OSA's Digital Library

Optics Express

Optics Express

  • Editor: Andrew M. Weiner
  • Vol. 22, Iss. 1 — Jan. 13, 2014
  • pp: 1105–1113

Femtosecond time-resolved X-ray absorption spectroscopy of liquid using a hard X-ray free electron laser in a dual-beam dispersive detection method

Yuki Obara, Tetsuo Katayama, Yoshihiro Ogi, Takayuki Suzuki, Naoya Kurahashi, Shutaro Karashima, Yuhei Chiba, Yusuke Isokawa, Tadashi Togashi, Yuichi Inubushi, Makina Yabashi, Toshinori Suzuki, and Kazuhiko Misawa  »View Author Affiliations

Optics Express, Vol. 22, Issue 1, pp. 1105-1113 (2014)

View Full Text Article

Enhanced HTML    Acrobat PDF (3084 KB)

Browse Journals / Lookup Meetings

Browse by Journal and Year


Lookup Conference Papers

Close Browse Journals / Lookup Meetings

Article Tools



We present femtosecond time-resolved X-ray absorption spectroscopy of aqueous solution using a hard x-ray free electron laser (SACLA) and a synchronized Ti:sapphire laser. The instrumental response time is 200 fs, and the repetition rate of measurement is 10 Hz. A cylindrical liquid beam 100 μm in diameter of aqueous ammonium iron(III) oxalate solution is photoexcited at 400 nm, and the transient X-ray absorption spectra are measured in the K-edge region of iron, 7.10 − 7.26 keV, using a dual X-ray beam dispersive detection method. Each of the dual beams has the pulse energy of 1.4 μJ, and pump-induced absorbance change on the order of 10−3 is successfully detected. The photoexcited iron complex exhibits a red shifted iron K-edge with the appearance time constant of 260 fs. The X-ray absorption difference spectra, with and without the pump pulses, are independent of time delay after 1.5 ps up to 100 ps, indicating that the photoexcited species is long-lived.

© 2014 Optical Society of America

OCIS Codes
(140.2600) Lasers and laser optics : Free-electron lasers (FELs)
(320.7120) Ultrafast optics : Ultrafast phenomena
(320.7150) Ultrafast optics : Ultrafast spectroscopy

ToC Category:
X-ray Optics

Original Manuscript: November 1, 2013
Revised Manuscript: December 23, 2013
Manuscript Accepted: December 23, 2013
Published: January 10, 2014

Yuki Obara, Tetsuo Katayama, Yoshihiro Ogi, Takayuki Suzuki, Naoya Kurahashi, Shutaro Karashima, Yuhei Chiba, Yusuke Isokawa, Tadashi Togashi, Yuichi Inubushi, Makina Yabashi, Toshinori Suzuki, and Kazuhiko Misawa, "Femtosecond time-resolved X-ray absorption spectroscopy of liquid using a hard X-ray free electron laser in a dual-beam dispersive detection method," Opt. Express 22, 1105-1113 (2014)

