The rotating-crystal method in femtosecond X-ray diffraction

B. Freyer; J. Stingl; F. Zamponi; M. Woerner; T. Elsaesser

doi:10.1364/OE.19.015506

The rotating-crystal method in femtosecond X-ray diffraction

B. Freyer, J. Stingl, F. Zamponi, M. Woerner, and T. Elsaesser

Optics Express
Vol. 19,
Issue 16,
pp. 15506-15515
(2011)
•https://doi.org/10.1364/OE.19.015506

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B. Freyer, J. Stingl, F. Zamponi, M. Woerner, and T. Elsaesser, "The rotating-crystal method in femtosecond X-ray diffraction," Opt. Express 19, 15506-15515 (2011)

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Related Topics
Table of Contents Category
- X-ray Optics
Optics & Photonics Topics
?

The topics in this list come from the OSA Optics and Photonics Topics applied to this article.
Previously assigned OCIS codes
- Equipment and techniques (000.2170)
- Femtosecond phenomena (320.2250)
- X-rays, soft x-rays, extreme ultraviolet (EUV) (340.7480)

About this Article
History
- Original Manuscript: May 23, 2011
- Revised Manuscript: June 23, 2011
- Manuscript Accepted: July 5, 2011
- Published: July 28, 2011

Accessible

Open Access

Abstract

We report the first implementation of the rotating-crystal method in femtosecond X-ray diffraction. Applying a pump-probe scheme with 100 fs hard X-ray probe pulses from a laser-driven plasma source, the novel technique is demonstrated by mapping structural dynamics of a photoexcited bismuth crystal via changes of the diffracted intensity on a multitude of Bragg reflections. The method is compared to femtosecond powder diffraction and to Bragg diffraction from a crystal with stationary orientation.

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References

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|
Year
|
Author
|
Publication

