Department of Biochemistry and Molecular Pharmacology, University of Massachusetts Medical School, Worcester, MA, 01605, USA.
Angew Chem Int Ed Engl. 2017 Nov 13;56(46):14400-14404. doi: 10.1002/anie.201704430. Epub 2017 Oct 10.
A strategy to expand anti-Stokes shifting from the far-red to deep-blue region in metal-free triplet-triplet annihilation upconversion (TTA-UC) is presented. The method is demonstrated by in vivo titration of the photorelease of an anticancer prodrug. This new TTA system has robust brightness and the longest anti-Stokes shift of any reported TTA system. TTA core-shell-structured prodrug delivery capsules that benefit from these properties were developed; they can operate with low-power density far-red light-emitting diode light. These capsules contain mesoporous silica nanoparticles preloaded with TTA molecules as the core, and amphiphilic polymers encapsulating anticancer prodrug molecules as the shell. When stimulated by far-red light, the intense TTA upconversion blue emission in the system activates the anticancer prodrug molecules and shows effective tumor growth inhibition in vivo. This work paves the way to new organic TTA upconversion techniques that are applicable to in vivo photocontrollable drug release and other biophotonic applications.
提出了一种在无金属三重态-三重态湮灭上转换（TTA-UC）中将反斯托克斯位移从远红区扩展到深蓝光区的策略。该方法通过体内滴定抗癌前药的光释放来证明。这种新的 TTA 系统具有很强的亮度和报道的 TTA 系统中最长的反斯托克斯位移。开发了受益于这些特性的 TTA 核壳结构前药递药胶囊；它们可以用低功率密度的远红光发光二极管灯进行操作。这些胶囊包含介孔硅纳米粒子作为核，负载 TTA 分子，两亲聚合物作为壳，包裹抗癌前药分子。当受到远红光刺激时，该系统中强烈的 TTA 上转换蓝光发射会激活抗癌前药分子，并在体内显示出有效的肿瘤生长抑制作用。这项工作为新的有机 TTA 上转换技术铺平了道路，这些技术适用于体内光控药物释放和其他生物光子应用。
