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Electron pair escape from fullerene cage via collective modes.

Schüler M, Pavlyukh Y, Bolognesi P, Avaldi L, Berakdar J - Sci Rep (2016)

Bottom Line: Experiment and theory evidence a new pathway for correlated two-electron release from many-body compounds following collective excitation by a single photon.Results from a full ab initio implementation for C60 fullerene are in line with experimental observations.The findings endorse the correlated two-electron photoemission as a powerful tool to access electronic correlation in complex systems.

View Article: PubMed Central - PubMed

Affiliation: Institut für Physik, Martin-Luther-Universität Halle-Wittenberg, 06099 Halle, Germany.

ABSTRACT
Experiment and theory evidence a new pathway for correlated two-electron release from many-body compounds following collective excitation by a single photon. Using nonequilibrium Green's function approach we trace plasmon oscillations as the key ingredient of the effective electron-electron interaction that governs the correlated pair emission in a dynamic many-body environment. Results from a full ab initio implementation for C60 fullerene are in line with experimental observations. The findings endorse the correlated two-electron photoemission as a powerful tool to access electronic correlation in complex systems.

No MeSH data available.


Related in: MedlinePlus

(a) Comparison of theoretical prediction of the coincidence spectrum to experimental data. Curves have been normalized to each others at one point. Gaussian broadening of the electronic states is set to η = 0.25 eV. (b) Normalized coincidence yield resolved in emission of the second electron from σ and π states, respectively. (c) Single-particle energies of the  molecule as function of the dominant angular momentum. Dot-dashed lines: accessible energy range of the plasmon modes (FWHM of the plasmon spectra Bν,L(ξ), shifted by the photoelectron energy ). Thick dashed lines: ideal dispersion for non-interacting particles on a sphere with radius R0 = 3.57 Å. Coincidence yield resolved with respect to plasmon modes (d), and multipolarity (e).
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f3: (a) Comparison of theoretical prediction of the coincidence spectrum to experimental data. Curves have been normalized to each others at one point. Gaussian broadening of the electronic states is set to η = 0.25 eV. (b) Normalized coincidence yield resolved in emission of the second electron from σ and π states, respectively. (c) Single-particle energies of the molecule as function of the dominant angular momentum. Dot-dashed lines: accessible energy range of the plasmon modes (FWHM of the plasmon spectra Bν,L(ξ), shifted by the photoelectron energy ). Thick dashed lines: ideal dispersion for non-interacting particles on a sphere with radius R0 = 3.57 Å. Coincidence yield resolved with respect to plasmon modes (d), and multipolarity (e).

Mentions: The computed coincidence photocurrent for the experimental setup of  eV is presented in Fig. 3(a) along with the data from the experiment. The equal energy-sharing case has been chosen by the experience on atoms, where this represents the case where the effects of the correlation and symmetry play a dominant role. Further tests (see supplementary information) show that, in contrast to the Auger process [Fig. 1(b)], all ingredients of Eq. (3) (and hence all steps in Fig. 2) are essential: matrix elements effects encoded in , plasmon dispersions Bν,L(ξ), radial profiles of the fluctuations densities Rν,L(r), and density of states . Hence, DPE in the present case adds new aspects to DPE from, e.g., atomic targets, and is a useful sensor for the e–e interaction mediated by charge-density fluctuations.


Electron pair escape from fullerene cage via collective modes.

Schüler M, Pavlyukh Y, Bolognesi P, Avaldi L, Berakdar J - Sci Rep (2016)

(a) Comparison of theoretical prediction of the coincidence spectrum to experimental data. Curves have been normalized to each others at one point. Gaussian broadening of the electronic states is set to η = 0.25 eV. (b) Normalized coincidence yield resolved in emission of the second electron from σ and π states, respectively. (c) Single-particle energies of the  molecule as function of the dominant angular momentum. Dot-dashed lines: accessible energy range of the plasmon modes (FWHM of the plasmon spectra Bν,L(ξ), shifted by the photoelectron energy ). Thick dashed lines: ideal dispersion for non-interacting particles on a sphere with radius R0 = 3.57 Å. Coincidence yield resolved with respect to plasmon modes (d), and multipolarity (e).
© Copyright Policy - open-access
Related In: Results  -  Collection

License
Show All Figures
getmorefigures.php?uid=PMC4834545&req=5

f3: (a) Comparison of theoretical prediction of the coincidence spectrum to experimental data. Curves have been normalized to each others at one point. Gaussian broadening of the electronic states is set to η = 0.25 eV. (b) Normalized coincidence yield resolved in emission of the second electron from σ and π states, respectively. (c) Single-particle energies of the molecule as function of the dominant angular momentum. Dot-dashed lines: accessible energy range of the plasmon modes (FWHM of the plasmon spectra Bν,L(ξ), shifted by the photoelectron energy ). Thick dashed lines: ideal dispersion for non-interacting particles on a sphere with radius R0 = 3.57 Å. Coincidence yield resolved with respect to plasmon modes (d), and multipolarity (e).
Mentions: The computed coincidence photocurrent for the experimental setup of  eV is presented in Fig. 3(a) along with the data from the experiment. The equal energy-sharing case has been chosen by the experience on atoms, where this represents the case where the effects of the correlation and symmetry play a dominant role. Further tests (see supplementary information) show that, in contrast to the Auger process [Fig. 1(b)], all ingredients of Eq. (3) (and hence all steps in Fig. 2) are essential: matrix elements effects encoded in , plasmon dispersions Bν,L(ξ), radial profiles of the fluctuations densities Rν,L(r), and density of states . Hence, DPE in the present case adds new aspects to DPE from, e.g., atomic targets, and is a useful sensor for the e–e interaction mediated by charge-density fluctuations.

Bottom Line: Experiment and theory evidence a new pathway for correlated two-electron release from many-body compounds following collective excitation by a single photon.Results from a full ab initio implementation for C60 fullerene are in line with experimental observations.The findings endorse the correlated two-electron photoemission as a powerful tool to access electronic correlation in complex systems.

View Article: PubMed Central - PubMed

Affiliation: Institut für Physik, Martin-Luther-Universität Halle-Wittenberg, 06099 Halle, Germany.

ABSTRACT
Experiment and theory evidence a new pathway for correlated two-electron release from many-body compounds following collective excitation by a single photon. Using nonequilibrium Green's function approach we trace plasmon oscillations as the key ingredient of the effective electron-electron interaction that governs the correlated pair emission in a dynamic many-body environment. Results from a full ab initio implementation for C60 fullerene are in line with experimental observations. The findings endorse the correlated two-electron photoemission as a powerful tool to access electronic correlation in complex systems.

No MeSH data available.


Related in: MedlinePlus