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Abstract
Jung Seung Nam†∥, Myeong-Gyun Kang†∥, Juhye Kang†∥, Sun-Young Park‡∥, Shin Jung C. Lee†, Hyun-Tak Kim†, Jeong Kon Seo§, Oh-Hoon Kwon†‡, Mi Hee Lim*†, Hyun-Woo Rhee*†, and Tae-Hyuk Kwon*†
† Department of Chemistry, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
‡ Center for Soft and Living Matter, Institute for Basic Science (IBS), Ulsan 44919, Republic of Korea
§ UNIST Central Research Facility, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
*Corresponding Authors
Author Contributions
∥J.S.N., M.-G.K., J.K., and S.-Y.P. contributed equally to this work.
Abstract
Protein inactivation by reactive oxygen species (ROS) such as singlet oxygen (1O2) and superoxide radical (O2-) is considered to trigger cell death pathways associated with protein dysfunction; however, the detailed mechanisms and direct involvement in photodynamic therapy (PDT) have not been revealed. Herein, we report Ir(III) complexes designed for ROS generation through a rational strategy to investigate protein modifications by ROS. The Ir(III) complexes are effective as PDT agents at low concentrations with low-energy irradiation (≤ 1 J cm-2) because of the relatively high 1O2 quantum yield (> 0.78), even with two-photon activation. Furthermore, two types of protein modifications (protein oxidation and photo-cross-linking) involved in PDT were characterized by mass spectrometry. These modifications were generated primarily in the endoplasmic reticulum and mitochondria, producing a significant effect for cancer cell death. Consequently, we present a plausible biologically applicable PDT modality that utilizes rationally designed photoactivatable Ir(III) complexes.
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