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Journal of the Optical Society of America B

Journal of the Optical Society of America B


  • Vol. 20, Iss. 1 — Jan. 1, 2003
  • pp: 246–253

Laser based soft-x-ray pulses for photoelectron spectroscopy of surfaces

G. Tsilimis, C. Benesch, J. Kutzner, and H. Zacharias  »View Author Affiliations

JOSA B, Vol. 20, Issue 1, pp. 246-253 (2003)

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Light pulses in the extreme ultraviolet (EUV) are generated in the photon energy range hν from 20 to 120 eV in the conversion media argon, neon, and helium by a tabletop high-repetition-rate 30-fs Ti:sapphire laser system. This high-harmonic radiation is applied in the energy range from 20 to 50 eV for photoelectron spectroscopy studies of clean and adsorbate covered Ni(111) and Pt(111) surfaces. The photoemission spectra of the clean Pt(111) surface show secondary electron emission structures that influence the cross-section analysis of CO-induced states. Taking these Pt resonances into consideration, the well-known 4σ and 5σ CO shape resonances are observed at photon energies of 37 and 28 eV. In contrast to previously published experimental data, a resonance is also observed at hν=31 eV for the CO 1π state. On the basis of theoretical approaches this signal structure is identified as an autoionization resonance, experimentally detected for the first time to our knowledge.

© 2003 Optical Society of America

OCIS Codes
(260.7200) Physical optics : Ultraviolet, extreme
(300.6540) Spectroscopy : Spectroscopy, ultraviolet
(320.7110) Ultrafast optics : Ultrafast nonlinear optics

G. Tsilimis, C. Benesch, J. Kutzner, and H. Zacharias, "Laser based soft-x-ray pulses for photoelectron spectroscopy of surfaces," J. Opt. Soc. Am. B 20, 246-253 (2003)

