Boosting the Energy Migration Upconversion through Inter-Shell Energy Transfer in Tb^(3+)-Doped Sandwich Structured Nanocrystals

作     者：Dan Xu Jin Xu Xiaoying Shang Shaohua Yu Wei Zheng Datao Tu Renfu Li Xueyuan Chen 

作者机构：CAS Key Laboratory of Design and Assembly of Functional NanostructuresFujian Key Laboratory of Nanomaterialsand State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002 University of Chinese Academy of SciencesBeijing 100049 Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of ChinaFuzhouFujian 350108 

出 版 物：《CCS Chemistry》 (中国化学会会刊（英文）)

年 卷 期：2022年第4卷第6期

页      面：2031-2042页

学科分类：081704[工学-应用化学] 07[理学] 08[工学] 0817[工学-化学工程与技术] 0703[理学-化学] 070301[理学-无机化学] 

基　　金：supported by the Science and Technology Cooperation Fund between Chinese and Australian Governments(grant no.2017YFE0132300) the Strategic Priority Research Program of the CAS(grant no.XDB20000000) the National Natural Science Foundation of China(grant nos.21771185,U1805252,12074380,12074379,and 21975257) the CAS/SAFEA International Partnership Program for Creative Research Teams 

主　　题：lanthanide nanocrystals energy migration upconversion sandwich structured inter-shell energy transfer energy management 

摘      要：It remained challenging to fabricate Tb^(3+)-doped lanthanide nanocrystals(NCs)to simultaneously acquire strong energy migration upconversion(EMU)emissions of Tb^(3+)while suppressing the Tm3+UV upconversion emissions that cause background biofluorescence issues in bioapplications based on Tb^(3+)-doped EMU ***,we report a novel sandwich structured core@shell@shell scheme for the design of EMU NCs,for example,NaLuF4∶Yb/Gd@NaGdF4∶Tm@NaLuF4∶Tb NCs,wherein Yb^(3+),Tm^(3+),and Tb^(3+)are incorporated separately into the inner core,middle shell,and outer shell,*** found that in the sandwich structured NCs,the effective inter-shell energy transfer from Gd^(3+)in the middle shell to Tb^(3+)in the outer shell accelerated the Yb^(3+)-Tm^(3+)five-photon upconversion and the subsequent Tm^(3+)to Gd^(3+)energy transfer processes,which could eventually lead to almost complete inhibition of Tm^(3+)UV upconversion emissions,concurrent with the strong EMU emissions of Tb^(3+).Our findings might stimulate new concepts for manipulating upconversion emissions of lanthanide NCs.