Generation of single-order laser harmonics in extreme ultraviolet (EUV) and the application to the time-resolved photoelectron spectroscopy of I₂ are demonstrated. The EUV pulses at 80 nm were generated from Kr as the 5th order harmonics of intense 400 nm laser pulses and then separated from other harmonic orders by a thin indium foil. The pump-probe photoelectron spectroscopy of I₂ in the B ³Π(0_u⁺) and B” ¹Π(1_u) states excited by visible laser pulses at 490 nm showed a rapid increase in the yield of atomic iodine (~400 fs), reflecting the dissociation dynamics evolving simultaneously in the two excited states.

© 2011 OSA

1. P. B. Corkum and F. Krausz, “Attosecond science,” Nat. Phys. 3(6), 381–387 (2007). [CrossRef]
2. M. Drescher, M. Hentschel, R. Kienberger, M. Uiberacker, V. Yakovlev, A. Scrinzi, T. Westerwalbesloh, U. Kleineberg, U. Heinzmann, and F. Krausz, “Time-resolved atomic inner-shell spectroscopy,” Nature 419(6909), 803–807 (2002). [CrossRef] [PubMed]
3. E. Goulielmakis, Z.-H. Loh, A. Wirth, R. Santra, N. Rohringer, V. S. Yakovlev, S. Zherebtsov, T. Pfeifer, A. M. Azzeer, M. F. Kling, S. R. Leone, and F. Krausz, “Real-time observation of valence electron motion,” Nature 466(7307), 739–743 (2010). [CrossRef] [PubMed]
4. A. L. Cavalieri, N. Müller, T. Uphues, V. S. Yakovlev, A. Baltuška, B. Horvath, B. Schmidt, L. Blümel, R. Holzwarth, S. Hendel, M. Drescher, U. Kleineberg, P. M. Echenique, R. Kienberger, F. Krausz, and U. Heinzmann, “Attosecond spectroscopy in condensed matter,” Nature 449(7165), 1029–1032 (2007). [CrossRef] [PubMed]
5. L. Nugent-Glandorf, M. Scheer, D. A. Samuels, A. M. Mulhisen, E. R. Grant, X. Yang, V. M. Bierbaum, and S. R. Leone, “Ultrafast time-resolved soft x-ray photoelectron spectroscopy of dissociating Br2.,” Phys. Rev. Lett. 87(19), 193002 (2001). [CrossRef] [PubMed]
6. P. Wernet, M. Odelius, K. Godehusen, J. Gaudin, O. Schwarzkopf, and W. Eberhardt, “Real-time evolution of the valence electronic structure in a dissociating molecule,” Phys. Rev. Lett. 103(1), 013001 (2009). [CrossRef] [PubMed]
7. E. Gagnon, P. Ranitovic, X.-M. Tong, C. L. Cocke, M. M. Murnane, H. C. Kapteyn, and A. S. Sandhu, “Soft X-ray-driven femtosecond molecular dynamics,” Science 317(5843), 1374–1378 (2007). [CrossRef] [PubMed]
8. A. Peralta Conde, J. Kruse, O. Faucher, P. Tzallas, E. P. Benis, and D. Charalambidis, “Realization of time-resolved two-vacuum-ultraviolet-photon ionization,” Phys. Rev. A 79(6), 061405 (2009). [CrossRef]
9. T. Brabec and F. Krausz, “Intense few-cycle laser fields: Frontiers of nonlinear optics,” Rev. Mod. Phys. 72(2), 545–591 (2000). [CrossRef]
10. E. Goulielmakis, M. Schultze, M. Hofstetter, V. S. Yakovlev, J. Gagnon, M. Uiberacker, A. L. Aquila, E. M. Gullikson, D. T. Attwood, R. Kienberger, F. Krausz, and U. Kleineberg, “Single-cycle nonlinear optics,” Science 320(5883), 1614–1617 (2008). [CrossRef] [PubMed]
11. H. Mashiko, S. Gilbertson, C. Li, S. D. Khan, M. M. Shakya, E. Moon, and Z. Chang, “Double optical gating of high-order harmonic generation with carrier-envelope phase stabilized lasers,” Phys. Rev. Lett. 100(10), 103906 (2008). [CrossRef] [PubMed]
12. J. Gaudin, S. Rehbein, P. Guttmann, S. Godé, G. Schneider, P. Wernet, and W. Eberhardt, “Selection of a single femtosecond high-order harmonic using a zone plate based monochromator,” J. Appl. Phys. 104(3), 033112–033114 (2008). [CrossRef]
13. F. Frassetto, P. Villoresi, and L. Poletto, “Beam separator for high-order harmonic radiation in the 3-10 nm spectral region,” J. Opt. Soc. Am. A 25(5), 1104–1114 (2008). [CrossRef]
