Harnessing Exciton Flux With a Single‐Stranded DNA‐Programmed Nanodevice
Abstract
ABSTRACT Natural and artificial nanosystems rely on functional module assembly, yet overcoming thermodynamic incompatibility in atomically precise nanodevice integration remains challenging. Here, we construct a single‐stranded DNA (ssDNA)‐directed nanodevice that achieves 94.3% quenching efficiency by harnessing asymmetric π–π interactions to split exciton energy levels. DNA spatial confinement orchestrates hydrophobic, covalent, and π–π interactions, enabling precise component arrangement. This nanodevice comprises a light‐harvesting engine, a vibrational metal nanocluster actuator and a programmable ssDNA. Asymmetric π–π interactions between fluorophore and metal nanocluster in DNA spatial confinements split fluorophore energy levels, directing exciton flux. Complementary DNA strands modulate engine‐actuator coupling, enabling enthalpy‐driven switching between radiative and non‐radiative pathways. By tuning DNA length and nanocluster ligands, we achieve continuous control over energy transfer efficiency. This programmable platform, manipulating non‐radiative decay via π–π interactions, establishes vibrational control as a general paradigm for nanoscale energy transduction.
Article Details
Authors (11)
Mulin Duan
State Key Laboratory of Synergistic Chem‐Bio Synthesis School of Chemistry and Chemical Engineering New Cornerstone Science Laboratory Frontiers Science Center for Transformative Molecules and National Center for Translational Medicine Shanghai Jiao Tong University Shanghai China
Yan Zhou
Haoran Zheng
Bingjie Yan
State Key Laboratory of Synergistic Chem‐Bio Synthesis School of Chemistry and Chemical Engineering New Cornerstone Science Laboratory Frontiers Science Center for Transformative Molecules and National Center for Translational Medicine Shanghai Jiao Tong University Shanghai China
Gaoang Zhou
State Key Laboratory of Synergistic Chem‐Bio Synthesis School of Chemistry and Chemical Engineering New Cornerstone Science Laboratory Frontiers Science Center for Transformative Molecules and National Center for Translational Medicine Shanghai Jiao Tong University Shanghai China
Siyuan Zhang
Shihua Luo
Department of Traumatology, Rui Jin Hospital, School of Medicine, Shanghai Jiao Tong University
Jing Chen
Chang Yan
Interdisciplinary Institute of NMR and Molecular Sciences, Hubei Province for Coal Conversion and New Carbon Materials, School of Chemistry and Chemical Engineering
Chunhai Fan
State Key Laboratory of Synergistic Chem-Bio Synthesis, School of Chemistry and Chemical Engineering, New Cornerstone Science Laboratory, Frontiers Science Center for Transformative Molecules, Zhang Jiang Institute for Advanced Study and National Center for Translational Medicine
Jianlei Shen
State Key Laboratory of Synergistic Chem-Bio Synthesis, School of Chemistry and Chemical Engineering, New Cornerstone Science Laboratory, Frontiers Science Center for Transformative Molecules and National Center for Translational Medicine, Shanghai Jiao Tong University