Atomlike, Hollow-Core–Bound Molecular Orbitals of C
            <sub>60</sub>

Feng, Min; Zhao, Jin; Petek, Hrvoje

doi:10.1126/science.1155866

Cited by 280 publications

(419 citation statements)

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“…For the cylindrical island structure, these states are characterized by the magnetic quantum number m, vertical (principal) quantum number n, and radial quantum number as given by Eq. (10).…”

Section: Discussionmentioning

confidence: 99%

“…In this way, image potential states (IS's) are Stark-shifted and actually become field emission resonances (FER's) as observed on different metal 1 and semiconductor surfaces. 2 FER's can be used to chemically identify different surface terminations from a study of the local changes in the work function [3][4][5][6][7] as well as to probe the effects of electron confinement in metallic 8,9 and molecular 10 nanostructures. Since the energetics of FER's is to a large extent determined by the electric field at the junction, the interpretation of the data is relatively simple.…”

Section: Introductionmentioning

confidence: 99%

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Localization, splitting, and mixing of field emission resonances induced by alkali metal clusters on Cu(100)

et al. 2011

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We report on a joint scanning tunneling microscopy (STM) and theoretical wave packet propagation study of field emission resonances (FER's) of nanosized alkali metal clusters deposited on a Cu(100) surface. In addition to FER's of the pristine Cu(100) surface, we observe the appearance of island-induced resonances that are particularly well resolved for STM bias voltage values corresponding to electron energies inside the projected band gap of the substrate. The corresponding dI/dV maps reveal island-induced resonances of different nature. Their electronic densities are localized either inside the alkali cluster or on its boundaries. Our model calculations allow us to explain the experimental results as due to the coexistence and mixing of two kinds of island-induced states. On the one side, since the alkali work function is lower than that of the substrate, the nanosized alkali metal clusters introduce intrinsic localized electronic states pinned to the vacuum level above the cluster. These states can be seen as the FER's of the complete alkali overlayer quantized by the cluster boundaries. On the other side, the attractive potential well due to the alkali metal cluster leads to two-dimensional (2D) localization of the FER's of the Cu(100) surface, the corresponding split component of the resonances appearing below the bottom of the parent continuum. Our main conclusions are based on the attractive nature of the alkali ad-island potential. They are of general validity and, therefore, significant to understand electron confinement in 2D.

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Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Localization, splitting, and mixing of field emission resonances induced by alkali metal clusters on Cu(100)

et al. 2011

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“…Concerning C-based materials, superatom states of adsorbed fullerenes can lead to the formation of free electron bands (61). Endohedral doping of fullerenes offers then a route to tailor the superatom state properties.…”

Section: Discussionmentioning

confidence: 99%

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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“…Among the clusters with various sizes, those deemed "superatoms" exhibit enhanced stabilities due to the electronic shell closing [5]. Many superatomic structures, such as C 60 [6], Al 13 [7], Na 40 [8] and Au 20 [9], have been experimentally confirmed. Recently, the Au 32 gold fullerene was revealed to have 1S 2 1P 6 1D 10 1F 14 electronic configuration, thus making a superatom [10,11].…”

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confidence: 99%

All-boron fullerene B40: a superatomic structure

Wang

2017

Sci. China Mater.

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By means of the first-principles calculations, we reveal that B 40 presents superatomic properties. It not only has superatomic 1S, 1P, 1D and 1F orbitals, but also has superatomic orbitals 2S, 2P, 2D and 2F. The superatomic 2F orbital of B 40 is partially occupied, thus adding six electrons to the cluster leads to a superatomic structure of fully occupied shells. , were also optimized at PBE0/ 6-31G* level. Frequency analyses were performed at the same level of theory to characterize the nature of the stationary points. Both B 40 and B 40 6− are true local minima, but B 40 8+ with fully occupied shell is a high order saddle point. Following the imaginary modes of B 40 8+ leads to the true local minimum without full-filled shell. The optimized geometries from different functionals are rather similar, and we only discuss the computational results from PBE0 because it has been tested extensively in previous works and found to be suitable for boron clusters [1,[20][21][22]. To investigate the electron delocalization or aromaticity of B 40 and its charged species, we calculated NICS (in ppm) [23,24] at the cage centers of the optimized geometries of the empty cage molecules using the gauge-independent atomic orbital (GIAO) method [25]. The verification of B 40 using PBE0/6-311 +G* level is shown in Table S2 in SI. All computations are carried out using the Gaussian09 package [26].Our calculations show that the ground state of B 40 fullerene (D 2d ) is non-spin-polarized singlet, with the low and high energy molecular orbitals (MOs) displayed in Figs 1, 2, respectively. Among the low-energy MOs, a double-occupied MO 7a 1 (marked by black) resembles an s-like atomic orbital, thus we call it the 1S superatomic orbital (that is, molecular orbital) for B 40 , and the specific orbital composition analyses are described in the fol-

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Atomlike, Hollow-Core–Bound Molecular Orbitals of C ₆₀

Cited by 280 publications

References 24 publications

Localization, splitting, and mixing of field emission resonances induced by alkali metal clusters on Cu(100)

Localization, splitting, and mixing of field emission resonances induced by alkali metal clusters on Cu(100)

Time-dependent electron phenomena at surfaces

All-boron fullerene B40: a superatomic structure

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Atomlike, Hollow-Core–Bound Molecular Orbitals of C 60

Cited by 280 publications

References 24 publications

Localization, splitting, and mixing of field emission resonances induced by alkali metal clusters on Cu(100)

Localization, splitting, and mixing of field emission resonances induced by alkali metal clusters on Cu(100)

Time-dependent electron phenomena at surfaces

All-boron fullerene B40: a superatomic structure

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Product

Resources

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Atomlike, Hollow-Core–Bound Molecular Orbitals of C ₆₀