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  1. Z. Chang, A. Rundquist, H. Wang, M. M. Murnane, and H. C. Kapteyn, “Generation of coherent soft x-rays at 2.7 nm using high harmonics,” Phys. Rev. Lett. 79, 2967–2970 (1997).
  2. Ch. Spielmann, N. H. Burnett, S. Sartania, R. Koppitsch, M. Schnürer, C. Kan, M. Lenzner, P. Wobrauschek, and F. Krausz, “Generation of coherent x-rays in the water window using 5-femtosecond laser pulses,” Science 278, 661–664 (1997).
  3. P. Siffalovic, M. Drescher, M. Spieweck, T. Wiesenthal, Y. C. Lim, R. Weidner, A. Elizarov, and U. Heinzmann, “Laser-based apparatus for extended ultraviolet femtosecond time-resolved photoemission spectroscopy,” Rev. Sci. Instrum. 72, 30–35 (2001).
  4. D. Riedel, J. L. Hernandez-Pozos, R. E. Palmer, S. Baggott, K. W. Kolasinski, and J. S. Foord, “Tunable pulsed vacuum ultraviolet light source for surface science and materials spectroscopy based on high order harmonic generation,” Rev. Sci. Instrum. 72, 1977–1983 (2001).
  5. M. Bauer, C. Lei, K. Read, R. Tobey, J. Gland, M. M. Murnane, and H. C. Kapteyn, “Direct observation of surface chemistry using ultrafast soft-x-ray pulses,” Phys. Rev. Lett. 87, 025501 (2001).
  6. P. Hofmann, S. R. Bare, N. V. Richardson, and D. A. King, “Orientation of chemisorped species from orthogonal-plane ARUPS: tilted CO on Pt{110} and upright CO on Pt{111},” Solid State Commun. 42, 645–651 (1982).
  7. G. Blyholder, “Molecular orbital view of chemisorbed carbon monoxide,” J. Phys. Chem. 68, 2772–2778 (1964).
  8. S. Hüfner, Photoelectron Spectroscopy (Springer-Verlag, Heidelberg, 1996).
  9. A. M. Bradshaw, “The structure and chemistry of adsorbed carbon monoxide,” Surf. Sci. 80, 215–225 (1979).
  10. S. R. Bare, K. Griffiths, P. Hoffmann, D. A. King, G. L. Nyberg, N. V. Richardson, “A synchrotron radiation study of the electronic and geometric structure of CO on Pt{110},” Surf. Sci. 120, 367–375 (1982).
  11. A. Nilsson, N. Wassdahl, M. Weinelt, O. Karis, T. Wiell, P. Bennich, J. Hasselström, A. Föhlisch, J. Stöhr, and M. Samant, “Local probing of the surface chemical bond using x-ray emission spectroscopy,” Appl. Phys. A 65, 147–154 (1997).
  12. H. Aizawa and S. Tsuneyuki, “First-principle study of CO bonding to Pt(111): validity of the Blyholder model,” Surf. Sci. 399, L364–L370 (1998).
  13. J. L. Dehmer, “Evidence of effective potential barriers in the x-ray absorption spectra of molecules,” J. Chem. Phys. 56, 4496–4504 (1972).
  14. T. J. Gil, C. L. Winstedad, J. A. Sheehy, R. E. Farren, and P. W. Lanhoff, “New theoretical perspectives on molecular shape resonances: Feshbach–Fano methods for Mulliken orbital analysis of photoionization continua,” Phys. Scr. T31, 179–188 (1990).
  15. M. N. Piancastelli, “The neverending story of shape resonances,” J. Electron Spectrosc. Relat. Phenom. 100, 167–190 (1999).
  16. H. Conrad, G. Ertl, J. Küppers, and E. E. Latta, “Adsorption of CO on clean and oxygen covered Ni(111),” Surf. Sci. 57, 475–484 (1976).
  17. K. L. Kostov, P. Jakob, and D. Menzel, “A new high density CO/oxygen coadsorbate layer on Pt(111) and its role in CO oxidation,” Surf. Sci. 377–379, 802–807 (1997).
  18. A. L’Huillier and Ph. Balcou, “High-order harmonic generation in rare gases with a 1-ps 1053-nm laser,” Phys. Rev. Lett. 70, 774–777 (1993).
  19. P. B. Corkum, “Plasma perspective on strong-field multiphoton ionization,” Phys. Rev. Lett. 71, 1994–1997 (1993).
  20. J. L. Krause, K. J. Schafer, and K. C. Kulander, “High-order harmonic generation from atoms and ions in the high intensity regime,” Phys. Rev. Lett. 68, 3535–3538 (1992).
  21. C.-G. Wahlström, J. Larsson, A. Persson, T. Starczewski, S. Svanberg, P. Salières, Ph. Balcou, and A. L’Huillier, “High-order harmonic generation in rare gases with an intense short-pulse laser,” Phys. Rev. A 48, 4709–4720 (1993).
  22. Data sheet provided for the toroid grating type, 540 00 210 (ISA Instruments S.A., Inc., Grasbrunn, Germany).
  23. M. Schnürer, Z. Cheng, M. Hentschel, G. Tempea, P. Kalman, Th. Brabec, and F. Krausz, “Absorption-limited generation of coherent ultrashort soft x-ray pulses,” Phys. Rev. Lett. 83, 722–725 (1999).
  24. H. Ibach and H. Lüth, Festkörperphysik (Springer-Verlag, Berlin, 1995).
  25. L. Nugent-Glandorf, M. Scheer, M. Krishnamurthy, J. W. Odom, and S. R. Leone, “Photoelectron spectroscopic determination of the energy bandwidths of high-order harmonics (7th-55th) produced by an ultrafast laser in neon,” Phys. Rev. A 62, 023812 (2000).
  26. G. Apai, P. S. Wehner, R. S. Williams, J. Stöhr, and D. A. Shirley, “Orientation of CO on Pt(111) and Ni(111) surfaces from angle-resolved photoemission,” Phys. Rev. Lett. 37, 1497–1500 (1976).
  27. G. Tsilimis, G. Fecher, J. Braun, J. Kutzner, and H. Zacharias, “Direct observation of final states in photoemission from Pt(111) excited by laser generated XUV radiation,” submitted to Europhys. Lett.
  28. F. Greuter, D. Heskett, E. W. Plummer, and H.-J. Freund, “Chemisorption of CO on Co(0001). Structure and electronic properties,” Phys. Rev. B 27, 7117–7135 (1983).
  29. D. A. Shirley, J. Stöhr, P. S. Wehner, R. S. Williams, and G. Apai, “Photoemission from noble metals and adsorbates using synchrotron radiation,” Phys. Scr. 16, 398–413 (1977).
  30. D. E. Eastman and J. K. Cashion, “Photoemission energy-level measurements of chemisorbed CO and O on Ni,” Phys. Rev. Lett. 27, 1520–1523 (1971).
  31. J. W. Davenport, “Ultraviolet photoionization cross sections for N2 and CO,” Phys. Rev. Lett. 36, 945–949 (1976).
  32. D. M. Collins and W. E. Spicer, “The adsorption of CO, O2 and H2 on Pt. II. Ultraviolet photoelectron spectroscopy studies,” Surf. Sci. 69, 114–132 (1977).
  33. D. Rieger, R. D. Schnell, and W. Steinmann, “Angular distribution patterns of photoelectrons from orbitals of CO adsorbed on Ni(100), Pt(111) and Pt(110),” Surf. Sci. 143, 157–176 (1984).
  34. C. W. Seabury, T. N. Rhodin, M. M. Traum, R. Benbow, and Z. Hurych, “Angle-resolved polarization-dependent photoemission studies of carbon monoxide on iridium surfaces,” Surf. Sci. 97, 363–376 (1980).
  35. P. Budau and G. Raseev, “Shape resonances in photoemission for CO molecules adsorbed on metallic surfaces: a model including backscattering,” Phys. Rev. B 51, 16993–17006 (1995).
  36. M. Stener, P. Decleva, I. Cacelli, R. Moccia, and R. Montuoro, “Response function study of CO photoionization: ab initio SCF and density functional results,” Chem. Phys. 272, 15–25 (2001).
  37. J. N. Miller, D. T. Ling, P. M. Stefan, D. L. Weissman, M. L. Shek, I. Lindau, and W. E. Spicer, “Synchrotron radiation studies of CO and H2O adsorbed on Pt,” Phys. Rev. B 24, 1917–1926 (1981).
  38. V. Dose, J. Rogozik, A. M. Bradshaw, and K. C. Prince, “Inverse photoemission from CO coadsorbed with K on Pt(111),” Surf. Sci. 179, 90–100 (1987).
  39. M. Stener and P. Decleva, “Time-dependent density functional calculations of molecular photoionization cross sections: N2 and PH3,” J. Chem. Phys. 112, 10871–10879 (2000).
  40. S. K. Semenov, N. A. Cherepkov, G. H. Fecher and G. Schönhense, “Generalization of the atomic random-phase-approximation method for diatomic molecules: N2 photoionization cross-section calculations,” Phys. Rev. A 61, 032704 (2000).

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