14. Y. Nabekawa, H. Hasegawa, E. J. Takahashi, and K. Midorikawa, “Production of doubly charged helium ions by two-photon absorption of an intense sub-10-fs soft x-ray pulse at 42 eV photon energy,” Phys. Rev. Lett. 94(4), 043001 (2005). [CrossRef] [PubMed]
15. A. Kosuge, T. Sekikawa, X. Zhou, T. Kanai, S. Adachi, and S. Watanabe, “Frequency-resolved optical gating of isolated attosecond pulses in the extreme ultraviolet,” Phys. Rev. Lett. 97(26), 263901 (2006). [CrossRef]
16. M. Fushitani, A. Matsuda, E. J. Takahashi, and A. Hishikawa, “Time-resolved reaction imaging by intense few-cycle laser pulses and laser high-order harmonics,” J. Phys.: Conf. Ser. 185, 012009 (2009). [CrossRef]
17. S. Zamith, V. Blanchet, B. Girard, J. Andersson, S. L. Sorensen, I. Hjelte, O. Bjorneholm, D. Gauyacq, J. Norin, J. Mauritsson, and A. L'Huillier, “The predissociation of highly excited states in acetylene by time-resolved photoelectron spectroscopy,” J. Chem. Phys. 119(7), 3763–3773 (2003). [CrossRef]
18. W. R. Hunter, D. W. Angel, and R. Tousey, “Thin films and their uses for the extreme ultraviolet,” Appl. Opt. 4(8), 891–898 (1965). [CrossRef]
19. F. R. Powell, J. F. Lindblom, S. F. Powell, and P. W. Vedder, “Thin film filter performance for extreme ultraviolet and x-ray applications,” Opt. Eng. 29(6), 614–624 (1990). [CrossRef]
20. E. Skantzakis, P. Tzallas, J. E. Kruse, C. Kalpouzos, O. Faucher, G. D. Tsakiris, and D. Charalambidis, “Tracking autoionizing-wave-packet dynamics at the 1-fs temporal scale,” Phys. Rev. Lett. 105(4), 043902 (2010). [CrossRef] [PubMed]
21. P. Tzallas, D. Charalambidis, N. A. Papadogiannis, K. Witte, and G. D. Tsakiris, “Direct observation of attosecond light bunching,” Nature 426(6964), 267–271 (2003). [CrossRef] [PubMed]
22. N. A. Papadogiannis, L. A. A. Nikolopoulos, D. Charalambidis, G. D. Tsakiris, P. Tzallas, and K. Witte, “Two-photon ionization of he through a superposition of higher harmonics,” Phys. Rev. Lett. 90(13), 133902 (2003). [CrossRef] [PubMed]
23. T. Horio, T. Fuji, Y. Suzuki, and T. Suzuki, “Probing ultrafast internal conversion through conical intersection via time-energy map of photoelectron angular anisotropy,” J. Am. Chem. Soc. 131(30), 10392–10393 (2009). [CrossRef] [PubMed]
24. A. Hishikawa, A. Matsuda, M. Fushitani, and E. J. Takahashi, “Visualizing recurrently migrating hydrogen in acetylene dication by intense ultrashort laser pulses,” Phys. Rev. Lett. 99(25), 258302 (2007). [CrossRef]
25. J. Tellinghuisen, “Transition strengths in the visible-infrared absorption spectrum of I2,” J. Chem. Phys. 76(10), 4736–4744 (1982). [CrossRef]
26. Y. Hikosaka, M. Fushitani, A. Matsuda, C.-M. Tseng, A. Hishikawa, E. Shigemasa, M. Nagasono, K. Tono, T. Togashi, H. Ohashi, H. Kimura, Y. Senba, M. Yabashi, and T. Ishikawa, “Multiphoton double ionization of Ar in intense extreme ultraviolet laser fields studied by shot-by-shot photoelectron spectroscopy,” Phys. Rev. Lett. 105(13), 133001 (2010). [CrossRef]
27. A. B. Cornford, D. C. Frost, C. A. McDowell, J. L. Ragle, and I. A. Stenhouse, “Photoelectron spectra of the halogens,” J. Chem. Phys. 54(6), 2651–2657 (1971). [CrossRef]
28. W. A. de Jong, L. Visscher, and W. C. Nieuwpoort, “Relativistic and correlated calculations on the ground, excited, and ionized states of iodine,” J. Chem. Phys. 107(21), 9046–9058 (1997). [CrossRef]
29. T. Kanai, X. Zhou, T. Sekikawa, S. Watanabe, and T. Togashi, “Generation of subterawatt sub-10-fs blue pulses at 1-5 kHz by broadband frequency doubling,” Opt. Lett. 28(16), 1484–1486 (2003). [CrossRef] [PubMed]
30. M. D. Feit, J. A. Fleck, and A. Steiger, “Solution of the Schrödinger equation by a spectral method,” J. Comput. Phys. 47(3), 412–433 (1982). [CrossRef]

Appl. Opt.