E. Colleted., “Dynamical structural science,” Acta Crystallogr., Sect. A 66, 133–280 (2010).
[Crossref] [PubMed]
A. Rousse, C. Rischel, and J. C. Gauthier, “Colloquium: femtosecond x-ray crystallography,” Rev. Mod. Phys. 73, 17–31 (2001).
[Crossref]
T. Elsaesser and M. Woerner, “Photoinduced structural dynamics of polar solids studied by femtosecond x-ray diffraction,” Acta Crystallogr., Sect. A 66, 168–178 (2010).
[Crossref] [PubMed]
W. L. Bragg, “The structure of some crystals as indicated by their diffraction of x-rays,” Proc. R. Soc. London, Ser. A 89, 248–277 (1913).
[Crossref]
C. Rischel, A. Rousse, I. Uschmann, P.-A. Albouy, J.-P. Geindre, P. Audebert, J.-C. Gauthier, E. Forster, J.-L. Martin, and A. Antonetti, “Femtosecond time-resolved X-ray diffraction from laser-heated organic films,” Nature 390, 490–492 (1997).
[Crossref]
C. Rose-Petruck, R. Jiminez, T. Guo, A. Cavalleri, C. Siders, J. A. Squier, B. C. Walker, and K. R. Wilson, “Picosecond millianstrom lattice dynamics measured by ultrafast x-ray diffraction,” Nature 398, 310–312 (1999).
[Crossref]
E. Collet, M.-H. Leme-Cailleau, M. Buron-Le Cointe, H. Cailleau, M. Wulff, T. Luty, S.-Y. Koshihara, M. Meyer, L. Toupet, P. Rabiller, and S. Techert, “Laser-induced ferroelectric structural order in an organic charge-transfer crystal,” Science 300, 612–615 (2003).
[Crossref] [PubMed]
K. Sokolowski-Tinten, C. Blome, J. Blums, A. Cavalleri, C. Dietrich, A. Tarasevitch, I. Uschmann, E. Förster, M. Kammler, M. Horn-von-Hoegen, and D. von der Linde, “Femtosecond X-ray measurement of coherent lattice vibrations near the Lindemann stability limit,” Nature 422, 287–289 (2003).
[Crossref] [PubMed]
M. Bargheer, N. Zhavoronkov, Y. Gritsai, J. C. Woo, D. S. Kim, M. Woerner, and T. Elsaesser, “Coherent atomic motions in a nanostructure studied by femtosecond x-ray diffraction,” Science 306, 1771–1773 (2004).
[Crossref] [PubMed]
D. M. Fritz, D. A. Reis, B. Adams, R. A. Akre, J. Arthur, C. Blome, P. H. Bucksbaum, A. L. Cavalieri, S. Engemann, S. Fahy, R. W. Falcone, P. H. Fuoss, K. J. Gaffney, M. J. George, J. Hajdu, M. P. Hertlein, P. B. Hillyard, M. Horn-von Hoegen, M. Kammler, J. Kaspar, R. Kienberger, P. Krejcik, S. H. Lee, A. M. Lindenberg, B. McFarland, D. Meyer, T. Montagne, A. D. Murray, A. J. Nelson, M. Nicoul, R. Pahl, J. Rudati, H. Schlarb, D. P. Siddons, K. Sokolowski-Tinten, T. Tschentscher, D. von der Linde, and J. B. Hastings, “Ultrafast bond softening in bismuth: mapping a solid’s interatomic potential with x-rays,” Science 315, 633–636 (2007).
[Crossref] [PubMed]
C. v. Korff Schmising, M. Bargheer, M. Kiel, N. Zhavoronkov, M. Woerner, T. Elsaesser, I. Vrejoiu, D. Hesse, and M. Alexe, “Coupled ultrafast lattice and polarization dynamics in ferroelectric nanolayers,” Phys. Rev. Lett. 98, 257601 (2007).
[Crossref]
S. L. Johnson, P. Beaud, C. J. Milne, F. S. Krasniqi, E. S. Zijlstra, M. E. Garcia, M. Kaiser, D. Grolimund, R. Abela, and G. Ingold, “Nanoscale depth-resolved coherent femtosecond motion in laser-excited bismuth,” Phys. Rev. Lett. 100, 155501 (2008).
[Crossref] [PubMed]
F. Zamponi, Z. Ansari, M. Woerner, and T. Elsaesser, “Femtosecond powder diffraction with a laser-driven hard x-ray source,” Opt. Express 18, 947–961 (2010).
[Crossref] [PubMed]
M. Woerner, F. Zamponi, Z. Ansari, J. Dreyer, B. Freyer, M. Premont-Schwarz, and T. Elsaesser, “Concerted electron and proton transfer in ionic crystals mapped by femtosecond x-ray powder diffraction,” J. Chem. Phys. 133, 064509 (2010).
[Crossref] [PubMed]
B. E. Warren, X-ray Diffraction (Dover Publications, 1990).
C. Giacovazzo, Fundamentals of Crystallography (Oxford University Press, 2002).
[PubMed]
U. W. Arndt, J. N. Champness, R. P. Phizackerley, and A. J. Wonacott, “A single-crystal oscillation camera for large unit cells,” J. Appl. Cryst. 6, 457–463 (1973).
[Crossref]
L. D. Landau, E. M. Lifshitz, and L. P. Pitaevskii, Electrodynamics of Continuous Media, 2nd ed. (Butterworth-Heinenann, 1984).
N. Zhavoronkov, Y. Gritsai, M. Bargheer, M. Woerner, Th. Elsaesser, F. Zamponi, I. Uschmann, and E. Förster, “Microfocus Cu Kα source for femtosecond x-ray science,” Opt. Lett. 30, 1737–1739 (2005).
[Crossref] [PubMed]
M. Bargheer, N. Zhavoronkov, R. Bruch, H. Legall, H. Stiel, M. Woerner, and T. Elsaesser, “Comparison of focusing optics for femtosecond X-ray diffraction,” Appl. Phys. B 80, 715–719 (2005).
[Crossref]
It is important to note that the experimentally observed damage does not change the X-ray diffraction pattern, i.e., the crystal structure, but the surface quality of the single crystal and, thus, the coupling of the optical pump beam into the crystal.
S. L. Johnson, P. Beaud, E. Vorobeva, C. J. Milne, E. D. Murray, S. Fahy, and G. Ingold, “Directly observing squeezed phonon states with femtosecond x-ray diffraction,” Phys. Rev. Lett. 102, 175503 (2009).
[Crossref] [PubMed]
S. L. Johnson, P. Beaud, E. Vorobeva, C. J. Milne, É. D. Murray, S. Fahy, and G. Ingold, “Non-equilibrium phonon dynamics studied by grazing-incidence femtosecond X-ray crystallography,” Acta Crystallogr., Sect. A 66, 157–167 (2010).
[Crossref] [PubMed]
W. Lu, M. Nicoul, U. Shymanovich, A. Tarasevitch, M. Kammler, M. Horn von Hoegen, D. von der Linde, and K. Sokolowski-Tinten, “Transient reversal of a Peierls-transition: Extreme phonon softening in laser-excited Bismuth,” in Ultrafast Phenomena XVII, M. Chergui, D. Jonas, E. Riedle, R. Schoenlein, and A. Taylor, eds. (Oxford University Press, 2011).
J. B. Woodhouse, A. L. A. Fields, and I. A. Bucklow, “X-ray mass absorption coefficients for gold, lead and bismuth in the range 1–10 Å,” J. Phys. D: Appl. Phys, 7, 483–489 (1974).
[Crossref]

