Abstract
Silicon(111) surfaces have been functionalized with mixed monolayers consisting of submonolayer coverages of immobilized 4-vinyl-2,2′-bipyridyl (1, vbpy) moieties, with the remaining atop sites of the silicon surface passivated by methyl groups. As the immobilized bipyridyl ligands bind transition metal ions, metal complexes can be assembled on the silicon surface. X-ray photoelectron spectroscopy (XPS) demonstrates that bipyridyl complexes of [Cp∗Rh], [Cp∗Ir], and [Ru(acac)2] were formed on the surface (Cp∗ is pentamethylcyclopentadienyl, acac is acetylacetonate). For the surface prepared with Ir, X-ray absorption spectroscopy at the Ir LIII edge showed an edge energy as well as post-edge features that were essentially identical with those observed on a powder sample of [Cp∗Ir(bpy)Cl]Cl (bpy is 2,2′-bipyridyl). Charge-carrier lifetime measurements confirmed that the silicon surfaces retain their highly favorable photoelectronic properties upon assembly of the metal complexes. Electrochemical data for surfaces prepared on highly doped, n-type Si(111) electrodes showed that the assembled molecular complexes were redox active. However the stability of the molecular complexes on the surfaces was limited to several cycles of voltammetry.
| Original language | English |
|---|---|
| Pages (from-to) | 15004-15012 |
| Number of pages | 9 |
| Journal | Dalton Transactions |
| Volume | 43 |
| Issue number | 40 |
| DOIs | |
| Publication status | Published - Oct 28 2014 |
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ASJC Scopus subject areas
- Inorganic Chemistry
- Medicine(all)
Cite this
Assembly, characterization, and electrochemical properties of immobilized metal bipyridyl complexes on silicon(111) surfaces. / Lattimer, Judith R C; Blakemore, James D.; Sattler, Wesley; Gul, Sheraz; Chatterjee, Ruchira; Yachandra, Vittal K.; Yano, Junko; Brunschwig, Bruce S.; Lewis, Nathan S; Gray, Harry B.
In: Dalton Transactions, Vol. 43, No. 40, 28.10.2014, p. 15004-15012.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Assembly, characterization, and electrochemical properties of immobilized metal bipyridyl complexes on silicon(111) surfaces
AU - Lattimer, Judith R C
AU - Blakemore, James D.
AU - Sattler, Wesley
AU - Gul, Sheraz
AU - Chatterjee, Ruchira
AU - Yachandra, Vittal K.
AU - Yano, Junko
AU - Brunschwig, Bruce S.
AU - Lewis, Nathan S
AU - Gray, Harry B.
PY - 2014/10/28
Y1 - 2014/10/28
N2 - Silicon(111) surfaces have been functionalized with mixed monolayers consisting of submonolayer coverages of immobilized 4-vinyl-2,2′-bipyridyl (1, vbpy) moieties, with the remaining atop sites of the silicon surface passivated by methyl groups. As the immobilized bipyridyl ligands bind transition metal ions, metal complexes can be assembled on the silicon surface. X-ray photoelectron spectroscopy (XPS) demonstrates that bipyridyl complexes of [Cp∗Rh], [Cp∗Ir], and [Ru(acac)2] were formed on the surface (Cp∗ is pentamethylcyclopentadienyl, acac is acetylacetonate). For the surface prepared with Ir, X-ray absorption spectroscopy at the Ir LIII edge showed an edge energy as well as post-edge features that were essentially identical with those observed on a powder sample of [Cp∗Ir(bpy)Cl]Cl (bpy is 2,2′-bipyridyl). Charge-carrier lifetime measurements confirmed that the silicon surfaces retain their highly favorable photoelectronic properties upon assembly of the metal complexes. Electrochemical data for surfaces prepared on highly doped, n-type Si(111) electrodes showed that the assembled molecular complexes were redox active. However the stability of the molecular complexes on the surfaces was limited to several cycles of voltammetry.
AB - Silicon(111) surfaces have been functionalized with mixed monolayers consisting of submonolayer coverages of immobilized 4-vinyl-2,2′-bipyridyl (1, vbpy) moieties, with the remaining atop sites of the silicon surface passivated by methyl groups. As the immobilized bipyridyl ligands bind transition metal ions, metal complexes can be assembled on the silicon surface. X-ray photoelectron spectroscopy (XPS) demonstrates that bipyridyl complexes of [Cp∗Rh], [Cp∗Ir], and [Ru(acac)2] were formed on the surface (Cp∗ is pentamethylcyclopentadienyl, acac is acetylacetonate). For the surface prepared with Ir, X-ray absorption spectroscopy at the Ir LIII edge showed an edge energy as well as post-edge features that were essentially identical with those observed on a powder sample of [Cp∗Ir(bpy)Cl]Cl (bpy is 2,2′-bipyridyl). Charge-carrier lifetime measurements confirmed that the silicon surfaces retain their highly favorable photoelectronic properties upon assembly of the metal complexes. Electrochemical data for surfaces prepared on highly doped, n-type Si(111) electrodes showed that the assembled molecular complexes were redox active. However the stability of the molecular complexes on the surfaces was limited to several cycles of voltammetry.
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U2 - 10.1039/c4dt01149j
DO - 10.1039/c4dt01149j
M3 - Article
VL - 43
SP - 15004
EP - 15012
JO - Dalton Transactions
JF - Dalton Transactions
SN - 1477-9226
IS - 40
ER -