One-Dimensional Delocalized Adsorbate Bloch States on a Semiconductor Surface:<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mrow><mml:mi>C</mml:mi></mml:mrow><mml:mrow><mml:mn>2</mml:mn></mml:mrow></mml:msub></mml:mrow><mml:mrow><mml:msub><mml:mrow><mml:mi>H</mml:mi></mml:mrow><mml:mrow><mml:mn>4</mml:mn></mml:mrow></mml:msub></mml:mrow><mml:mi>/</mml:mi><mml:mi>Si</mml:mi><mml:mo>(</mml:mo><mml:mn>001</mml:mn><mml:mo>)</mml:mo><mml:mi>−</mml:mi><mml:mo>

Widdra, W.; Fink, Andreas H.; Gokhale, Shubha; Trischberger, P.; Menzel, D.; Birkenheuer, U.; Gutdeutsch, U.; Rösch, Notker

doi:10.1103/physrevlett.80.4269

Cited by 70 publications

(56 citation statements)

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“…This system has been thoroughly characterized experimentally and theoretically. [13][14][15] We demonstrate that for this strongly coupled surface complex, the RIXS spectrum resulting from selective excitation into the unoccupied CSi * resonance can be interpreted with the help of density-functional ͑DF͒ calculations. In addition, we show how excitation into different resonances leads to a significant photon energy dependence of the RIXS spectral features, even though the molecule is strongly perturbed upon interaction with the substrate.…”

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confidence: 89%

“…14,15 In combination with first-principles calculations, C 2 H 4 was shown to be adsorbed on top of a Si(001)-(2ϫ1) dimer, with the C-C bond axis rotated in the surface plane by 11.4°relative to the Si-Si dimer axis. 14,15 This rotation, originally attributed to the spatial overlap of valence MO's between neighboring C 2 H 4 adsorbates, leads to the formation of a onedimensional-band-like dispersion of the 1b 2u -and 1b 1g -derived C-H bonding states along the dimer rows of the Si(001)-(2ϫ1) surface. Our recent polarization-dependent near-edge x-ray-absorption fine-structure investigation of the unoccupied adsorbate states 13 confirms the picture of the surface chemical bond derived in those earlier studies.…”

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confidence: 98%

“…The adsorption system of C 2 H 4 on Si(001)-(2 ϫ1) exhibits local C 2 symmetry according to angle-resolved UV photoemission spectroscopy ͑ARUPS͒. 14,15 In combination with first-principles calculations, C 2 H 4 was shown to be adsorbed on top of a Si(001)-(2ϫ1) dimer, with the C-C bond axis rotated in the surface plane by 11.4°relative to the Si-Si dimer axis. 14,15 This rotation, originally attributed to the spatial overlap of valence MO's between neighboring C 2 H 4 adsorbates, leads to the formation of a onedimensional-band-like dispersion of the 1b 2u -and 1b 1g -derived C-H bonding states along the dimer rows of the Si(001)-(2ϫ1) surface.…”

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confidence: 99%

“…In absorption with the electric-field vector oriented normal to the surface, two equally strong absorption resonances were observed below the ionization threshold at 285.3 eV and 286.5 eV. Assuming sp 3 hybridized carbon atoms 13,14,15 with tetrahedrally oriented bonds, the resonance at 285.3 eV was assigned to the *-derived states related to C-Si ( CSi * ) bonds.…”

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confidence: 99%

“…Due to symmetry selection rules for scattering off the C 1s core level, the RIXS spectral features with the electric-field vector in a given direction stem from C 2p-type valence orbitals oriented in the same direction. Using the known ultraviolet photoemission spectroscopy ͑UPS͒ binding energies 14 and the results of our calculations, we can assign the spectral features to the adsorbate valence level structure. MO's of free ethene are invoked to assign the UPS spectrum of the adsorption system, assuming that they contribute preferentially to the corresponding states of the coupled system.…”

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Electronic structure and screening dynamics of ethene on single-domain Si(001) from resonant inelastic x-ray scattering

