Highly efficient upconversion photodynamic performance of rare-earth-coupled dual-photosensitizers: ultrafast experiments and excited-state calculations
Author:
Yang Yubiao1, Zhang Lei1, Xiao Chao1, Huang Zhencheng1, Zhao Fuli1ORCID, Yin Jinchang2ORCID
Affiliation:
1. School of Physics, State Key Laboratory of Optoelectronic Materials and Technologies , Sun Yat-Sen University , Guangzhou 510275 , China 2. School of Biomedical Engineering, Health Science Center , Shenzhen University , Shenzhen 518060 , China
Abstract
Abstract
Upconversion photodynamic therapy (UC-PDT), which integrates upconversion nanoparticles (UCNPs) with photosensitizers (PSs), presents a promising advancement in the field of phototherapy. However, despite the extensive studies focused on the design and synthesis of UCNPs, there is a paucity of systematic research on the mechanisms underlying the synergistic upconversion photodynamic effects. Here we have synthesized upconversion core@dotted-shell nanoparticles (CDSNPs) and covalently tethered them with two distinct PSs, thereby constructing a dual-PS UC-PDT system with high synergistic photodynamic performance. To unravel the mechanism underlying the synergism, we employed a combination of quantum mechanical calculations and ultrafast time-resolved spectroscopy techniques. The results indicate that rare earth oxides play a pivotal role in enhancing the intersystem crossing processes of PSs through modulating their excited electronic states. Additionally, Förster resonance energy transfer between two distinct PSs contributes to the amplification of triplet state populations, thus further enhancing the photodynamic effect. In vitro experiments demonstrate that the prepared CDSNPs based dual-PS system exhibits excellent biocompatibility with normal cells and exceptional synergistic photodynamic efficacy against tumor cells upon near-infrared excitation. This research contributes theoretical insights into the design and application of multi-photosensitizer UC-PDT systems, laying the groundwork for more efficient preclinical implementations in the future.
Funder
Basic and Applied Basic Research Foundation of Guangdong Province National Natural Science Foundation of China Fundamental Research Funds for the Central Universities
Publisher
Walter de Gruyter GmbH
Subject
Electrical and Electronic Engineering,Atomic and Molecular Physics, and Optics,Electronic, Optical and Magnetic Materials,Biotechnology
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