2010 (5)

E. Colleted., “Dynamical structural science,” Acta Crystallogr., Sect. A 66, 133–280 (2010).
[Crossref] [PubMed]

T. Elsaesser and M. Woerner, “Photoinduced structural dynamics of polar solids studied by femtosecond x-ray diffraction,” Acta Crystallogr., Sect. A 66, 168–178 (2010).
[Crossref] [PubMed]

S. L. Johnson, P. Beaud, E. Vorobeva, C. J. Milne, É. D. Murray, S. Fahy, and G. Ingold, “Non-equilibrium phonon dynamics studied by grazing-incidence femtosecond X-ray crystallography,” Acta Crystallogr., Sect. A 66, 157–167 (2010).
[Crossref] [PubMed]

M. Woerner, F. Zamponi, Z. Ansari, J. Dreyer, B. Freyer, M. Premont-Schwarz, and T. Elsaesser, “Concerted electron and proton transfer in ionic crystals mapped by femtosecond x-ray powder diffraction,” J. Chem. Phys. 133, 064509 (2010).
[Crossref] [PubMed]

F. Zamponi, Z. Ansari, M. Woerner, and T. Elsaesser, “Femtosecond powder diffraction with a laser-driven hard x-ray source,” Opt. Express 18, 947–961 (2010).
[Crossref] [PubMed]

2009 (1)

S. L. Johnson, P. Beaud, E. Vorobeva, C. J. Milne, E. D. Murray, S. Fahy, and G. Ingold, “Directly observing squeezed phonon states with femtosecond x-ray diffraction,” Phys. Rev. Lett. 102, 175503 (2009).
[Crossref] [PubMed]

2008 (1)

S. L. Johnson, P. Beaud, C. J. Milne, F. S. Krasniqi, E. S. Zijlstra, M. E. Garcia, M. Kaiser, D. Grolimund, R. Abela, and G. Ingold, “Nanoscale depth-resolved coherent femtosecond motion in laser-excited bismuth,” Phys. Rev. Lett. 100, 155501 (2008).
[Crossref] [PubMed]

2007 (2)

