Decay mechanisms of excited electrons in quantum-well states of ultrathin Pb islands grown on Si(111): Scanning tunneling spectroscopy and theory

Hong, I-Po; Brun, Christophe; Patthey, F.; Sklyadneva, I. Yu.; Zubizarreta, X.; Heid, R.; Silkin, V. M.; Echenique, Pedro M.; Bohnen, K.‐P.; Chulkov, Eugene V.; Schneider, W. D.

doi:10.1103/physrevb.80.081409

Cited by 53 publications

(71 citation statements)

References 34 publications

(31 reference statements)

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“…Another remarkable feature of the Pb overlayer systems is the Fermi-liquid behavior of the excited electrons starting from a single Pb monolayer (54,55). This is corroborated by relativistic calculations of the e-e contribution for bulk Pb, especially for the parent band of the Pb(111) QWSs, the bulk band which crosses E F along the ΓL direction.…”

Section: Confinement Effects In Electron Dynamicssupporting

confidence: 53%

“…This is corroborated by relativistic calculations of the e-e contribution for bulk Pb, especially for the parent band of the Pb(111) QWSs, the bulk band which crosses E F along the ΓL direction. Even the inclusion of the e-ph contribution to the lifetime broadening of excited states at relatively low temperatures does not deviate the lifetime broadening from the quadratic dependence on energy (54). This dependence can be explained by strong screening effects in Pb systems.…”

Section: Confinement Effects In Electron Dynamicsmentioning

confidence: 85%

“…Theoretical calculations have also addressed these systems (54,56). Experimentally, it was shown that the lowest electron excited state energy oscillates with the Pb film thickness, leading to strong oscillations in the electron-electron (e-e) (55) and elec- tron-phonon (e-ph) (54) scattering contributions to the lifetime broadening.…”

Section: Confinement Effects In Electron Dynamicsmentioning

confidence: 99%

“…Recently, a model overlayer system, namely Pb(111) overlayers on Si(111) and Cu(111), was studied by scanning tunneling (54) and two-phototon photoemission (55) techniques. Theoretical calculations have also addressed these systems (54,56).…”

Section: Confinement Effects In Electron Dynamicsmentioning

confidence: 99%

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Time-dependent electron phenomena at surfaces

Muiño

Sánchez‐Portal

Silkin

et al. 2010

Proc. Natl. Acad. Sci. U.S.A.

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Femtosecond and subfemtosecond time scales typically rule electron dynamics at metal surfaces. Recent advance in experimental techniques permits now remarkable precision in the description of these processes. In particular, shorter time scales, smaller system sizes, and spin-dependent effects are current targets of interest. In this article, we use state-of-the-art theoretical methods to analyze these refined features of electron dynamics. We show that the screening of localized charges at metal surfaces is created locally in the attosecond time scale, while collective excitations transfer the perturbation to larger distances in longer time scales. We predict that the elastic width of the resonance in excited alkali adsorbates on ferromagnetic surfaces can depend on spin orientation in a counterintuitive way. Finally, we quantitatively evaluate the electron-electron and electron-phonon contributions to the electronic excited states widths in ultrathin metal layers. We conclude that confinement and spin effects are key factors in the behavior of electron dynamics at metal surfaces.lifetimes | spin effects | time-dependent phenomena C hemistry is driven by electrons. Chemical dynamics is often determined by electron dynamics, with electronically excited states frequently acting as necessary intermediate steps in chemical activity. The understanding and control of charge transfer times and electronic excitation survival times is thus a necessary step to understand, control, and design physical and chemical processes at surfaces.Dynamics of electronic excitations at metal surfaces has been widely investigated both experimentally (1-6) and theoretically (5, 7-13). As a consequence, deep understanding has been reached about the mechanisms ruling electron decay and electron charge transfer. However, recent advances in experimental tools are raising new challenges, many of them linked to shorter time scales, smaller system sizes, and/or spin effects. In this article, we present fresh results on these expanding topics, in an effort to blaze trails in electron dynamics research.At surfaces, electron excitation, charge exchange, and electron decay typically take place in the femtosecond (fs) and attosecond (as) time scales (1 as ¼ 10 −18 s, 1 fs ¼ 10 −15 s) (i.e., at times much faster than any nuclear motion). Advance in laser-based experimental techniques has carried research on this field to a new frontier, in which direct measurements of electron processes in this time scale are possible. Attosecond spectroscopy, for instance, is nowadays able to discern the individual elementary steps in photoemission from surfaces (i.e., excitation, transport, and emission) (14, 15). Access to experimental information in the attosecond scale is asking for new theoretical concepts. In particular, one of the relevant questions is how electronic excitations are created in time and how the environment reacts in such time scale. In the photocreation of localized holes in adsorbates at metallic surfaces, this question can be reformulated as...

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Section: Confinement Effects In Electron Dynamicssupporting

confidence: 53%

Section: Confinement Effects In Electron Dynamicsmentioning

confidence: 85%

Section: Confinement Effects In Electron Dynamicsmentioning

confidence: 99%

Section: Confinement Effects In Electron Dynamicsmentioning

confidence: 99%

See 2 more Smart Citations

Time-dependent electron phenomena at surfaces

Muiño

Sánchez‐Portal

Silkin

et al. 2010

Proc. Natl. Acad. Sci. U.S.A.

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“…[1][2][3][4][5][6] In particular, the e-ph coupling affects the lifetime and the dispersion of excited electrons (or holes). 2,7,8 The lifetime or the linewidth (inverse lifetime) is an essential quantity, describing the decay of electron (hole) excitations 7,9 which are important in many processes such as photochemical and catalytical reactions. 10,11 Lead as a strong-coupling superconductor has been a focus of various theoretical studies of electron-phonon coupling properties, 6,[12][13][14][15][16][17][18][19][20][21] and a very detailed information concerning the e-ph interaction at the Fermi level (E F ) is now available.…”

Section: Introductionmentioning

confidence: 99%

Electron-phonon interaction in bulk Pb: Beyond the Fermi surface

et al. 2012

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The electron-phonon interaction in bulk Pb and the influence of spin-orbit coupling (SOC) on the pairing strength are investigated within the density-functional theory and linear-response approach in the mixed-basis pseudopotential representation. We find that the SOC-induced modifications of both electronic bands and lattice vibrations result in striking changes in the phonon-induced scattering of excited electrons (holes). The strength of the momentum-averaged electron-phonon interaction λ(E) ranges from 0 to 2.5 while the contribution to λ(E) from particular electronic states can even exceed 4. It is found that the coupling strength is exceedingly strong for phonon-induced transitions between electronic states of p and d symmetry. The electron-phonon coupling in Pb also shows a band dependence which, in particular, results in two different sets of electron-phonon coupling parameters on the two sheets of the Fermi surface.

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