He Shan, Lai Runchen, Jiang Qike, Han Yaoyao, Luo Xiao, Tian Yuyang, Liu Xue, Wu Kaifeng
State Key Laboratory of Molecular Reaction Dynamics, Dynamics Research Center for Energy and Environmental Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning, 116023, China.
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning, 116023, China.
Angew Chem Int Ed Engl. 2020 Sep 28;59(40):17726-17731. doi: 10.1002/anie.202009066. Epub 2020 Aug 11.
Triplet energy transfer from inorganic nanocrystals to molecular acceptors has attracted strong attention for high-efficiency photon upconversion. Here we study this problem using CsPbBr and CdSe nanocrystals as triplet donors and carboxylated anthracene isomers as acceptors. We find that the position of the carboxyl anchoring group on the molecule dictates the donor-acceptor coupling to be either through-bond or through-space, while the relative strength of the two coupling pathways is controlled by the wavefunction leakage of nanocrystals that can be quantitatively tuned by nanocrystal sizes or shell thicknesses. By simultaneously engineering molecular geometry and nanocrystal wavefunction, energy transfer and photon upconversion efficiencies of a nanocrystal/molecule system can be improved by orders of magnitude.
从无机纳米晶体到分子受体的三线态能量转移因高效光子上转换而备受关注。在此，我们以CsPbBr和CdSe纳米晶体作为三线态供体，以羧基化蒽异构体作为受体来研究这一问题。我们发现分子上羧基锚定基团的位置决定了供体 - 受体耦合是通过化学键还是通过空间，而这两种耦合途径的相对强度由纳米晶体的波函数泄漏控制，纳米晶体尺寸或壳层厚度可对其进行定量调节。通过同时设计分子几何结构和纳米晶体波函数，纳米晶体/分子体系的能量转移和光子上转换效率可提高几个数量级。