et al. 2004

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We present a resonant inelastic x-ray scattering ͑RIXS͒ study of a strongly bound adsorbate on a semiconductor surface, C 2 H 4 /Si(001). The valence electronic structure as well as the photon energy dependence in RIXS can be studied without the dominating effect of dynamic metallic screening. We demonstrate that for this strongly coupled system the RIXS spectrum resulting from a selective excitation into the unoccupied CSi * resonance can be interpreted with the help of density-functional calculations. In addition, we show how excitation into different resonances leads to a significant photon energy dependence of the RIXS spectral features, not seen in strongly coupled adsorbate systems on metals. DOI: 10.1103/PhysRevB.69.153408 PACS number͑s͒: 73.20.Hb, 78.70.En The investigation of resonant inelastic scattering in the soft x-ray spectral range using third-generation synchrotron radiation sources has recently attracted great interest as a powerful method for detailed electronic structure determination.1 The inelastic-scattering process can be described as a transition from the electronic ground state of a system via an intermediate resonant core-excited state into a final state which is electronically and/or vibrationally excited. This event can be studied by either detecting scattered photons or secondary Auger electrons. The former case involving photons in the incoming as well as the outgoing channel has the advantage of being almost independent of the sample environment, thus enabling even electronic structure studies of complex interfaces and liquids. Resonant inelastic x-ray scattering ͑RIXS͒ is governed by the dipole operator, and therefore has a well-defined polarization dependence and anisotropy, which provides insight into spatial orientation and symmetry properties of the systems studied.2 Furthermore, due to the element specificity of the resonant excitation process, one is able to probe the electronic structure of complex heteronuclear systems for selected states. 1,3 In crystalline solids, momentum conservation in RIXS can be used to access the k-resolved band structure. 4 In adsorption systems, RIXS effectively suppresses contributions from the much larger number of substrate atoms and thus permits to access the atom-specific valence electronic structure of the adsorbate, 2,3,5 allowing significantly improved understanding of the surface chemical bond. 3,5 In free molecules, RIXS depends strongly on the energy of the incoming photon as a result of the interference of degenerate or near-degenerate intermediate states in the scattering process. 6 Furthermore, excitation to different resonances leads to significant differences in the spectral shape of the scattering spectra because of strong symmetry selection rules. 6 For adsorbed molecules, this situation changes because coupling to the substrate, which modifies the dynamic response of the core-hole RIXS intermediate state, has to be taken into account. To date only adsorbates on metallic substrates have been investigated with RIXS. For these...

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Electronic structure and screening dynamics of ethene on single-domain Si(001) from resonant inelastic x-ray scattering

et al. 2004

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Site‐Specific Reactivity of Ethylene at Distorted Dangling‐Bond Configurations on Si(001)

et al. 2017

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Differences in adsorption and reaction energetics for ethylene on Si(001) are reported with respect to distorted dangling-bond configurations induced by hydrogen precoverage, as obtained by DFT calculations. This can help to understand the influence of surface defects and precoverage on the reactivity of organic molecules on semiconductor surfaces in general. The results show that the reactivity of surface dimers fully enclosed by hydrogen-covered atoms is essentially unchanged compared to the clean surface. This is confirmed by scanning tunneling microscopy measurements. On the contrary, adsorption sites with partially covered surface dimers show a drastic increase in reactivity. This is due to a lowering of the reaction barrier by more than 50 % relative to the clean surface, which is in line with previous experiments. Adsorption on dimers enclosed by molecule (ethylene)-covered surface atoms is reported to have a strongly decreased reactivity, as a result of destabilization of the intermediate state due to steric repulsion; this is quantified through periodic energy decomposition analysis. Furthermore, an approach for the calculation of Gibbs energies of adsorption based on statistical thermodynamics considerations is applied to the system. The results show that the loss in molecular entropy leads to a significant destabilization of adsorption states.

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Robert‐Wichard‐Pohl‐Preis: Ultraschneller Ladungstransfer und lokalisierter Bindungsbruch: Die Kopplung von Molekülen an Oberflächen lässt sich durch die gezielte Anregung der Elektronen im Molekül charakterisieren und beeinflussen

Menzel

2000

Phys. Bl.

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Die chemische Physik der Oberflächen ist ein wichtiges Teilgebiet der Oberflächenphysik. Ihr Ziel ist ein tiefgehendes Verständnis der Veränderungen, die in Atomen und Molekülen durch deren Bindung an eine Oberfläche verursacht werden. Diese Veränderungen sind die Basis von so wichtigen Effekten wie der heterogenen Katalyse, Schichtwachstum, Reibung und Schmierung, Halbleiterstrukturierung und vielen anderen. In diesem Artikel beschreibe ich zwei neue Experimente, in denen wir die elektronische Anregung von Molekülen auf Oberflächen dazu ausnutzen, die chemischen Bindungskräfte zu studieren und zu manipulieren. Durch Anregung und Messung mit schmalbandiger Synchrotronstrahlung können wir nun chemische Reaktionen gezielt steuern.

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One-Dimensional Delocalized Adsorbate Bloch States on a Semiconductor Surface:C2H4/Si(001)−

Cited by 70 publications

References 13 publications

Electronic structure and screening dynamics of ethene on single-domain Si(001) from resonant inelastic x-ray scattering

Electronic structure and screening dynamics of ethene on single-domain Si(001) from resonant inelastic x-ray scattering

Site‐Specific Reactivity of Ethylene at Distorted Dangling‐Bond Configurations on Si(001)

Robert‐Wichard‐Pohl‐Preis: Ultraschneller Ladungstransfer und lokalisierter Bindungsbruch: Die Kopplung von Molekülen an Oberflächen lässt sich durch die gezielte Anregung der Elektronen im Molekül charakterisieren und beeinflussen

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