Dynamic Diglyme-Mediated Self-Assembly of Gold Nanoclusters

W. Scott Compel; O. Andrea Wong; Xi Chen; Chongyue Yi; Roy Geiss; Hannu Häkkinen; Kenneth L. Knappenberger; Christopher J. Ackerson

doi:10.1021/acsnano.5b02850

Dynamic Diglyme-Mediated Self-Assembly of Gold Nanoclusters

W. Scott Compel, O. Andrea Wong, Xi Chen, Chongyue Yi, Roy Geiss, Hannu Häkkinen, Kenneth L. Knappenberger, Christopher J. Ackerson

Chemistry

Research output: Contribution to journal › Article › peer-review

35 Scopus citations

Abstract

We report the assembly of gold nanoclusters by the nonthiolate ligand diglyme into discrete and dynamic assemblies. To understand this surprising phenomenon, the assembly of Au₂₀(SC₂H₄Ph)₁₅-diglyme into Au₂₀(SC₂H₄Ph)₁₅-diglyme-Au₂₀(SC₂H₄Ph)₁₅ is explored in detail. The assembly is examined by high-angle annular dark field scanning transmission electron microscopy, size exclusion chromatography, mass spectrometry, IR spectroscopy, and calorimetry. We establish a dissociation constant for dimer to monomer conversion of 20.4 μM. Theoretical models validated by transient absorption spectroscopy predict a low-spin monomer and a high-spin dimer, with assembly enabled through weak diglyme oxygen-gold interactions. Close spatial coupling allows electron delocalization between the nanoparticle cores. The resulting assemblies thus possess optical and electronic properties that emerge as a result of assembly.

Original language	English (US)
Pages (from-to)	11690-11698
Number of pages	9
Journal	ACS nano
Volume	9
Issue number	12
DOIs	https://doi.org/10.1021/acsnano.5b02850
State	Published - Nov 3 2015

All Science Journal Classification (ASJC) codes

General Materials Science
General Engineering
General Physics and Astronomy

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10.1021/acsnano.5b02850

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title = "Dynamic Diglyme-Mediated Self-Assembly of Gold Nanoclusters",

abstract = "We report the assembly of gold nanoclusters by the nonthiolate ligand diglyme into discrete and dynamic assemblies. To understand this surprising phenomenon, the assembly of Au20(SC2H4Ph)15-diglyme into Au20(SC2H4Ph)15-diglyme-Au20(SC2H4Ph)15 is explored in detail. The assembly is examined by high-angle annular dark field scanning transmission electron microscopy, size exclusion chromatography, mass spectrometry, IR spectroscopy, and calorimetry. We establish a dissociation constant for dimer to monomer conversion of 20.4 μM. Theoretical models validated by transient absorption spectroscopy predict a low-spin monomer and a high-spin dimer, with assembly enabled through weak diglyme oxygen-gold interactions. Close spatial coupling allows electron delocalization between the nanoparticle cores. The resulting assemblies thus possess optical and electronic properties that emerge as a result of assembly.",

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AU - Compel, W. Scott

AU - Wong, O. Andrea

AU - Chen, Xi

AU - Yi, Chongyue

AU - Geiss, Roy

AU - Häkkinen, Hannu

AU - Knappenberger, Kenneth L.

AU - Ackerson, Christopher J.

PY - 2015/11/3

Y1 - 2015/11/3

N2 - We report the assembly of gold nanoclusters by the nonthiolate ligand diglyme into discrete and dynamic assemblies. To understand this surprising phenomenon, the assembly of Au20(SC2H4Ph)15-diglyme into Au20(SC2H4Ph)15-diglyme-Au20(SC2H4Ph)15 is explored in detail. The assembly is examined by high-angle annular dark field scanning transmission electron microscopy, size exclusion chromatography, mass spectrometry, IR spectroscopy, and calorimetry. We establish a dissociation constant for dimer to monomer conversion of 20.4 μM. Theoretical models validated by transient absorption spectroscopy predict a low-spin monomer and a high-spin dimer, with assembly enabled through weak diglyme oxygen-gold interactions. Close spatial coupling allows electron delocalization between the nanoparticle cores. The resulting assemblies thus possess optical and electronic properties that emerge as a result of assembly.

AB - We report the assembly of gold nanoclusters by the nonthiolate ligand diglyme into discrete and dynamic assemblies. To understand this surprising phenomenon, the assembly of Au20(SC2H4Ph)15-diglyme into Au20(SC2H4Ph)15-diglyme-Au20(SC2H4Ph)15 is explored in detail. The assembly is examined by high-angle annular dark field scanning transmission electron microscopy, size exclusion chromatography, mass spectrometry, IR spectroscopy, and calorimetry. We establish a dissociation constant for dimer to monomer conversion of 20.4 μM. Theoretical models validated by transient absorption spectroscopy predict a low-spin monomer and a high-spin dimer, with assembly enabled through weak diglyme oxygen-gold interactions. Close spatial coupling allows electron delocalization between the nanoparticle cores. The resulting assemblies thus possess optical and electronic properties that emerge as a result of assembly.

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Dynamic Diglyme-Mediated Self-Assembly of Gold Nanoclusters

Abstract

All Science Journal Classification (ASJC) codes

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