• W. R. Hunter, D. W. Angel, and R. Tousey, “Thin films and their uses for the extreme ultraviolet,” Appl. Opt. 4(8), 891–898 (1965). [CrossRef]

J. Am. Chem. Soc.

• T. Horio, T. Fuji, Y. Suzuki, and T. Suzuki, “Probing ultrafast internal conversion through conical intersection via time-energy map of photoelectron angular anisotropy,” J. Am. Chem. Soc. 131(30), 10392–10393 (2009). [CrossRef] [PubMed]

J. Appl. Phys.

• J. Gaudin, S. Rehbein, P. Guttmann, S. Godé, G. Schneider, P. Wernet, and W. Eberhardt, “Selection of a single femtosecond high-order harmonic using a zone plate based monochromator,” J. Appl. Phys. 104(3), 033112–033114 (2008). [CrossRef]

J. Chem. Phys.

• J. Tellinghuisen, “Transition strengths in the visible-infrared absorption spectrum of I2,” J. Chem. Phys. 76(10), 4736–4744 (1982). [CrossRef]
• A. B. Cornford, D. C. Frost, C. A. McDowell, J. L. Ragle, and I. A. Stenhouse, “Photoelectron spectra of the halogens,” J. Chem. Phys. 54(6), 2651–2657 (1971). [CrossRef]
• W. A. de Jong, L. Visscher, and W. C. Nieuwpoort, “Relativistic and correlated calculations on the ground, excited, and ionized states of iodine,” J. Chem. Phys. 107(21), 9046–9058 (1997). [CrossRef]
• S. Zamith, V. Blanchet, B. Girard, J. Andersson, S. L. Sorensen, I. Hjelte, O. Bjorneholm, D. Gauyacq, J. Norin, J. Mauritsson, and A. L'Huillier, “The predissociation of highly excited states in acetylene by time-resolved photoelectron spectroscopy,” J. Chem. Phys. 119(7), 3763–3773 (2003). [CrossRef]

J. Comput. Phys.

• M. D. Feit, J. A. Fleck, and A. Steiger, “Solution of the Schrödinger equation by a spectral method,” J. Comput. Phys. 47(3), 412–433 (1982). [CrossRef]

J. Opt. Soc. Am. A

• F. Frassetto, P. Villoresi, and L. Poletto, “Beam separator for high-order harmonic radiation in the 3-10 nm spectral region,” J. Opt. Soc. Am. A 25(5), 1104–1114 (2008). [CrossRef]

J. Phys.: Conf. Ser.

• M. Fushitani, A. Matsuda, E. J. Takahashi, and A. Hishikawa, “Time-resolved reaction imaging by intense few-cycle laser pulses and laser high-order harmonics,” J. Phys.: Conf. Ser. 185, 012009 (2009). [CrossRef]

Nat. Phys.

• P. B. Corkum and F. Krausz, “Attosecond science,” Nat. Phys. 3(6), 381–387 (2007). [CrossRef]

Nature

• M. Drescher, M. Hentschel, R. Kienberger, M. Uiberacker, V. Yakovlev, A. Scrinzi, T. Westerwalbesloh, U. Kleineberg, U. Heinzmann, and F. Krausz, “Time-resolved atomic inner-shell spectroscopy,” Nature 419(6909), 803–807 (2002). [CrossRef] [PubMed]
• E. Goulielmakis, Z.-H. Loh, A. Wirth, R. Santra, N. Rohringer, V. S. Yakovlev, S. Zherebtsov, T. Pfeifer, A. M. Azzeer, M. F. Kling, S. R. Leone, and F. Krausz, “Real-time observation of valence electron motion,” Nature 466(7307), 739–743 (2010). [CrossRef] [PubMed]
• A. L. Cavalieri, N. Müller, T. Uphues, V. S. Yakovlev, A. Baltuška, B. Horvath, B. Schmidt, L. Blümel, R. Holzwarth, S. Hendel, M. Drescher, U. Kleineberg, P. M. Echenique, R. Kienberger, F. Krausz, and U. Heinzmann, “Attosecond spectroscopy in condensed matter,” Nature 449(7165), 1029–1032 (2007). [CrossRef] [PubMed]
• P. Tzallas, D. Charalambidis, N. A. Papadogiannis, K. Witte, and G. D. Tsakiris, “Direct observation of attosecond light bunching,” Nature 426(6964), 267–271 (2003). [CrossRef] [PubMed]

Opt. Eng.

• F. R. Powell, J. F. Lindblom, S. F. Powell, and P. W. Vedder, “Thin film filter performance for extreme ultraviolet and x-ray applications,” Opt. Eng. 29(6), 614–624 (1990). [CrossRef]

Opt. Lett.

