Molecule Length-Induced Reentrant Self-Organization of Alkanes in Monolayers Adsorbed on Au(111)

Marchenko, Alexandr; Cousty, J.

doi:10.1103/physrevlett.84.5363

Cited by 80 publications

(91 citation statements)

References 17 publications

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“…1b) recorded in 1-phenyloctane solvent (for spacer-layer-stability tests see Supplementary Section 1.2). The average length of an individual n-C 30 H 62 unit is (3.75 ± 0.05) nm, calculated from the in situ STM topographs and is in agreement with previous STM reports on identical systems 25,26 . The van der Waals binding energy between the alkyl-spacer and Au(111) calculated from molecular dynamics structures (Fig.…”

Section: Organic Spacer/gold Interaction In Liquidssupporting

confidence: 77%

“…We further show that the organic spacer layer combined with in situ spectroscopy can sense energy-level shifts (energy resolution ∼50 meV) in chemically tailored molecules, which are rationalized using density functional theory (DFT) calculations. Importantly, the organic spacer serves as an intermediate cushioning layer that prevents metal-induced topological defects in single-layer graphene, thus opening a route towards engineering ultraflat two-dimensional nanostructures on metal supports.Organic spacer/gold interaction in liquids n-C 30 H 62 (solubilized in 1-phenyloctane) spray-deposited on Au(111) (Methods) at room temperature 24 forms close-packed two-dimensional lamellar structures 25,26 . The formation of ordered alkyl-organic layers and their lower dielectric constant (∼2) in comparison with inorganic spacers (NaCl, ε:∼6) make them…”

mentioning

confidence: 99%

“…Organic spacer/gold interaction in liquids n-C 30 H 62 (solubilized in 1-phenyloctane) spray-deposited on Au(111) (Methods) at room temperature 24 forms close-packed two-dimensional lamellar structures 25,26 . The formation of ordered alkyl-organic layers and their lower dielectric constant (∼2) in comparison with inorganic spacers (NaCl, ε:∼6) make them…”

mentioning

confidence: 99%

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Nanoelectrical analysis of single molecules and atomic-scale materials at the solid/liquid interface

et al. 2014

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Evaluating the built-in functionality of nanomaterials under practical conditions is central for their proposed integration as active components in next-generation electronics. Low-dimensional materials from single atoms to molecules have been consistently resolved and manipulated under ultrahigh vacuum at low temperatures. At room temperature, atomic-scale imaging has also been performed by probing materials at the solid/liquid interface. We exploit this electrical interface to develop a robust electronic decoupling platform that provides precise information on molecular energy levels recorded using in situ scanning tunnelling microscopy/spectroscopy with high spatial and energy resolution in a high-density liquid environment. Our experimental findings, supported by ab initio electronic structure calculations and atomic-scale molecular dynamics simulations, reveal direct mapping of single-molecule structure and resonance states at the solid/liquid interface. We further extend this approach to resolve the electronic structure of graphene monolayers at atomic length scales under standard room-temperature operating conditions.T he elemental properties of carbon nanostructures are environment dependent. Interpreting the synergism between electronically active nanomaterials and their local chemical domain is pivotal to both scientific and technological interests. Scanning probe microscopy operated at cryogenic conditions with functionalized metal tips 1,2 in combination with inorganic decoupling platforms 3,4 is a widely adopted technique to examine the intramolecular structure of organic materials. In addition to probing matter under ultrahigh-vacuum conditions, scanning tunnelling microscopy (STM) operated at the solid/liquid interface 5-11 has previously been demonstrated to record real-time molecular dynamics 7,12-14 , register ultrafast chemical reactions 8,15 , probe the structure of supra-molecular architectures [16][17][18] and chemical-fieldeffect transistors 19 , and perform spectral analysis of molecules 6,13,20 and real-space visualization of biomolecules 5 at room temperature. It would be highly attractive to capitalize on principal findings from these two research disciplines to probe the precise electronic states in liquids and quantitatively describe the functionality of single molecules and two-dimensional nanostructures. The experimental challenge lies in addressing the electrochemical congestion present at the solid/liquid electrical interface at room temperature, which stems from the high mobility of organic molecules on metals, the dynamics of the solvent that serves as a liquid sheath and the detrimental effects of the metallic platform due to mixing of metal bands with discrete molecular electronic states 21 . A potential strategy is to employ nonpolar, highly viscous liquid sheaths with low affinity towards the substrate and to engineer a spacer layer 3,22,23 that electrically disconnects the organic material of interest from metal-induced perturbations. The bottom-up construction of the spac...

