NanoCluster Beacons Enable Detection of a Single <i>N</i><sup>6</sup>-Methyladenine

Chen, Yu An; Obliosca, Judy M.; Liu, Chia‐Jyi; Liu, Cong; Gwozdz, Mary L.; Yeh, Hsin Chih

doi:10.1021/jacs.5b06038

Cited by 50 publications

(40 citation statements)

References 33 publications

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“…Fluorescence enhancement of DNA‐Ag NC sensors may also be achieved by bringing the Ag nucleation sequence in close proximity to G‐rich enhancer sequences. This observation has led to burgeoning interest in a series of ‘turn‐on’ probes for sensitive nucleic acid detection (even able to detect single nucleotide polymorphisms or SNP for short) . For example, Yeh et al designed a new type of fluorescent molecular probe, which they termed as chameleon NanoCluster Beacon (cNCB) (Figure A) .…”

Section: Desirable Features Of Metal Ncs For Theranostic Applicationsmentioning

confidence: 99%

Rational Design of Biomolecular Templates for Synthesizing Multifunctional Noble Metal Nanoclusters toward Personalized Theranostic Applications

Mok

Loh

et al. 2016

Adv Healthcare Materials

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thiolate-protected, [ 3 ] protein/peptide-templated, [ 4 ] and DNA-templated [ 5 ] ones. The last two types of metal NCs use biomolecules as templates to direct the synthesis (thus termed as biotemplated metal NCs), which afford more attractive features such as good aqueous solubility, superb biocompatibility, and versatile surface chemistries, [ 6 ] in addition to their ultrasmall size and superior photoluminescent optical properties. These desirable features render biotemplated metal NCs as promising candidates for various biomedical applications like imaging, [ 7 ] sensing, [ 7b,8 ] delivery [ 9 ] and therapeutics. [ 10 ] Theranostics is a revolutionary treatment strategy proposed by Funkhouser in 1998, which combines accurate diagnosis and targeted therapeutics. [ 11 ] From the list of individal biomedical applications mentioned earlier, a combination of sensing and imaging modalities would be fundamental for disease diagnosis. [ 12 ] In the same vein, image-guided targetedtherapy allows for real-time in vivo monitoring of the pharmacokinetics and pharmacodynamics of the therapeutic agent to enhance treatment effi ciency. [ 13 ] Through the ingenious combination of selective modalities, a highly potent and personalized theranostic agent could be developed. In particular, NC-based systems are poised to be the next versatile theranostic platform. This is because the intrinsic photoluminescence of the noble metal core can be harnessed for fl uorescence imaging, and tailor-made to exhibit unique optical properties for therapy, such as the generation of singlet oxygen [ 14 ] to substitute organicbased photosensitizers for possible photodynamic cancer treatments. In addition to the metal core, the biomolecular ligand shell surrounding the metal NC core can be easily functionalized with biorecognition moieties for sensing and targeted delivery. Due to the large surface to volume ratio of metal NCs, it can also serve as a reservoir sink to load multiple drugs/ genes and be modifi ed with sensing/imaging agents to imbue both therapeutic and diagnostic functions.The selective marriage of respective modalities to form theranostic biotemplated metal NCs will have a far-reaching impact on the future of medicine and healthcare. There are large amounts of work that use randomly picked natural biomolecules as templates to synthesize metal NCs for biomedical

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Section: Desirable Features Of Metal Ncs For Theranostic Applicationsmentioning

confidence: 99%

Rational Design of Biomolecular Templates for Synthesizing Multifunctional Noble Metal Nanoclusters toward Personalized Theranostic Applications

Mok

Loh

et al. 2016

Adv Healthcare Materials

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“…All of these factors contribute to the failure of standard hybridization-based methods for the detection of 6mA in DNA. To surmount this challenge, several methods based on selective polymerase, 7 sensitive restriction enzymes 8 and the distinct stabilities between A/6mA–G base pairs 9 have been developed for the detection of 6mA in DNA. However, both the selectivity and sensitivity of some methods require further improvement.…”

Section: Introductionmentioning

confidence: 99%

Selective detection of N6-methyladenine in DNA via metal ion-mediated replication and rolling circle amplification

et al. 2017

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“…35–37 We are motivated to understand this specific complex because tunable and switchable chromophores are the foundation of a new class of optical sensors. 20,22,23,34,38,39 …”

Section: Introductionmentioning

confidence: 99%

DNA-Directed Fluorescence Switching of Silver Clusters

et al. 2015

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Silver clusters with ≲30 atoms are molecules with diverse electronic spectra and wide-ranging emission intensities. Specific cluster chromophores form within DNA strands, and we consider a DNA scaffold that transforms a pair of silver clusters. This ~20-nucleotide strand has two components, a cluster domain (S1) that stabilizes silver clusters and a recognition site (S2) that hybridizes with complementary oligonucleotides (S2C). The single-stranded S1-S2 exclusively develops clusters with violet absorption and low emission. This conjugate hybridizes with S2C to form S1-S2:S2C, and the violet chromophore transforms to a fluorescent counterpart with λex ≈ 490 nm/λem ≈ 550 nm and with ~100-fold stronger emission. Our studies focus on both the S1 sequence and structure that direct this violet → blue-green cluster transformation. From the sequence perspective, C4X sequences with X = adenine, thymine, and/or guanine favor the blue-green cluster, and the specificity of the binding site depends on three factors: the number of C4X repeats, the identity of the X nucleobase, and the number of contiguous cytosines. A systematic series of oligonucleotides identified the optimal S1 sequence C4AC4T and discerned distinct roles for the adenine, thymine, and cytosines. From the structure perspective, two factors guide the conformation of the C4AC4T sequence: hybridization with the S2C complement and coordination by the cluster adduct. Spectroscopic and chromatographic studies show that the single-stranded C4AC4T is folded by its blue-green cluster adduct. We propose a structural model in which the two C4X motifs within C4AC4T are cross-linked by the encapsulated cluster. These studies suggest that the structures of the DNA host and the cluster adduct are interdependent.

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NanoCluster Beacons Enable Detection of a Single N⁶-Methyladenine

Cited by 50 publications

References 33 publications

Rational Design of Biomolecular Templates for Synthesizing Multifunctional Noble Metal Nanoclusters toward Personalized Theranostic Applications

Rational Design of Biomolecular Templates for Synthesizing Multifunctional Noble Metal Nanoclusters toward Personalized Theranostic Applications

Selective detection of N6-methyladenine in DNA via metal ion-mediated replication and rolling circle amplification

DNA-Directed Fluorescence Switching of Silver Clusters

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NanoCluster Beacons Enable Detection of a Single N6-Methyladenine

Cited by 50 publications

References 33 publications

Rational Design of Biomolecular Templates for Synthesizing Multifunctional Noble Metal Nanoclusters toward Personalized Theranostic Applications

Rational Design of Biomolecular Templates for Synthesizing Multifunctional Noble Metal Nanoclusters toward Personalized Theranostic Applications

Selective detection of N6-methyladenine in DNA via metal ion-mediated replication and rolling circle amplification

DNA-Directed Fluorescence Switching of Silver Clusters

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NanoCluster Beacons Enable Detection of a Single N⁶-Methyladenine