Nanoscale Phase Segregation of Mixed Thiolates on Gold Nanoparticles

Harkness, Kellen M.; Baliński, A.; McLean, John A.; Cliffel, David E.

doi:10.1002/anie.201102882

Cited by 80 publications

(116 citation statements)

References 42 publications

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“…19 In a separate work, a power spectral density method to analyze these images has been developed, and it has established that identical information can be extracted from images taken in different laboratories, further confirming the validity of these images. 20 The existence of patchy ligand shell morphology has also been supported by atomic force microscopy, 5 infrared spectroscopy, 21 nuclear magnetic resonance spectroscopy, 22,23 matrix-assisted laser desorption/ionization ion mobility mass spectrometry (MALDI-IM-MS), 24 and electron spin resonance (ESR) spectroscopy. 25, 26 Glotzer and co-workers have shown through coarsegrained and molecular dynamics simulations that the stripe morphology forms because of an interplay between the enthalpy of phase separation and a conformational entropy that arises when longer molecules are at a domain boundary with shorter ones.…”

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confidence: 99%

High-Resolution Scanning Tunneling Microscopy Characterization of Mixed Monolayer Protected Gold Nanoparticles

et al. 2013

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Gold nanoparticles protected by a binary mixture of thiolate molecules have a ligand shell that can spontaneously separate into nanoscale domains. Complex morphologies arise in such ligand shells, including striped, patchy, and Janus domains. Characterization of these morphologies remains a challenge. Scanning tunneling microscopy (STM) imaging has been one of the key approaches to determine these structures, yet the imaging of nanoparticles' surfaces faces difficulty stemming from steep surface curvature, complex molecular structures, and the possibility of imaging artifacts in the same size range. Images obtained to date have lacked molecular resolution, and only domains have been resolved. There is a clear need for images that resolve the molecular arrangement that leads to domain formation on the ligand shell of these particles. Herein we report an advance in the STM imaging of gold nanoparticles, revealing some of the molecules that constitute the domains in striped and Janus gold nanoparticles. We analyze the images to determine molecular arrangements on parts of the particles, highlight molecular "defects" present in the ligand shell, show persistence of the features across subsequent images, and observe the transition from quasi-molecular to domain resolution. The ability to resolve single molecules in the ligand shell of nanoparticles could lead to a more comprehensive understanding of the role of the ligand structure in determining the properties of mixed-monolayer-protected gold nanoparticles.

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High-Resolution Scanning Tunneling Microscopy Characterization of Mixed Monolayer Protected Gold Nanoparticles

et al. 2013

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“…Previous studies have suggested that bidentate ligands, each end being in a dynamic equilibrium with the solution phase, will eventually migrate into positions corresponding to the minimal point of the conformational potential energy surface for the epitope. 51,67,68 This phenomenon, which could take place through lateral translation of thiol termini or through a series of dissociative and associative steps, should eventually allow for large, multidentate structures to adopt a structure which should be similar to a native structure.…”

Section: Biomimicry Of Native Antigens On Aunps In Vitromentioning

confidence: 99%

Biomimetic monolayer-protected gold nanoparticles for immunorecognition

et al. 2012

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Gold nanoparticles (AuNPs) protected by self-assembled monolayers (SAMs) are capable of presenting precisely engineered surfaces at the nanoscale, allowing the mimicry of biomacromolecules on an artificial platform. Here we review the generation, characterization, and applications of monolayer-protected AuNPs that have been designed for immunorecognition by the integration of an oligopeptide epitope into the protecting monolayer. The resulting peptide-AuNP conjugate is an effective platform for biomimesis, as demonstrated by multiple studies. Recent work is presented and future directions for this field of research are discussed.

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“…Different techniques have shown their existence, including high-resolution scanning tunnelling microscopy (STM) [17], NMR [18], mass spectrometry [19] and neutron scattering [20]. The formation of narrow nanodomains is believed to be due to an entropic contribution arising from the mixing of ligand molecules of different lengths and bulkiness at the nanoparticle surfaces.…”

Section: Introductionmentioning

confidence: 99%

Co-precipitation of oppositely charged nanoparticles: the case of mixed ligand nanoparticles

Moglianetti¹,

Ponomarev²,

Szybowski³

et al. 2015

J. Phys. D: Appl. Phys.

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Colloid stability is of high importance in a multitude of fields ranging from food science to biotechnology. There is strong interest in studying the stability of small particles (of a size of a few nanometres) with complex surface structures, that make them resemble the complexity of proteins and other natural biomolecules, in the presence of oppositely charged nanoparticles. While for nanoparticles with homogeneously charged surfaces an abrupt precipitation has been observed at the neutrality of charges, data are missing about the stability of nanoparticles when they have more complex surface structures, like the presence of hydrophobic patches. To study the role of these hydrophobic patches in the stability of nanoparticles a series of negatively charged nanoparticles has been synthesized with different ratios of hydrophobic content and with control on the structural distribution of the hydrophobic moiety, and then titrated with positively charged nanoparticles. For nanoparticles with patchy nanodomains, the influence of hydrophobic content was observed together with the influence of the size of the nanoparticles. By contrast, for nanoparticles with a uniform distribution of hydrophobic ligands, size changes and hydrophobic content did not play any role in co-precipitation behaviour. A comparison of these two sets of nanoparticles suggests that nanodomains present at the surfaces of nanoparticles are playing an important role in stability against co-precipitation.

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Nanoscale Phase Segregation of Mixed Thiolates on Gold Nanoparticles

Cited by 80 publications

References 42 publications

High-Resolution Scanning Tunneling Microscopy Characterization of Mixed Monolayer Protected Gold Nanoparticles

High-Resolution Scanning Tunneling Microscopy Characterization of Mixed Monolayer Protected Gold Nanoparticles

Biomimetic monolayer-protected gold nanoparticles for immunorecognition

Co-precipitation of oppositely charged nanoparticles: the case of mixed ligand nanoparticles

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