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Published on: August 1, 2018
Engineering Synergistic Intra-/Intermolecular Conformational Locking via Side-Chain Branching: A β-Sheet-Inspired
1Department of Chemistry, Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction, Division of Life Science and State Key Laboratory of Molecular Neuroscience, The Hong Kong University of Science and Technology, Kowloon, Hong Kong, China.
Researchers engineered stable noncovalent conformational locks (NoCL) networks in phototheranostic aggregates (PTAs). This strategy enhances PTA rigidity and light-harvesting for improved multimodal cancer phototheranostics.
Area of Science:
- Materials Science
- Nanotechnology
- Biomedical Engineering
Background:
- Engineering stable noncovalent conformational locks (NoCL) networks is crucial for phototheranostic aggregates (PTAs) with enhanced rigidity and light-harvesting.
- Complex intermolecular interactions pose challenges in developing robust PTAs.
Purpose of the Study:
- To develop a side-chain isomerization strategy for manipulating NoCL networks in planar-structured NIR-II multimodal PTAs.
- To investigate the impact of side-chain structure on aggregate conformation and phototheranostic performance.
Main Methods:
- Synthesis of isomeric pairs with linear (l-series) and branched (b-series) alkyl side-chains.
- Crystallographic analysis to determine aggregate conformation.
- Theoretical calculations and femtosecond transient absorption spectroscopy to study electronic properties.
Main Results:
- The b-series, with branched side-chains, adopted a fully planar conformation stabilized by a dual NoCL network, unlike the twisted l-series.
- The dual NoCL network in b-series PTAs narrowed the energy gap and optimized excited-state dissipation.
- Enhanced phototheranostic performance, including superior ROS generation, NIR-II brightness, and photothermal properties, was observed in b-series PTAs.
Conclusions:
- A novel design paradigm for multifunctional PTAs using side-chain isomerization was established.
- Aggregate-level structure-property relationships were elucidated, demonstrating the effectiveness of dual NoCL networks.
- Branched side-chain PTAs show significant potential for multimodal NIR-II phototheranostics of tumors.
