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Title: Ionization and fragmentation of solid C{sub 60} by femtosecond laser ablation

Abstract

Ionization and fragmentation of solid C{sub 60} dispersed on a silicon plate are investigated by femtosecond laser ablation. Bimodal mass distribution with large fragment ions C{sub 60-2n}{sup +} (0{<=}n{<=}11) and small fragment ions C{sub n}{sup +} (13{<=}n{<=}28), formation of dimer ion (C{sub 60}){sub 2}{sup +}, and delayed ionization of C{sub 60} have been observed as reported in gas phase experiments with nanosecond laser excitation. Metastable dissociation of small fragment ions C{sub n}{sup +} has been observed for the first time, which suggests different structures of fragment ions compared with those of well-studied carbon cluster ions. From these observations, strong coupling of laser energy to electronic degrees of freedom of solid C{sub 60} has been revealed for femtosecond laser ablation as compared with excitation in the gas phase.

Authors:
; ; ; ; ;  [1];  [2];  [2];  [2];  [2]
  1. Discovery Research Institute, RIKEN, 2-1 Hirosawa, Saitama 351-0198 (Japan)
  2. (Japan)
Publication Date:
OSTI Identifier:
20991218
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 126; Journal Issue: 6; Other Information: DOI: 10.1063/1.2565642; (c) 2007 American Institute of Physics; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ABLATION; DEGREES OF FREEDOM; DISSOCIATION; EXCITATION; FRAGMENTATION; FULLERENES; ION PAIRS; IONS; LASERS; MASS DISTRIBUTION; PHOTOIONIZATION; PHOTOLYSIS; STRONG-COUPLING MODEL