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Section: Organic Spacer/gold Interaction In Liquidssupporting

confidence: 77%

mentioning

confidence: 99%

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Nanoelectrical analysis of single molecules and atomic-scale materials at the solid/liquid interface

et al. 2014

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“…In contrast, long alkyl chains adsorbed on inert surfaces such as a graphite basal plane and Au(111) surface are flat-lying and form a self-assembled lamellar structure [5][6][7][8][9][10][11]. The SAMs of these lamellar structures are expected to show a different class of functionalities.…”

Section: Introductionmentioning

confidence: 99%

Cyclic Voltammetry and in situ Infrared Reflection Absorption Spectroscopy on Kinetic Effect of Physisorbed Dioctadecylsulfide on a Cu-UPD Process on Au(111) Electrode Surface

Endō

Ozaki

Nakamura

et al. 2018

e-J. Surf. Sci. Nanotech.

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The presence of a self-assembled monolayer (SAM) of dioctadecyl sulfide (DOS) on a Au(111) electrode affects the underpotential deposition (UPD) of copper in sulfuric acid solution. The first stage of the UPD, i.e., formation of the• lattice comprising the honeycomb structure of copper, is delayed by the DOS SAM of the lower-density phase, in which the chain axis is parallel to the surface. Neutral molecules are preferentially adsorbed on the Au(111) electrode surface at around the potential of zero charge (pzc), which is approximately −0.1 V (vs. Hg|Hg2SO4) in sulfuric acid solution. The adsorption of copper ions at this potential is inhibited by the DOS SAM, which delays the successive Cu-UPD process in the first stage. In contrast, the DOS SAM of the higher-density phase, in which the chain axis is standing upright, inhibits the entire UPD process.

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“…1(a) [5][6][7][8][9]. Flat-lying alkyl chains are in contact with the substrate with the entire molecule.…”

Section: Introductionmentioning

confidence: 99%

n-Alkane Monolayer on a Au(111) Template for Metal Growth

Endō

Ozaki

Nakamura

et al. 2015

e-J. Surf. Sci. Nanotech.

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The growth of gold on top of a n-alkane monolayer, which consists of lamellar assemblies with close-packed flat-lying chains, is observed by using scanning tunneling microscopy. The n-alkane monolayer sustains gold atoms, and penetration of the atoms into the monolayer is inhibited. The molecular conformation is unaffected and the arrangement is only slightly changed upon deposition of the gold atoms. Two-dimensional clusters are grown and a smooth monolayer is finally obtained.

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Molecule Length-Induced Reentrant Self-Organization of Alkanes in Monolayers Adsorbed on Au(111)

Abstract: We report the observation by scanning tunneling microscopy of the reentrant self-organization of n-alkanes (C(n)H(2n+2)) in monolayers adsorbed on Au(111) induced by a variation of the chain length. In the investigated range of lengths ( 10 Show more

Cited by 80 publications

References 17 publications

Nanoelectrical analysis of single molecules and atomic-scale materials at the solid/liquid interface

Nanoelectrical analysis of single molecules and atomic-scale materials at the solid/liquid interface

Cyclic Voltammetry and <i>in situ</i> Infrared Reflection Absorption Spectroscopy on Kinetic Effect of Physisorbed Dioctadecylsulfide on a Cu-UPD Process on Au(111) Electrode Surface

<i>n</i>-Alkane Monolayer on a Au(111) Template for Metal Growth<i><sup> </sup></i>

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