Kong Jintao, Shang Xiaoying, Zheng Wei, Chen Xueyuan, Tu Datao, Wang Meng, Song Jun, Qu Junle
Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province, College of Physics and Optoelectronic Engineering, Shenzhen University, Shenzhen 518060, P. R. China.
CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of Nanomaterials, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, P. R. China.
J Phys Chem Lett. 2020 May 7;11(9):3672-3680. doi: 10.1021/acs.jpclett.0c00619. Epub 2020 Apr 27.
Energy transfer upconversion (ETU) can efficiently upconvert near-infrared photons into higher-energy photons. Although a comprehensive understanding of ETU is fundamental to the design of ETU materials, the basic excited-state decay kinetics of ETU remains a complicated problem. Here we unravel the mechanism underlying ETU decay in benchmark β-NaYF:Er and β-NaYF:Ln/Yb (Ln = Er, Ho, Tm) ETU microcrystals by combining rate equation analyses with ETU decay measurements. The results show that all of the excited states of one ETU system decay concordantly, with the ETU decay of the emitting state determined by only its intrinsic decay and the product of the ETU decays of the two intermediate states directly responsible for the emitting-state photon upconversion. This general mechanism may serve as a basic rule for excited-state kinetics in upconversion microparticles and nanoparticles, which could provide detailed insight into ETU processes and guide the design of efficient ETU materials.
能量转移上转换(ETU)能够有效地将近红外光子上转换为更高能量的光子。尽管全面理解ETU对于ETU材料的设计至关重要,但ETU的基本激发态衰变动力学仍然是一个复杂的问题。在此,我们通过将速率方程分析与ETU衰变测量相结合,揭示了基准β-NaYF:Er和β-NaYF:Ln/Yb(Ln = Er、Ho、Tm)ETU微晶中ETU衰变的潜在机制。结果表明,一个ETU系统的所有激发态协同衰变,发射态的ETU衰变仅由其固有衰变以及直接负责发射态光子上转换的两个中间态的ETU衰变产物决定。这一通用机制可作为上转换微粒和纳米颗粒中激发态动力学的基本规则,可为ETU过程提供详细的见解,并指导高效ETU材料的设计。