Journal
NANOSCALE ADVANCES
Volume 2, Issue 9, Pages 3921-3932Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0na00381f
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Funding
- Institute of Materials Research and Engineering (IMRE), A*STAR under the Biomimetic and Biomedical Materials Program [IMRE/17-1P1404, IMRE/14-1C0420]
- Newcastle University [RSA/CCEAMD5010]
- National University of Singapore
- University of Illinois at Urbana-Champaign
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DNA-templated silver nanoclusters (AgNCs) are an emerging class of ultrasmall (<2 nm) fluorophores with increasing popularity for bioimaging due to their facile synthesis and tunable emission color. However, design rules correlating different nucleotide sequences with the photoemission properties of AgNCs are still largely unknown, preventing the rational design of DNA templates to fine-tune the emission color, brightness and functionalities of AgNCs for any targeted applications. Herein, we report a systematic investigation to understand the empirical influences of the four basic DNA nucleotides on AgNC synthesis and their effects on photoluminescence properties. After establishing the importance of nucleotide-Ag(+)binding and AgNC encapsulation within DNA tetraplex structures, we then determined the unique attributes of each individual nucleobase using different combinations of systematically varied DNA templates. Using the empirical design rules established herein, we were able to predict the photoluminescence behaviours of AgNCs templated by complex aptamer sequences with specific binding affinity to human cancer cells, and to deliberately control their emission color by rational modifications of the DNA template sequences for targeted bioimaging. Our empirical findings from this systematic experimentation can contribute towards the rational design of DNA sequences to customise the photoluminescence properties and biofunctionalities of DNA-protected AgNCs towards multicolour targeted bioimaging applications.
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