Citation Formats

Kobayashi, T., Kato, T., Matsuo, Y., Kurata-Nishimura, M., Kawai, J., Hayashizaki, Y., Genomic Science Center, RIKEN, 1-7-22 Suehiro-cho, Tsurumi, Yokohama, Kanagawa 230-0045, Nishina Center for Accelerator-Based Science, RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198, Genomic Science Center, RIKEN, 1-7-22 Suehiro-cho, Tsurumi, Yokohama, Kanagawa 230-0045, and Discovery Research Institute, RIKEN, 2-1 Hirosawa, Saitama 351-0198, Japan and Genomic Science Center, RIKEN, 1-7-22 Suehiro-cho, Tsurumi, Yokohama, Kanagawa 230-0045. Ionization and fragmentation of solid C{sub 60} by femtosecond laser ablation. United States: N. p., 2007. Web. doi:10.1063/1.2565642.
Kobayashi, T., Kato, T., Matsuo, Y., Kurata-Nishimura, M., Kawai, J., Hayashizaki, Y., Genomic Science Center, RIKEN, 1-7-22 Suehiro-cho, Tsurumi, Yokohama, Kanagawa 230-0045, Nishina Center for Accelerator-Based Science, RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198, Genomic Science Center, RIKEN, 1-7-22 Suehiro-cho, Tsurumi, Yokohama, Kanagawa 230-0045, & Discovery Research Institute, RIKEN, 2-1 Hirosawa, Saitama 351-0198, Japan and Genomic Science Center, RIKEN, 1-7-22 Suehiro-cho, Tsurumi, Yokohama, Kanagawa 230-0045. Ionization and fragmentation of solid C{sub 60} by femtosecond laser ablation. United States. doi:10.1063/1.2565642.
Kobayashi, T., Kato, T., Matsuo, Y., Kurata-Nishimura, M., Kawai, J., Hayashizaki, Y., Genomic Science Center, RIKEN, 1-7-22 Suehiro-cho, Tsurumi, Yokohama, Kanagawa 230-0045, Nishina Center for Accelerator-Based Science, RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198, Genomic Science Center, RIKEN, 1-7-22 Suehiro-cho, Tsurumi, Yokohama, Kanagawa 230-0045, and Discovery Research Institute, RIKEN, 2-1 Hirosawa, Saitama 351-0198, Japan and Genomic Science Center, RIKEN, 1-7-22 Suehiro-cho, Tsurumi, Yokohama, Kanagawa 230-0045. Wed . "Ionization and fragmentation of solid C{sub 60} by femtosecond laser ablation". United States. doi:10.1063/1.2565642.
@article{osti_20991218,
title = {Ionization and fragmentation of solid C{sub 60} by femtosecond laser ablation},
author = {Kobayashi, T. and Kato, T. and Matsuo, Y. and Kurata-Nishimura, M. and Kawai, J. and Hayashizaki, Y. and Genomic Science Center, RIKEN, 1-7-22 Suehiro-cho, Tsurumi, Yokohama, Kanagawa 230-0045 and Nishina Center for Accelerator-Based Science, RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198 and Genomic Science Center, RIKEN, 1-7-22 Suehiro-cho, Tsurumi, Yokohama, Kanagawa 230-0045 and Discovery Research Institute, RIKEN, 2-1 Hirosawa, Saitama 351-0198, Japan and Genomic Science Center, RIKEN, 1-7-22 Suehiro-cho, Tsurumi, Yokohama, Kanagawa 230-0045},
abstractNote = {Ionization and fragmentation of solid C{sub 60} dispersed on a silicon plate are investigated by femtosecond laser ablation. Bimodal mass distribution with large fragment ions C{sub 60-2n}{sup +} (0{<=}n{<=}11) and small fragment ions C{sub n}{sup +} (13{<=}n{<=}28), formation of dimer ion (C{sub 60}){sub 2}{sup +}, and delayed ionization of C{sub 60} have been observed as reported in gas phase experiments with nanosecond laser excitation. Metastable dissociation of small fragment ions C{sub n}{sup +} has been observed for the first time, which suggests different structures of fragment ions compared with those of well-studied carbon cluster ions. From these observations, strong coupling of laser energy to electronic degrees of freedom of solid C{sub 60} has been revealed for femtosecond laser ablation as compared with excitation in the gas phase.},
doi = {10.1063/1.2565642},
journal = {Journal of Chemical Physics},
number = 6,
volume = 126,
place = {United States},
year = {Wed Feb 14 00:00:00 EST 2007},
month = {Wed Feb 14 00:00:00 EST 2007}
}
  • We report here the resonance effect in femtosecond laser ablation of solid C{sub 60} by investigating wavelength and fluence dependence of product ion species. When the ablation laser wavelength is far from the molecular absorption band of C{sub 60}, we observe both C{sub 60-2n}{sup +} fragment ions and C{sub 60+2n}{sup +} cluster ions as well as C{sub 60}{sup +} parent ion. Delayed ionization of C{sub 60} is not significant. When the ablation laser wavelength is near resonant with the molecular absorption, we observe C{sub 60}{sup +} and some amount of C{sub 60-2n}{sup +} fragment ions depending on the laser fluence.more » Delayed ionization of C{sub 60} is significant in this case, which indicates high internal energy of C{sub 60} molecule. From the observations, we confirm the strong coupling of femtosecond laser energy with C{sub 60} molecule when the molecular absorption is high at the ablation laser wavelength.« less
  • Ionization and fragmentation of C{sub 60} fullerenes is studied in elliptically polarized, intense fs laser fields at 797 nm [I=(0.5-4.3)x10{sup 14} W cm{sup -2}] and contrasted with Xe{sup +}, utilizing time-of-flight mass spectrometry. Very pronounced changes of parent and fragment ion yield as a function of ellipticity are observed. At lower intensities reduction of the ion yield for circular polarization establishes a coherent two-photon process connected with the key role of the LUMO+1(t{sub 1g})'doorway state' and multielectron dynamics. Comparison with the behavior at 399 nm corroborates this finding. At high intensities enhanced fragmentation is observed which is tentatively attributed tomore » returning loops of electron trajectories by the combined action of the C{sub 60}{sup +} field and the circular laser field.« less
  • Fragment ions from C{sub 60} induced by 2 MeV (v=1.7 a.u.) Si{sup 2+} impacts are measured in coincidence with the number distributions of secondary electrons under conditions of single-electron loss and single-electron capture collisions. Multifragmentation, leading to disintegration of cage structure, is found to occur at surprisingly low charge states of r{approx_equal}3. Also, we find that mass distributions of fragment ions are nearly the same for loss and capture collisions provided that the number of electrons ejected, due to electronic energy deposition from an incident ion, are the same. Present results indicate evidently that the internal excitation, rather than themore » charge state r of transiently formed prefragmented parent ions C{sub 60}{sup r+}**, plays the essential role in C{sub 60} fragmentation in fast heavy ion collisions.« less
  • Ionization efficiency curves of both singly and doubly charged fullerene ions (C[sub 60[minus]2n][sup m+], n = 1-5, m = 1 and 2) were determined for the first time, employing electron impact ionization. Appearance energies of all these fragment ions were derived from these data. Relative abundances of the fragment ions were computed from the measured ion intensities and compared with those available in the literature. The results of the present investigation are compared with the data available in the literature on multiply charged and fragment ions. Based on the measured appearance energies of the fragment ions, ionization energies for themore » formation of doubly charged fragment ions are derived. Enthalpies of formation of C[sub 60[minus]2n] (fragment) fullerenes are derived for the first time. The enthalpy data of fullerenes derived in the present work support the loss of C[sub 2n] as the mechanism of fragmentation. 102 refs., 15 figs., 10 tabs.« less