Hydrogen adsorption on an open metal surface:<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mrow><mml:mi mathvariant="normal">H</mml:mi></mml:mrow><mml:mrow><mml:mn>2</mml:mn></mml:mrow></mml:msub></mml:mrow><mml:mo>/</mml:mo><mml:mi mathvariant="normal">Pd</mml:mi><mml:mn /><mml:mo>(</mml:mo><mml:mn>210</mml:mn><mml:mo>)</mml:mo><mml:mn /></mml:math>

Lischka, Markus; Groß, Axel

doi:10.1103/physrevb.65.075420

Cited by 91 publications

(62 citation statements)

References 43 publications

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“…Note, that this downshift is not caused by the interaction of the two additional hydrogen atoms with Pd. Atomic hydrogen adsorption hardly changes the LDOS of Pd, as our and previous [21] calculations confirm. It has to be pointed out that the relative intensities of the synthetic valence band spectrum are not well reproduced, which might be attributable to matrix element effects present in the photoemission process.…”

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confidence: 80%

Chemical Interactions at Metal/Molecule Interfaces in Molecular Junctions—A Pathway Towards Molecular Recognition

et al. 2009

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Small organic molecules as potential building-blocks for future nanoelectronic devices [1][2][3][4][5] will require new types of sensors able to identify/quantify molecules in appropriate solutions on a single-molecule level. Recently, an elegant new method has been proposed [6] that allows detection of small aromatic units like 4-aminothiophenol (4-ATP) molecules by measuring the tunneling resistance between two metal electrodes separated by a short distance (a few nanometers). While, from a simple point of view, an increase in conductivity should be expected because of the bridging of the tunnelling gap by one or more molecules (thus offering molecular orbitals as additional transport channels), a decreased conductivity was observed experimentally with a reduction factor that depended on the type of molecule present in the solution. Here, we report on combined experimental and theoretical efforts aimed at unravelling this phenomenon by studying the electronic properties of one of the metal electrodes in such a molecular junction.For this purpose, a 4-ATP self-assembled monolayer (SAM) has been prepared on top of a Au(111) crystal, which, in a second step, has been metallized by a nearly closed Pd overlayer of monoatomic height by means of a recently developed electrochemical approach. [7][8][9][10] Photoelectron spectroscopy together with density functional theory (DFT) taking into account all contributing parts of the molecular junction finally allowed analysis of its structural setup and its electronic properties. Angle-resolved X-ray photoelectron spectroscopy (XPS) reveals that the 4-ATP SAM actually consists of a minimum of two molecular layers. Most importantly, using ultraviolet photoelectron spectroscopy (UPS) and DFT simulations, strong chemical interactions between the metal overlayer and the amino groups are found to play a decisive role in determining the overall electronic properties, and thus the transport properties of the SAM/metal contact, as will be demonstrated in the following.It is well-known that 4-ATP has a strong tendency to form multilayers on Au(111), which lead to scanning tunnelling microscopy (STM) images with considerable height variations and of blurred contrast when it comes to molecular-scale resolution.[11] Even for highly diluted solutions (sub-millimolar concentrations of the 4-ATP), more than just one layer is generally formed. On the other hand, reductive desorption of thiols from gold surfaces is known to occur at electrode potentials negative of À0.1 V vs. standard calomel electrode (SCE), which may be considered an appropriate means for desolving any thiol in excess of the first layer.[12] In Figure 1 cyclic voltammograms are shown for Au(111) in 0.1 M H 2 SO 4 , after the electrode had been immersed for 15 min in a 0.1 Â 10 À3 M 4-ATP/0.1 M H 2 SO 4 modification solution. While the first cycle (dash-dotted line, start at þ0.2 V vs. SCE in the negative direction) was restricted to the stability range of the 4-ATP adlayer, i.e., 0 and þ0.4 V, the second cycle (solid line)...

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Chemical Interactions at Metal/Molecule Interfaces in Molecular Junctions—A Pathway Towards Molecular Recognition

et al. 2009

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“…The first labels indicate the adsorption energy in a descending order ͑see also Table IV below͒ and the label in parentheses gives the coordination of the S atom at the particular site. Ϫ6.1% Ϫ4.8% Ϫ11.6% Ϫ6.5% ⌬d 5,6 Ϫ2.0% ϩ0.2% ϩ22.8% ϩ18.5% ⌬d 6,7 ϩ3.6% Ϫ8.2% Ϫ6.9% ⌬d 7,8 Ϫ2.7% Ϫ3.1% Ϫ1.7% ⌬d 8,9 ϩ0.0% ϩ6.3% ϩ2.8%…”

Section: Energetics and Relaxations Of Stepped Pd Surfacesmentioning

confidence: 99%

“…7. Relaxations have been considered for the steps on the Pt͑111͒ surface 35,36 and on different Cu surfaces.…”

Section: Energetics and Relaxations Of Stepped Pd Surfacesmentioning

confidence: 99%

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Ab initiostudies of stepped Pd surfaces with and without S

et al. 2003

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We have performed a comprehensive first-principles study of the electronic and geometric structure of a set of clean and S covered vicinal Pd surfaces of ͑111͒ and ͑110͒, namely Pd͑211͒, Pd͑331͒, Pd͑320͒, and Pd͑551͒, each having three-atom wide terraces. The trends in the multilayer relaxation patterns can generally be explained on the basis of charge smoothening which makes the vicinals of Pd͑110͒ prone to larger and deeper relaxations in comparison to the Pd͑111͒ counterparts. A range of adsorption energies for preferred adsorption sites for S is found on all four surfaces, with Pd͑320͒ being the most receptive. We show that the adsorbate can have considerable effect on multilayer relaxations and registry of the substrate atoms. We discuss the nature of the S-Pd bonding and how this bonding is affected by the surface geometry and coordination. We relate the poisoning effect of S to the changes in the electronic structure of the substrate atoms.

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“…Very few exceptions concern Pd (210) [14,15], Pd (311) [16][17][18] and Pd(211) [19]. Despite the general tendency of hydrogen atoms to occupy highly coordinated sites is also preserved on the stepped surfaces, it was shown that the highest energy was not always related to a hydrogen atom being adsorbed on the highest coordinated site [15,19]. In addition, there is a strong need to distinguish between the sites with even the same coordination number as not all of them are equivalent [19].…”

Section: Introductionmentioning

confidence: 99%

Hydrogen adsorption on Pd(133) surface

Tomaszewska

StÄTMpieÅ„

2009

Open Physics

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Abstract:An approach based on measurements of the total energy distribution (TED) of field emitted electrons is used in order to examine properties of the Pd(133) from the aspect of hydrogen adsorption. The most favourable sites offered to a hydrogen atom to be adsorbed are indicated and an attempt to ascribe the peaks of the enhancement factor R in the TED spectrum to the specific adsorption sites is made.PACS (2008)

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Hydrogen adsorption on an open metal surface:H2/Pd(210)

Cited by 91 publications

References 43 publications

Chemical Interactions at Metal/Molecule Interfaces in Molecular Junctions—A Pathway Towards Molecular Recognition

Chemical Interactions at Metal/Molecule Interfaces in Molecular Junctions—A Pathway Towards Molecular Recognition

Ab initiostudies of stepped Pd surfaces with and without S

Hydrogen adsorption on Pd(133) surface

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