Magic Numbers in DNA-Stabilized Fluorescent Silver Clusters Lead to Magic Colors

Copp, Stacy M.; Schultz, Danielle M.; Swasey, Steven M.; Pavlovich, J.; Debord, Mark; Chiu, Alexander G.; Olsson, Kevin; Gwinn, E. G.

doi:10.1021/jz500146q

Cited by 140 publications

(363 citation statements)

References 43 publications

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“…Prior studies of other silver cluster-DNA conjugates attribute this difference to the loss of 6 H + from the phosphate backbone because the cluster was oxidized. 60,61 Second, the separate charge state peaks exhibited fine structure that depended on the natural abundances of 51.8% 107 Ag and 48.2% 109 Ag. The peak spacings and distributions followed a model based on the molecular formula of the oligonucleotide (C 187 H 244 O 118 N 65 P 19 ) with 10 Ag (Figure 3B and Figure S6 in the Supporting Information).…”

Section: ■ Resultsmentioning

confidence: 99%

Ten-Atom Silver Cluster Signaling and Tempering DNA Hybridization

et al. 2015

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Silver clusters with ∼10 atoms are molecules, and specific species develop within DNA strands. These molecular metals have sparsely organized electronic states with distinctive visible and near-infrared spectra that vary with cluster size, oxidation, and shape. These small molecules also act as DNA adducts and coordinate with their DNA hosts. We investigated these characteristics using a specific cluster-DNA conjugate with the goal of developing a sensitive and selective biosensor. The silver cluster has a single violet absorption band (λ(max) = 400 nm), and its single-stranded DNA host has two domains that stabilize this cluster and hybridize with target oligonucleotides. These target analytes transform the weakly emissive violet cluster to a new chromophore with blue-green absorption (λ(max) = 490 nm) and strong green emission (λ(max) = 550 nm). Our studies consider the synthesis, cluster size, and DNA structure of the precursor violet cluster-DNA complex. This species preferentially forms with relatively low amounts of Ag(+), high concentrations of the oxidizing agent O2, and DNA strands with ≳20 nucleotides. The resulting aqueous and gaseous forms of this chromophore have 10 silvers that coalesce into a single cluster. This molecule is not only a chromophore but also an adduct that coordinates multiple nucleobases. Large-scale DNA conformational changes are manifested in a 20% smaller hydrodynamic radius and disrupted nucleobase stacking. Multidentate coordination also stabilizes the single-stranded DNA and thereby inhibits hybridization with target complements. These observations suggest that the silver cluster-DNA conjugate acts like a molecular beacon but is distinguished because the cluster chromophore not only sensitively signals target analytes but also stringently discriminates against analogous competing analytes.

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Section: ■ Resultsmentioning

confidence: 99%

Ten-Atom Silver Cluster Signaling and Tempering DNA Hybridization

et al. 2015

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“…[ 47 ] Changes in the proximity of silver ions can also affect the highest occupied molecular orbital -lowest unoccupied molecular orbital (HOMO-LUMO) gap and change the photophysical properties. [ 24 ] …”

Section: Single Molecule Measurements: Antibunchingmentioning

confidence: 99%

Single‐Molecule Characterization of Near‐Infrared‐Emitting Silver Nanoclusters

Hooley

Paolucci

Liao

et al. 2015

Advanced Optical Materials

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In this paper, single molecule spectroscopy is used to probe the photophysical heterogeneity of near‐infrared emitting silver nanoclusters stabilized in single stranded DNA containing 24 cytosines (C24‐AgNCs). Focusing on this subset of emitters allows us to address and correlate their photophysical parameters. The results suggest that for these near‐infrared emitting C24‐AgNCs, the broad range of observed photophysical properties is due to the spectral heterogeneity of two species, one of which has a broad range of emission maxima and decay times. This conclusion is drawn by analyzing the results of a large number of single C24‐AgNCs where, for the first time, emission maxima, fluorescence decay times, fluorescence intensity, blinking, and photon antibunching are determined simultaneously. The single molecule measurements also reveal that some of the C24‐AgNCs can change their spectral properties during the measurement, while photon antibunching measurements verified that all the analyzed C24‐AgNCs behave as single emitters. While the overall spectral heterogeneity can be related to the immobilization in the polymer film and/or intrinsic heterogeneity of the C24‐AgNCs emitters, the exact origin of the dynamical changes has not been fully determined. However, changes in the AgNCs geometry, local environment, or changes in the DNA conformation are possible explanations.

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“…30 Gwinn's group and Dickson's group have done studies especially on short singlestranded DNA. 8,9,[33][34][35][36] Yeh, Martinez, Werner, and co-workers have carried out investigations on DNA detection probes with a greater focus on guanine bases. 12,23,[37][38][39] In addition to the experimental work, theoretical investigations have also been performed on DNA-AgNCs by several groups.…”

Section: Introductionmentioning

confidence: 99%

Research Update: Density functional theory investigation of the interactions of silver nanoclusters with guanine

2017

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Bare and guanine-complexed silver clusters Ag n z (n = 2-6; z = 0-2) are examined using density functional theory to elucidate the geometries and binding motifs that are present experimentally. Whereas the neutral systems remain planar in this size range, a 2D-3D transition occurs at Ag 5 + for the cationic system and at Ag 4 2+ for the dicationic system. Neutral silver clusters can bind with nitrogen 3 or with the pi system of the base. However, positively charged clusters interact with nitrogen 7 and the neighboring carbonyl group. Thus, the cationic silver-DNA clusters present experimentally may preferentially interact at these sites. © 2017 Author (s)

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Magic Numbers in DNA-Stabilized Fluorescent Silver Clusters Lead to Magic Colors

Cited by 140 publications

References 43 publications

Ten-Atom Silver Cluster Signaling and Tempering DNA Hybridization

Ten-Atom Silver Cluster Signaling and Tempering DNA Hybridization

Single‐Molecule Characterization of Near‐Infrared‐Emitting Silver Nanoclusters

Research Update: Density functional theory investigation of the interactions of silver nanoclusters with guanine

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