D. M. Fritz, D. A. Reis, B. Adams, R. A. Akre, J. Arthur, C. Blome, P. H. Bucksbaum, A. L. Cavalieri, S. Engemann, S. Fahy, R. W. Falcone, P. H. Fuoss, K. J. Gaffney, M. J. George, J. Hajdu, M. P. Hertlein, P. B. Hillyard, M. Horn-von Hoegen, M. Kammler, J. Kaspar, R. Kienberger, P. Krejcik, S. H. Lee, A. M. Lindenberg, B. McFarland, D. Meyer, T. Montagne, A. D. Murray, A. J. Nelson, M. Nicoul, R. Pahl, J. Rudati, H. Schlarb, D. P. Siddons, K. Sokolowski-Tinten, T. Tschentscher, D. von der Linde, and J. B. Hastings, “Ultrafast bond softening in bismuth: mapping a solid’s interatomic potential with x-rays,” Science 315, 633–636 (2007).
[Crossref] [PubMed]

C. v. Korff Schmising, M. Bargheer, M. Kiel, N. Zhavoronkov, M. Woerner, T. Elsaesser, I. Vrejoiu, D. Hesse, and M. Alexe, “Coupled ultrafast lattice and polarization dynamics in ferroelectric nanolayers,” Phys. Rev. Lett. 98, 257601 (2007).
[Crossref]

2005 (2)

M. Bargheer, N. Zhavoronkov, R. Bruch, H. Legall, H. Stiel, M. Woerner, and T. Elsaesser, “Comparison of focusing optics for femtosecond X-ray diffraction,” Appl. Phys. B 80, 715–719 (2005).
[Crossref]

N. Zhavoronkov, Y. Gritsai, M. Bargheer, M. Woerner, Th. Elsaesser, F. Zamponi, I. Uschmann, and E. Förster, “Microfocus Cu Kα source for femtosecond x-ray science,” Opt. Lett. 30, 1737–1739 (2005).
[Crossref] [PubMed]

2004 (1)

M. Bargheer, N. Zhavoronkov, Y. Gritsai, J. C. Woo, D. S. Kim, M. Woerner, and T. Elsaesser, “Coherent atomic motions in a nanostructure studied by femtosecond x-ray diffraction,” Science 306, 1771–1773 (2004).
[Crossref] [PubMed]

2003 (2)

E. Collet, M.-H. Leme-Cailleau, M. Buron-Le Cointe, H. Cailleau, M. Wulff, T. Luty, S.-Y. Koshihara, M. Meyer, L. Toupet, P. Rabiller, and S. Techert, “Laser-induced ferroelectric structural order in an organic charge-transfer crystal,” Science 300, 612–615 (2003).
[Crossref] [PubMed]

K. Sokolowski-Tinten, C. Blome, J. Blums, A. Cavalleri, C. Dietrich, A. Tarasevitch, I. Uschmann, E. Förster, M. Kammler, M. Horn-von-Hoegen, and D. von der Linde, “Femtosecond X-ray measurement of coherent lattice vibrations near the Lindemann stability limit,” Nature 422, 287–289 (2003).
[Crossref] [PubMed]

2001 (1)

A. Rousse, C. Rischel, and J. C. Gauthier, “Colloquium: femtosecond x-ray crystallography,” Rev. Mod. Phys. 73, 17–31 (2001).
[Crossref]

1999 (1)

C. Rose-Petruck, R. Jiminez, T. Guo, A. Cavalleri, C. Siders, J. A. Squier, B. C. Walker, and K. R. Wilson, “Picosecond millianstrom lattice dynamics measured by ultrafast x-ray diffraction,” Nature 398, 310–312 (1999).
[Crossref]

1997 (1)

C. Rischel, A. Rousse, I. Uschmann, P.-A. Albouy, J.-P. Geindre, P. Audebert, J.-C. Gauthier, E. Forster, J.-L. Martin, and A. Antonetti, “Femtosecond time-resolved X-ray diffraction from laser-heated organic films,” Nature 390, 490–492 (1997).
[Crossref]

1974 (1)