Sort:  Author  |  Year  |  Journal  |  Reset  


  1. T. J. Penfold, C. J. Milne, and M. Chergui, “Recent advances in ultrafast X-ray absorption spectroscopy of solutions,” in Advances in Chemical Physics, S. A. Rice and A. R. Dinner, eds. (John Wiley, 2013), vol. 153.
  2. L. X. Chen, “Probing transient molecular structures in photochemical processes using laser-initiated time-resolved X-ray absorption spectroscopy,” Annu. Rev. Phys. Chem. 56(1), 221–254 (2005). [CrossRef] [PubMed]
  3. L. X. Chen, W. J. H. Jäger, G. Jennings, D. J. Gosztola, A. Munkholm, J. P. Hessler, “Capturing a photoexcited molecular structure through time-domain X-ray absorption fine structure,” Science 292(5515), 262–264 (2001). [CrossRef] [PubMed]
  4. J. J. Rehr, R. C. Albers, “Theoretical approaches to x-ray absorption fine structure,” Rev. Mod. Phys. 72(3), 621–654 (2000). [CrossRef]
  5. P. A. Lee, P. H. Citrin, P. Eisenberger, B. M. Kincaid, “Extended X-ray absorption fine structure—its strengths and limitations as a structural tool,” Rev. Mod. Phys. 53(4), 769–806 (1981). [CrossRef]
  6. S. Nozawa, T. Sato, M. Chollet, K. Ichiyanagi, A. Tomita, H. Fujii, S. Adachi, S. Y. Koshihara, “Direct Probing of spin state dynamics coupled with electronic and structural modifications by picosecond time-resolved XAFS,” J. Am. Chem. Soc. 132(1), 61–63 (2010). [CrossRef] [PubMed]
  7. R. W. Schoenlein, S. Chattopadhyay, H. H. W. Chong, T. E. Glover, P. A. Heimann, C. V. Shank, A. A. Zholents, M. S. Zolotorev, “Generation of femtosecond pulses of synchrotron radiation,” Science 287(5461), 2237–2240 (2000). [CrossRef] [PubMed]
  8. S. Khan, K. Holldack, T. Kachel, R. Mitzner, T. Quast, “Femtosecond undulator radiation from sliced electron bunches,” Phys. Rev. Lett. 97(7), 074801 (2006). [CrossRef] [PubMed]
  9. P. Beaud, S. L. Johnson, A. Streun, R. Abela, D. Abramsohn, D. Grolimund, F. Krasniqi, T. Schmidt, V. Schlott, G. Ingold, “Spatiotemporal stability of a femtosecond hard-X-ray undulator source studied by control of coherent optical phonons,” Phys. Rev. Lett. 99(17), 174801 (2007). [CrossRef] [PubMed]
  10. Ch. Bressler, C. Milne, V.-T. Pham, A. Elnahhas, R. M. van der Veen, W. Gawelda, S. Johnson, P. Beaud, D. Grolimund, M. Kaiser, C. N. Borca, G. Ingold, R. Abela, M. Chergui, “Femtosecond XANES study of the light-induced spin crossover dynamics in an iron(II) complex,” Science 323(5913), 489–492 (2009). [CrossRef] [PubMed]
  11. V.-T. Pham, T. J. Penfold, R. M. van der Veen, F. A. Lima, A. El Nahhas, S. L. Johnson, P. Beaud, R. Abela, C. Bressler, I. Tavernelli, C. J. Milne, M. Chergui, “Probing the transition from hydrophilic to hydrophobic solvation with atomic scale resolution,” J. Am. Chem. Soc. 133(32), 12740–12748 (2011). [CrossRef] [PubMed]
  12. M. M. Murnane, H. C. Kapteyn, R. W. Falcone, “High density plasmas produced by ultrafast laser pulses,” Phys. Rev. Lett. 62(2), 155–158 (1989). [CrossRef] [PubMed]
  13. F. Ráksi, K. R. Wilson, Z. Jiang, A. Ikhlef, C. Y. Côté, J.-C. Kieffer, “Ultrafast X-ray absorption probing of a chemical reaction,” J. Chem. Phys. 104, 6066–6069 (1996). [CrossRef]
  14. J. Chen, H. Zhang, I. V. Tomov, M. Wolfsberg, X. Ding, P. M. Rentzepis, “Transient structures and kinetics of the ferrioxalate redox reaction studied by time-resolved EXAFS, optical spectroscopy, and DFT,” J. Phys. Chem. A 111(38), 9326–9335 (2007). [CrossRef] [PubMed]
  15. W.-K. Chen, J. Chen, P. M. Rentzepis, “Electron transfer mechanism in organometallic molecules studied by subpicosecond extended X-ray absorption fine structure spectroscopy,” J. Phys. Chem. B 117(16), 4332–4339 (2013). [CrossRef] [PubMed]
  16. P. Emma, R. Akre, J. Arthur, R. Bionta, C. Bostedt, J. Bozek, A. Brachmann, P. Bucksbaum, R. Coffee, F.-J. Decker, Y. Ding, D. Dowell, S. Edstrom, A. Fisher, J. Frisch, S. Gilevich, J. Hastings, G. Hays, Ph. Hering, Z. Huang, R. Iverson, H. Loos, M. Messerschmidt, A. Miahnahri, S. Moeller, H.-D. Nuhn, G. Pile, D. Ratner, J. Rzepiela, D. Schultz, T. Smith, P. Stefan, H. Tompkins, J. Turner, J. Welch, W. White, J. Wu, G. Yocky, J. Galayda, “First lasing and operation of an Ångstrom-wavelength free-electron laser,” Nat. Photonics 4(9), 641–647 (2010). [CrossRef]
