Journal
NANO LETTERS
Volume 17, Issue 7, Pages 4443-4452Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.7b01593
Keywords
Surface capping ligands; metallic nanoparticles; nanoscale surface curvature; plasmon-enhanced spectroscopy; ligand dynamics; ligand exchange
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Funding
- National Science Foundation CAREER Award [DMR-1253231]
- ASPIRE-I Track-I Award from the University of South Carolina (USC) Office of Vice President for Research
- GAANN Fellowship by the Department of Education through GAANN [P200A120075]
- SPARC Graduate Research Grant from the USC Office of the Vice President for Research
- Dissertation Fellowship from USC NanoCenter
- Jiangsu University Study-Abroad Funds [20162673]
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1253231] Funding Source: National Science Foundation
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The interfacial adsorption, desorption, and exchange behaviors of thiolated ligands on nanotextured Au nanoparticle surfaces exhibit phenomenal site-to-site variations essentially dictated by the local surface curvatures, resulting in heterogeneous thermodynamic and kinetic profiles remarkably more sophisticated than those associated with the self-assembly of organothiol ligand monolayers on atomically flat Au surfaces. Here we use plasmon-enhanced Raman scattering as a spectroscopic tool combining time-resolving and molecular fingerprinting capabilities to quantitatively correlate the ligand dynamics with detailed molecular structures in real time under a diverse set of ligand adsorption, desorption, and exchange conditions at both equilibrium and nonequilibrium states, which enables us to delineate the effects of nanoscale surface curvature on the binding affinity, cooperativity, structural ordering, and the adsorption/desorption/exchange kinetics of organothiol ligands on colloidal Au nanoparticles. This work provides mechanistic insights on the key thermodynamic, kinetic) and geometric factors underpinning the surface curvature-dependent interfacial ligand behaviors, which serve, as a central knowledge framework guiding the site-selective incorporation of desired surface functionalities into individual metallic nanoparticles for specific applications.
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