J. B. Woodhouse, A. L. A. Fields, and I. A. Bucklow, “X-ray mass absorption coefficients for gold, lead and bismuth in the range 1–10 Å,” J. Phys. D: Appl. Phys, 7, 483–489 (1974).
[Crossref]

1973 (1)

U. W. Arndt, J. N. Champness, R. P. Phizackerley, and A. J. Wonacott, “A single-crystal oscillation camera for large unit cells,” J. Appl. Cryst. 6, 457–463 (1973).
[Crossref]

1913 (1)

W. L. Bragg, “The structure of some crystals as indicated by their diffraction of x-rays,” Proc. R. Soc. London, Ser. A 89, 248–277 (1913).
[Crossref]

Abela, R.

Adams, B.

Akre, R. A.

Albouy, P.-A.

Alexe, M.

Ansari, Z.

F. Zamponi, Z. Ansari, M. Woerner, and T. Elsaesser, “Femtosecond powder diffraction with a laser-driven hard x-ray source,” Opt. Express 18, 947–961 (2010).
[Crossref] [PubMed]

Antonetti, A.

Arndt, U. W.

U. W. Arndt, J. N. Champness, R. P. Phizackerley, and A. J. Wonacott, “A single-crystal oscillation camera for large unit cells,” J. Appl. Cryst. 6, 457–463 (1973).
[Crossref]

Arthur, J.

Audebert, P.

Bargheer, M.

Beaud, P.

Blome, C.

Blums, J.

Bragg, W. L.

W. L. Bragg, “The structure of some crystals as indicated by their diffraction of x-rays,” Proc. R. Soc. London, Ser. A 89, 248–277 (1913).
[Crossref]

Bruch, R.

Bucklow, I. A.

Bucksbaum, P. H.

Buron-Le Cointe, M.

Cailleau, H.

Cavalieri, A. L.

Cavalleri, A.

Champness, J. N.

U. W. Arndt, J. N. Champness, R. P. Phizackerley, and A. J. Wonacott, “A single-crystal oscillation camera for large unit cells,” J. Appl. Cryst. 6, 457–463 (1973).
[Crossref]

Collet, E.

Dietrich, C.

Dreyer, J.

Elsaesser, T.

F. Zamponi, Z. Ansari, M. Woerner, and T. Elsaesser, “Femtosecond powder diffraction with a laser-driven hard x-ray source,” Opt. Express 18, 947–961 (2010).
[Crossref] [PubMed]

T. Elsaesser and M. Woerner, “Photoinduced structural dynamics of polar solids studied by femtosecond x-ray diffraction,” Acta Crystallogr., Sect. A 66, 168–178 (2010).
[Crossref] [PubMed]

Elsaesser, Th.

Engemann, S.

Fahy, S.

Falcone, R. W.

Fields, A. L. A.

Forster, E.

Förster, E.

Freyer, B.

Fritz, D. M.

Fuoss, P. H.

Gaffney, K. J.

Garcia, M. E.

Gauthier, J. C.

A. Rousse, C. Rischel, and J. C. Gauthier, “Colloquium: femtosecond x-ray crystallography,” Rev. Mod. Phys. 73, 17–31 (2001).
[Crossref]

Gauthier, J.-C.

Geindre, J.-P.

George, M. J.

Giacovazzo, C.

C. Giacovazzo, Fundamentals of Crystallography (Oxford University Press, 2002).
[PubMed]

Gritsai, Y.

Grolimund, D.

Guo, T.

Hajdu, J.

Hastings, J. B.

Hertlein, M. P.

Hesse, D.

Hillyard, P. B.

Horn von Hoegen, M.

W. Lu, M. Nicoul, U. Shymanovich, A. Tarasevitch, M. Kammler, M. Horn von Hoegen, D. von der Linde, and K. Sokolowski-Tinten, “Transient reversal of a Peierls-transition: Extreme phonon softening in laser-excited Bismuth,” in Ultrafast Phenomena XVII, M. Chergui, D. Jonas, E. Riedle, R. Schoenlein, and A. Taylor, eds. (Oxford University Press, 2011).