• T. Kanai, X. Zhou, T. Sekikawa, S. Watanabe, and T. Togashi, “Generation of subterawatt sub-10-fs blue pulses at 1-5 kHz by broadband frequency doubling,” Opt. Lett. 28(16), 1484–1486 (2003). [CrossRef] [PubMed]

Phys. Rev. A

• A. Peralta Conde, J. Kruse, O. Faucher, P. Tzallas, E. P. Benis, and D. Charalambidis, “Realization of time-resolved two-vacuum-ultraviolet-photon ionization,” Phys. Rev. A 79(6), 061405 (2009). [CrossRef]

Phys. Rev. Lett.

• H. Mashiko, S. Gilbertson, C. Li, S. D. Khan, M. M. Shakya, E. Moon, and Z. Chang, “Double optical gating of high-order harmonic generation with carrier-envelope phase stabilized lasers,” Phys. Rev. Lett. 100(10), 103906 (2008). [CrossRef] [PubMed]
• E. Skantzakis, P. Tzallas, J. E. Kruse, C. Kalpouzos, O. Faucher, G. D. Tsakiris, and D. Charalambidis, “Tracking autoionizing-wave-packet dynamics at the 1-fs temporal scale,” Phys. Rev. Lett. 105(4), 043902 (2010). [CrossRef] [PubMed]
• N. A. Papadogiannis, L. A. A. Nikolopoulos, D. Charalambidis, G. D. Tsakiris, P. Tzallas, and K. Witte, “Two-photon ionization of he through a superposition of higher harmonics,” Phys. Rev. Lett. 90(13), 133902 (2003). [CrossRef] [PubMed]
• L. Nugent-Glandorf, M. Scheer, D. A. Samuels, A. M. Mulhisen, E. R. Grant, X. Yang, V. M. Bierbaum, and S. R. Leone, “Ultrafast time-resolved soft x-ray photoelectron spectroscopy of dissociating Br2.,” Phys. Rev. Lett. 87(19), 193002 (2001). [CrossRef] [PubMed]
• P. Wernet, M. Odelius, K. Godehusen, J. Gaudin, O. Schwarzkopf, and W. Eberhardt, “Real-time evolution of the valence electronic structure in a dissociating molecule,” Phys. Rev. Lett. 103(1), 013001 (2009). [CrossRef] [PubMed]
• Y. Nabekawa, H. Hasegawa, E. J. Takahashi, and K. Midorikawa, “Production of doubly charged helium ions by two-photon absorption of an intense sub-10-fs soft x-ray pulse at 42 eV photon energy,” Phys. Rev. Lett. 94(4), 043001 (2005). [CrossRef] [PubMed]
• A. Kosuge, T. Sekikawa, X. Zhou, T. Kanai, S. Adachi, and S. Watanabe, “Frequency-resolved optical gating of isolated attosecond pulses in the extreme ultraviolet,” Phys. Rev. Lett. 97(26), 263901 (2006). [CrossRef]
• Y. Hikosaka, M. Fushitani, A. Matsuda, C.-M. Tseng, A. Hishikawa, E. Shigemasa, M. Nagasono, K. Tono, T. Togashi, H. Ohashi, H. Kimura, Y. Senba, M. Yabashi, and T. Ishikawa, “Multiphoton double ionization of Ar in intense extreme ultraviolet laser fields studied by shot-by-shot photoelectron spectroscopy,” Phys. Rev. Lett. 105(13), 133001 (2010). [CrossRef]
• A. Hishikawa, A. Matsuda, M. Fushitani, and E. J. Takahashi, “Visualizing recurrently migrating hydrogen in acetylene dication by intense ultrashort laser pulses,” Phys. Rev. Lett. 99(25), 258302 (2007). [CrossRef]

Rev. Mod. Phys.

• T. Brabec and F. Krausz, “Intense few-cycle laser fields: Frontiers of nonlinear optics,” Rev. Mod. Phys. 72(2), 545–591 (2000). [CrossRef]

Science

• E. Goulielmakis, M. Schultze, M. Hofstetter, V. S. Yakovlev, J. Gagnon, M. Uiberacker, A. L. Aquila, E. M. Gullikson, D. T. Attwood, R. Kienberger, F. Krausz, and U. Kleineberg, “Single-cycle nonlinear optics,” Science 320(5883), 1614–1617 (2008). [CrossRef] [PubMed]
• E. Gagnon, P. Ranitovic, X.-M. Tong, C. L. Cocke, M. M. Murnane, H. C. Kapteyn, and A. S. Sandhu, “Soft X-ray-driven femtosecond molecular dynamics,” Science 317(5843), 1374–1378 (2007). [CrossRef] [PubMed]

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