Impact of Ice Structure on Ultrafast Electron Dynamics in<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msub><mml:mi mathvariant="normal">D</mml:mi><mml:mn>2</mml:mn></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:math>Clusters on Cu(111)

Stähler, Julia; Mehlhorn, Michael; Bovensiepen, Uwe; Meyer, Michael; Kusmierek, D. O.; Morgenstern, Karina; Wolf, Martin

doi:10.1103/physrevlett.98.206105

Cited by 47 publications

(52 citation statements)

References 18 publications

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“…We now discuss the time-dependent evolution of the binding energy and the population decay, which has been observed in the fs to ps range at amorphous ice-metal interfaces 24,34,40 and in liquid water, 42 where it has been attributed to dynamical screening during the solvated electron formation. However, for crystalline ice on Ru(001), we observe a localized state (e T ) stabilized by 1 eV with respect to the delocalized state (n ) 1) ( Figure 3).…”

Section: Thermally Activated Relaxation Among Conformational Substatesmentioning

confidence: 99%

A Dynamic Landscape from Femtoseconds to Minutes for Excess Electrons at Ice−Metal Interfaces

et al. 2008

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Stabilization of excess electrons is studied at crystalline ice-metal interfaces by femtosecond time-resolved two-photon photoelectron spectroscopy and ab initio calculations. Following optical excitation into delocalized image potential states, electrons localize at pre-existing defects which are located at the ice-vacuum interface. Remarkably, the stabilization of these trapped electrons is monitored continuously from femtoseconds up to minutes. By first principle calculations we identify defect structures, that support excess electrons in front of crystalline ice surfaces, and suggest that the stabilization proceeds through subsequent conformational substates. The excess electron wave functions are efficiently screened from the underlying bulk and explain the long residence times observed in the experiment. Thereby, we shed light on the collective character of the nuclear rearrangement that determines the energetics over all timescales.

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Section: Thermally Activated Relaxation Among Conformational Substatesmentioning

confidence: 99%

A Dynamic Landscape from Femtoseconds to Minutes for Excess Electrons at Ice−Metal Interfaces

et al. 2008

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“…The ultrafast dynamics of electrons photoinjected into thin water-ice films on metal substrates were studied in detail by Bovensiepen and co-workers. [7][8][9] They found that electron transfer from the optically excited substrate into the ice conduction band was followed by solvation leading to electron localization on an ultrafast time scale. The solvated electrons were reported to have picosecond lifetimes, mainly limited by tunneling back to the metal substrate.…”

Section: Introductionmentioning

confidence: 99%

“…Significantly, the electron lifetime was found to be morphology dependent, with evidence that the electron was localized at the ice-vacuum interface for water-ice clusters on metal substrates. 9 Sanche and co-workers studied the effect of electron attachment to water-ice films following lowenergy electron bombardment. 3,10,11 They found that the solvated electrons formed following attachment from the gas phase have relatively long lifetimes, and support a variety of chemical reactions, including dissociative electron attachment to halocarbons.…”

Section: Introductionmentioning

confidence: 99%

Photoelectric emission from the alkali metal doped vacuum-ice interface

Vondrak

Meech

Plane

2009

The Journal of Chemical Physics

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The photoelectron photoemission spectra and thresholds for low coverages of Li and K adsorbed on water-ice have been measured, compared with photoionization spectra of the gas-phase atoms, and modeled by quantum chemical calculations. For both alkali metals the threshold for photoemission is dramatically decreased and the cross section increased on adsorption to the water-ice surface. Quantum chemical calculations suggest that the initial state is formed by the metal atoms adsorbed into the water-ice surface, forming a state with a delocalized electron distribution. This state is metastable and decays on the hundreds of seconds time scale at 92 K. The decay is markedly faster for Li than for K, probably due to diffusion into the ice film.

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“…15,16 UHV studies of electron population dynamics, energy relaxation, band structure and localization phenomena are commonplace for a large variety of metal-dielectric interfaces using two-photon photoemission (2PPE). [17][18][19][20][21] 2PPE can access interfacial electronic states and track the dielectric response of adsorbed thin films. A sub-hundred femtosecond pulse and its second harmonic impinge upon an Ag substrate with a controllable time delay of femtoseconds to picoseconds between pulses.…”

Section: Introductionmentioning

confidence: 99%

The Ultrafast Dynamics of Image Potential State Electrons at the Dimethylsulfoxide/Ag(111) Interface

et al. 2008

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Angle-resolved two-photon photoemission was used to study the energy relaxation, population decay and localization dynamics of image potential state (IPS) electrons in ultrathin films of dimethylsulfoxide (DMSO) on an Ag(111) substrate. Dynamic energy shifts of 50 ± 10 meV and 220 ± 10 meV were observed for n=1 IPS electrons at one monolayer and two monolayer coverages of DMSO, respectively. The difference in energy shifts is attributed to rotational hindrance of the molecular dipole in the chemisorptive first monolayer. The finding confirms the proposed mechanism for the low differential capacitance of dimethylsulfoxide at noble metal interfaces in solution. A novel description of the IPS as a surface capacitance is presented to facilitate comparisons with electrochemical systems.

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Impact of Ice Structure on Ultrafast Electron Dynamics inD2OClusters on Cu(111)

Cited by 47 publications

References 18 publications

A Dynamic Landscape from Femtoseconds to Minutes for Excess Electrons at Ice−Metal Interfaces

A Dynamic Landscape from Femtoseconds to Minutes for Excess Electrons at Ice−Metal Interfaces

Photoelectric emission from the alkali metal doped vacuum-ice interface

The Ultrafast Dynamics of Image Potential State Electrons at the Dimethylsulfoxide/Ag(111) Interface

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