Silver clusters as both chromophoric reporters and DNA ligands

Jeffrey T. Petty, Banabihari Giri, Ian C. Miller, David A. Nicholson, Orlin O. Sergev, Taylor M. Banks, Sandra P. Story

Research output: Contribution to journalArticle

30 Citations (Scopus)

Abstract

Molecular silver clusters conjugated with DNA act as analyte sensors. Our studies evaluate a type of cluster-laden DNA strand whose structure and silver stoichiometry change with hybridization. The sensor strand integrates two functions: the 3′ region binds target DNA strands through base recognition while the 5′ sequence C3AC3AC3TC 3A favors formation of a near-infrared absorbing and emitting cluster. This precursor form exclusively harbors an ∼11 silver atom cluster that absorbs at 400 nm and that condenses its single-stranded host. The 3′ recognition site associates with a complementary target strand, thereby effecting a 330 nm red-shift in cluster absorption and a background-limited recovery of cluster emission at 790 nm. One factor underlying these changes is sensor unfolding and aggregation. Variations in salt and oligonucleotide concentrations control cluster development by influencing DNA association. Structural studies using fluorescence anisotropy, fluorescence correlation spectroscopy, and size exclusion chromatography show that the sensor-cluster conjugate opens and subsequently dimerizes with hybridization. A second factor contributing to the spectral and photophysical changes is cluster transformation. Empirical silver stoichiometries are preserved through hybridization, so hybridized, dimeric near-infrared conjugates host twice the amount of silver in relation to their violet absorbing predecessors. These DNA structure and net silver stoichiometry alterations provide insight into how DNA-silver conjugates recognize analytes.

Original languageEnglish (US)
Pages (from-to)2183-2190
Number of pages8
JournalAnalytical Chemistry
Volume85
Issue number4
DOIs
StatePublished - Feb 19 2013

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Silver
Ligands
DNA
Stoichiometry
Sensors
Fluorescence
Infrared radiation
Size exclusion chromatography
Ports and harbors
Oligonucleotides
Anisotropy
Agglomeration
Salts
Association reactions
Spectroscopy
Recovery
Atoms

ASJC Scopus subject areas

  • Analytical Chemistry

Cite this

Petty, J. T., Giri, B., Miller, I. C., Nicholson, D. A., Sergev, O. O., Banks, T. M., & Story, S. P. (2013). Silver clusters as both chromophoric reporters and DNA ligands. Analytical Chemistry, 85(4), 2183-2190. https://doi.org/10.1021/ac303531y

Silver clusters as both chromophoric reporters and DNA ligands. / Petty, Jeffrey T.; Giri, Banabihari; Miller, Ian C.; Nicholson, David A.; Sergev, Orlin O.; Banks, Taylor M.; Story, Sandra P.

In: Analytical Chemistry, Vol. 85, No. 4, 19.02.2013, p. 2183-2190.

Research output: Contribution to journalArticle

Petty, JT, Giri, B, Miller, IC, Nicholson, DA, Sergev, OO, Banks, TM & Story, SP 2013, 'Silver clusters as both chromophoric reporters and DNA ligands', Analytical Chemistry, vol. 85, no. 4, pp. 2183-2190. https://doi.org/10.1021/ac303531y
Petty JT, Giri B, Miller IC, Nicholson DA, Sergev OO, Banks TM et al. Silver clusters as both chromophoric reporters and DNA ligands. Analytical Chemistry. 2013 Feb 19;85(4):2183-2190. https://doi.org/10.1021/ac303531y
Petty, Jeffrey T. ; Giri, Banabihari ; Miller, Ian C. ; Nicholson, David A. ; Sergev, Orlin O. ; Banks, Taylor M. ; Story, Sandra P. / Silver clusters as both chromophoric reporters and DNA ligands. In: Analytical Chemistry. 2013 ; Vol. 85, No. 4. pp. 2183-2190.
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