Horn-von Hoegen, M.

Horn-von-Hoegen, M.

Ingold, G.

Jiminez, R.

Johnson, S. L.

Kaiser, M.

Kammler, M.

Kaspar, J.

Kiel, M.

Kienberger, R.

Kim, D. S.

Korff Schmising, C. v.

Koshihara, S.-Y.

Krasniqi, F. S.

Krejcik, P.

Landau, L. D.

L. D. Landau, E. M. Lifshitz, and L. P. Pitaevskii, Electrodynamics of Continuous Media, 2nd ed. (Butterworth-Heinenann, 1984).

Lee, S. H.

Legall, H.

Leme-Cailleau, M.-H.

Lifshitz, E. M.

L. D. Landau, E. M. Lifshitz, and L. P. Pitaevskii, Electrodynamics of Continuous Media, 2nd ed. (Butterworth-Heinenann, 1984).

Lindenberg, A. M.

Lu, W.

Luty, T.

Martin, J.-L.

McFarland, B.

Meyer, D.

Meyer, M.

Milne, C. J.

Montagne, T.

Murray, A. D.

Murray, E. D.

Murray, É. D.

Nelson, A. J.

Nicoul, M.

Pahl, R.

Phizackerley, R. P.

U. W. Arndt, J. N. Champness, R. P. Phizackerley, and A. J. Wonacott, “A single-crystal oscillation camera for large unit cells,” J. Appl. Cryst. 6, 457–463 (1973).
[Crossref]

Pitaevskii, L. P.

L. D. Landau, E. M. Lifshitz, and L. P. Pitaevskii, Electrodynamics of Continuous Media, 2nd ed. (Butterworth-Heinenann, 1984).

Premont-Schwarz, M.

Rabiller, P.

Reis, D. A.

Rischel, C.

A. Rousse, C. Rischel, and J. C. Gauthier, “Colloquium: femtosecond x-ray crystallography,” Rev. Mod. Phys. 73, 17–31 (2001).
[Crossref]

Rose-Petruck, C.

Rousse, A.

A. Rousse, C. Rischel, and J. C. Gauthier, “Colloquium: femtosecond x-ray crystallography,” Rev. Mod. Phys. 73, 17–31 (2001).
[Crossref]

Rudati, J.

Schlarb, H.

Shymanovich, U.

Siddons, D. P.

Siders, C.

Sokolowski-Tinten, K.

Squier, J. A.

Stiel, H.

Tarasevitch, A.

Techert, S.

Toupet, L.

Tschentscher, T.

Uschmann, I.

von der Linde, D.

Vorobeva, E.

Vrejoiu, I.

Walker, B. C.

Warren, B. E.

B. E. Warren, X-ray Diffraction (Dover Publications, 1990).

Wilson, K. R.

Woerner, M.

T. Elsaesser and M. Woerner, “Photoinduced structural dynamics of polar solids studied by femtosecond x-ray diffraction,” Acta Crystallogr., Sect. A 66, 168–178 (2010).
[Crossref] [PubMed]

F. Zamponi, Z. Ansari, M. Woerner, and T. Elsaesser, “Femtosecond powder diffraction with a laser-driven hard x-ray source,” Opt. Express 18, 947–961 (2010).
[Crossref] [PubMed]

Wonacott, A. J.

U. W. Arndt, J. N. Champness, R. P. Phizackerley, and A. J. Wonacott, “A single-crystal oscillation camera for large unit cells,” J. Appl. Cryst. 6, 457–463 (1973).
[Crossref]

Woo, J. C.

Woodhouse, J. B.

Wulff, M.

Zamponi, F.

F. Zamponi, Z. Ansari, M. Woerner, and T. Elsaesser, “Femtosecond powder diffraction with a laser-driven hard x-ray source,” Opt. Express 18, 947–961 (2010).
[Crossref] [PubMed]

Zhavoronkov, N.

