Excitation dynamics of Rydberg states in C60

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MARC

Boyle, Mark (author)

Excitation dynamics of Rydberg states in C60

Article/chapterEnglish2005

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2005-10-25
Springer Science and Business Media LLC,2005

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LIBRIS-ID:oai:gup.ub.gu.se/55832
https://gup.ub.gu.se/publication/55832URI
https://doi.org/10.1140/epjd/e2005-00281-7DOI

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Language:English

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Subject category:art swepub-publicationtype

Notes

The electron and nuclear dynamics of C60 fullerenes irradiated with femtosecond laser pulses are investigated with photoelectron and photoion spectroscopy. The focus of this work is the detailed exploration of the population mechanism of Rydberg levels within the excitation process of neutral C60. The effect of excitation wavelength, intensity, chirp, and polarization on the kinetic energy distribution of photoelectrons in single-pulse experiments gives first insight into the underlying processes. In combination with time-resolved two-color pump-probe spectroscopy depending on either pump, or probe pulse intensity, a more complete picture of the interaction can be drawn. The results point towards a very interesting but nevertheless complex behavior including four steps: (i) non-adiabatic multielectron excitation of the HOMO (hu) → LUMO+1 (t1g) transition; (ii) thermalization within the hot electron cloud on a time scale below 100fs, followed by a coupling of energy to vibrational modes of the molecule via doorway state(s); (iii) population of electronically excited Rydberg states by multiphoton absorption, and (iv) single photon ionization from the excited Rydberg states. This excitation process results in a characteristic sequence of photoelectron lines in the photoemission spectra. The comparison of the experimental results with recent theoretical work gives convincing evidence that non-adiabatic multielectron dynamics (NMED) plays a key role for the understanding of the response of C60 to short-pulse laser radiation.

Subject headings and genre

NATURVETENSKAP Fysik Atom- och molekylfysik och optik hsv//swe
NATURAL SCIENCES Physical Sciences Atom and Molecular Physics and Optics hsv//eng
fullerenes

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Laarmann, T. (author)
Hoffmann, K. (author)
Hedén, Martin,1976Gothenburg University,Göteborgs universitet,Institutionen för fysik (GU),Department of Physics (GU) (author)
Campbell, Eleanor E B,1960Gothenburg University,Göteborgs universitet,Institutionen för fysik (GU),Department of Physics (GU)(Swepub:gu)xcamel (author)
Schulz, C.P. (author)
Hertel, Ingolf,1941 (author)
Göteborgs universitetInstitutionen för fysik (GU) (creator_code:org_t)

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In:European Physical Journal D: Springer Science and Business Media LLC36, s. 339-3511434-60601434-6079

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NATURAL SCIENCES: NATURAL SCIENCES; and Physical Science ...; and Atom and Molecul ...

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By the university: University of Gothenburg

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