  17. T. Ishikawa, H. Aoyagi, T. Asaka, Y. Asano, N. Azumi, T. Bizen, H. Ego, K. Fukami, T. Fukui, Y. Furukawa, S. Goto, H. Hanaki, T. Hara, T. Hasegawa, T. Hatsui, A. Higashiya, T. Hirono, N. Hosoda, M. Ishii, T. Inagaki, Y. Inubushi, T. Itoga, Y. Joti, M. Kago, T. Kameshima, H. Kimura, Y. Kirihara, A. Kiyomichi, T. Kobayashi, C. Kondo, T. Kudo, H. Maesaka, X. M. Maréchal, T. Masuda, S. Matsubara, T. Matsumoto, T. Matsushita, S. Matsui, M. Nagasono, N. Nariyama, H. Ohashi, T. Ohata, T. Ohshima, S. Ono, Y. Otake, C. Saji, T. Sakurai, T. Sato, K. Sawada, T. Seike, K. Shirasawa, T. Sugimoto, S. Suzuki, S. Takahashi, H. Takebe, K. Takeshita, K. Tamasaku, H. Tanaka, R. Tanaka, T. Tanaka, T. Togashi, K. Togawa, A. Tokuhisa, H. Tomizawa, K. Tono, S. Wu, M. Yabashi, M. Yamaga, A. Yamashita, K. Yanagida, C. Zhang, T. Shintake, H. Kitamura, N. Kumagai, “A compact X-ray free-electron laser emitting in the sub-Ångström region,” Nat. Photonics 6(8), 540–544 (2012). [CrossRef]
  18. Y. Inubushi, K. Tono, T. Togashi, T. Sato, T. Hatsui, T. Kameshima, K. Togawa, T. Hara, T. Tanaka, H. Tanaka, T. Ishikawa, M. Yabashi, “Determination of the pulse duration of an X-ray free electron laser using highly resolved single-shot spectra,” Phys. Rev. Lett. 109(14), 144801 (2012). [CrossRef] [PubMed]
  19. H. T. Lemke, C. Bressler, L. X. Chen, D. M. Fritz, K. J. Gaffney, A. Galler, W. Gawelda, K. Haldrup, R. W. Hartsock, H. Ihee, J. Kim, K.-H. Kim, J.-H. Lee, M. M. Nielsen, A. B. Stickrath, W. Zhang, D. Zhu, M. Cammarata, “Femtosecond X-ray absorption spectroscopy at a hard X-ray free electron laser: application to spin crossover dynamics,” J. Phys. Chem. A 117(4), 735–740 (2013). [CrossRef] [PubMed]
  20. R. Bonifacio, C. Pellegrini, L. M. Narducci, “Collective instabilities and high-gain regime in a free electron laser,” Opt. Commun. 50(6), 373–378 (1984). [CrossRef]
  21. T. Katayama, Y. Inubushi, Y. Obara, T. Sato, T. Togashi, K. Tono, T. Hatsui, T. Kameshima, A. Bhattacharya, Y. Ogi, N. Kurahashi, K. Misawa, T. Suzuki, M. Yabashi, “Femtosecond x-ray absorption spectroscopy with hard x-ray free electron laser,” Appl. Phys. Lett. 103(13), 131105 (2013). [CrossRef]
  22. C. A. Parker, C. G. Hatchard, “Photodecomposition of complex oxalates—some preliminary experiments by flash photolysis,” J. Phys. Chem. 63(1), 22–26 (1959). [CrossRef]
  23. B. A. DeGraff, G. D. Cooper, “Photochemistry of the ferrioxalate system,” J. Phys. Chem. 75(19), 2897–2902 (1971). [CrossRef]
  24. M. Yabashi, J. B. Hastings, M. S. Zolotorev, H. Mimura, H. Yumoto, S. Matsuyama, K. Yamauchi, T. Ishikawa, “Single-shot spectrometry for X-ray free-electron lasers,” Phys. Rev. Lett. 97(8), 084802 (2006). [CrossRef] [PubMed]
  25. M. Saes, F. van Mourik, W. Gawelda, M. Kaiser, M. Chergui, C. Bressler, D. Grolimund, R. Abela, T. E. Glover, P. A. Heimann, R. W. Schoenlein, S. L. Johnson, A. M. Lindenberg, R. W. Falcone, “A setup for ultrafast time-resolved X-ray absorption spectroscopy,” Rev. Sci. Instrum. 75(1), 24–30 (2004). [CrossRef]
  26. W. Gawelda, V.-T. Pham, M. Benfatto, Y. Zaushitsyn, M. Kaiser, D. Grolimund, S. L. Johnson, R. Abela, A. Hauser, C. Bressler, M. Chergui, “Structural determination of a short-lived excited iron(II) complex by picosecond X-ray absorption spectroscopy,” Phys. Rev. Lett. 98(5), 057401 (2007). [CrossRef] [PubMed]

Cited By

Alert me when this paper is cited

OSA is able to provide readers links to articles that cite this paper by participating in CrossRef's Cited-By Linking service. CrossRef includes content from more than 3000 publishers and societies. In addition to listing OSA journal articles that cite this paper, citing articles from other participating publishers will also be listed.


Fig. 1 Fig. 2 Fig. 3
Fig. 4 Fig. 5

« Previous Article  |  Next Article »

OSA is a member of CrossRef.

CrossCheck Deposited