Adsorption and electronic structure of submonolayer Ca on Ag(111) DOI
Heeseon Lim, Yanan Wang, Namitha James

и другие.

Physical review. B./Physical review. B, Год журнала: 2024, Номер 110(7)

Опубликована: Авг. 2, 2024

By frequency-time spectroscopy, microscopy, and electronic structure theory, we investigate the low coverage adsorption of Ca on an Ag(111) surface. The chemisorption alkaline-earth atoms starting from their closed $4{s}^{2}$ shell configuration differs that open $n{s}^{1}$ alkali-metal because they retain some $4s$ electron charge can involve hybridization with low-lying unoccupied $3d$ orbitals. Spectroscopic investigation by three-photon photoemission (3PP) reveals states dominant 3d-orbital character, as confirmed theory. Coverage-specific spectral features enable attribution to two distinct phases at submonolayer coverages, which are atomic scale scanning tunneling microscopy spectroscopy measurements. Furthermore, time-resolved 3PP a resonant two-photon transition between occupied $(\ensuremath{\sim}\ensuremath{-}0.3 \mathrm{eV})$ $(\ensuremath{\sim}2.7 s- $d$-orbital character. Interferometric measurements probing this resonance reveal dephasing time $\ensuremath{\sim}21$ fs population lifetime $\ensuremath{\sim}52$ for transiently populated $d$-like state $\ensuremath{\sim}2.7$ eV above ${E}_{F}$. Contrary atom chemisorption, characteristic development importance adsorbate Ag substrate interactions cause low-coverage condensation into compact islands. Discovery long-lived $d$-character informs catalytic optoelectronic applications element Ca.

Язык: Английский

Adsorption and electronic structure of submonolayer Ca on Ag(111) DOI
Heeseon Lim, Yanan Wang, Namitha James

и другие.

Physical review. B./Physical review. B, Год журнала: 2024, Номер 110(7)

Опубликована: Авг. 2, 2024

By frequency-time spectroscopy, microscopy, and electronic structure theory, we investigate the low coverage adsorption of Ca on an Ag(111) surface. The chemisorption alkaline-earth atoms starting from their closed $4{s}^{2}$ shell configuration differs that open $n{s}^{1}$ alkali-metal because they retain some $4s$ electron charge can involve hybridization with low-lying unoccupied $3d$ orbitals. Spectroscopic investigation by three-photon photoemission (3PP) reveals states dominant 3d-orbital character, as confirmed theory. Coverage-specific spectral features enable attribution to two distinct phases at submonolayer coverages, which are atomic scale scanning tunneling microscopy spectroscopy measurements. Furthermore, time-resolved 3PP a resonant two-photon transition between occupied $(\ensuremath{\sim}\ensuremath{-}0.3 \mathrm{eV})$ $(\ensuremath{\sim}2.7 s- $d$-orbital character. Interferometric measurements probing this resonance reveal dephasing time $\ensuremath{\sim}21$ fs population lifetime $\ensuremath{\sim}52$ for transiently populated $d$-like state $\ensuremath{\sim}2.7$ eV above ${E}_{F}$. Contrary atom chemisorption, characteristic development importance adsorbate Ag substrate interactions cause low-coverage condensation into compact islands. Discovery long-lived $d$-character informs catalytic optoelectronic applications element Ca.

Язык: Английский

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