective design strategies.展开更多
基金supported by the National Natural Science Foundation of China(Nos.52122308,21905253,and 51973200)the Natural Science Foundation of Henan Province(No.202300410372).
文摘Currently,there is a strong drive to discover alternative materials that exhibit room-temperature phosphorescence(RTP)for displays,bioimaging,and data security.Ideally,these materials should be nontoxic,cheap,and possess controllable photoluminescent properties.Carbon dots(CDs)possess each of these characteristics,but to date,less attention has been paid to their RTP mechanism.Herein,we synthesized a series of CDs by self-crosslinking and carbonization of precursor.The resultant CDs were luminescent and exhibited a bright,micro-second afterglow lifetime.To increase the RTP,a second microwave processing step was used to coat the CDs with polyvinyl alcohol(PVA),polyacrylamide(PAM),or tetraethyl orthosilicate(TEOS),producing CDs@PVA,CDs@PAM,and CDs@TEOS composites.The core-shell structure acted to enhance crosslinking at the surface of the CDs to boost the RTP,creating abundant energy levels for intersystem crossover.In situ X-ray photoelectron spectroscopy verified electron transfer during luminescence.Finally,we present a design rule that can be used to tune the quantum yields and RTP lifetime of CDs,based on the effective stabilization of triplet excited states through the extent and strength of cross-linking.This simple strategy provides a flexible route for guiding the further development of CDs with tailored RTP properties for various applications.
基金the Ministry of Education and Synergetic Innovation Center for Organic Electronics and Information Displays,LiaoNing Revitalization Talents Program(grant no.XLYC1902111)and the Key Projects of the Department of Education,Liaoning Province(grant no.LZD202005)for their financial support of this research.
文摘Purely organic room-temperature phosphors,which have received extensive attention as emerging stateof-the-art luminescent materials in various fields,have a longer lifetime than fluorophores.The energy gap law and El-Sayed’s rule provide clear design principles for the development of organic room-temperature phosphorescence.Therefore,the incorporation of heteroatoms(such as sulfur and phosphorus)usually promotes the intersystem crossing rate and increases the 3(π,π*)configuration to realize long lifetimes.Furthermore,boron-containing phosphors not only display excellent phosphorescence properties but also expand El-Sayed’s rule without(n,π*)transitions.This review summarizes recent work on organic phosphorescence of heterocycles with boron,sulfur,and phosphorus heteroatoms and highlights the significance of the guidelines for constructing efficient phosphorescence molecules.This work is instrumental in further diversifying the pool of phosphorescent molecules and developing new and effective design strategies.