Zijlstra, E. S.

Acta Crystallogr., Sect. A (3)

E. Colleted., “Dynamical structural science,” Acta Crystallogr., Sect. A 66, 133–280 (2010).
[Crossref] [PubMed]

T. Elsaesser and M. Woerner, “Photoinduced structural dynamics of polar solids studied by femtosecond x-ray diffraction,” Acta Crystallogr., Sect. A 66, 168–178 (2010).
[Crossref] [PubMed]

Appl. Phys. B (1)

J. Appl. Cryst. (1)

U. W. Arndt, J. N. Champness, R. P. Phizackerley, and A. J. Wonacott, “A single-crystal oscillation camera for large unit cells,” J. Appl. Cryst. 6, 457–463 (1973).
[Crossref]

J. Chem. Phys. (1)

J. Phys. D: Appl. Phys, (1)

Nature (3)

Opt. Express (1)

F. Zamponi, Z. Ansari, M. Woerner, and T. Elsaesser, “Femtosecond powder diffraction with a laser-driven hard x-ray source,” Opt. Express 18, 947–961 (2010).
[Crossref] [PubMed]

Opt. Lett. (1)

Phys. Rev. Lett. (3)

Proc. R. Soc. London, Ser. A (1)

W. L. Bragg, “The structure of some crystals as indicated by their diffraction of x-rays,” Proc. R. Soc. London, Ser. A 89, 248–277 (1913).
[Crossref]

Rev. Mod. Phys. (1)

A. Rousse, C. Rischel, and J. C. Gauthier, “Colloquium: femtosecond x-ray crystallography,” Rev. Mod. Phys. 73, 17–31 (2001).
[Crossref]

Science (3)

Other (5)

B. E. Warren, X-ray Diffraction (Dover Publications, 1990).

C. Giacovazzo, Fundamentals of Crystallography (Oxford University Press, 2002).
[PubMed]

L. D. Landau, E. M. Lifshitz, and L. P. Pitaevskii, Electrodynamics of Continuous Media, 2nd ed. (Butterworth-Heinenann, 1984).

It is important to note that the experimentally observed damage does not change the X-ray diffraction pattern, i.e., the crystal structure, but the surface quality of the single crystal and, thus, the coupling of the optical pump beam into the crystal.

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Fig. 1 Comparison between the (a) powder diffraction and (b) rotating-crystal method. The samples were (a) an ammonium sulfate [AS, (NH₄)₂SO₄] powder sample, and (b) a single crystal of AS. The patterns were taken in the femtosecond X-ray setup with an integration time of 300 s each.

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Fig. 2 (a) Schematic of the experimental set-up for femtosecond X-ray diffraction including typical diffraction patterns. (b) Set-up for femtosecond powder diffraction. (c) Set-up for femtosecond rotating-crystal diffraction.

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Fig. 3 Femtosecond grazing-incidence rotating-crystal diffraction setup showing the 800 nm pump, X-ray probe and diffracted beams. The diamond beam splitter is a diamond single crystal, which is cut parallel to the (111) lattice plane and aligned for the (111) reflection. The CCD screen shows the four reflections which were measured in the femtosecond experiment.

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Fig. 4 Time resolved reflectivity change of the (111) reflection of Bismuth, measured under comparable experimental conditions as in [12]. The solid line is plotted to guide the eye.

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Fig. 5 Reflectivity change of particular reflections measured with the rotating-crystal experiment. The solid lines are guides to the eye.

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Equations (2)

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P_{r o t} = \frac{I_{0}}{Δ φ} \frac{r_{e}^{2} λ^{3} V F_{h k l}^{2}}{v^{2}} \frac{1 + {cos}^{2} 2 θ_{h k l}}{4 sin θ_{h k l} {\hat{H}}^{h k l} (\hat{r} \times \hat{k})}

\frac{P_{r o t}}{P_{p o w}} = \frac{1}{π} \frac{1}{cos θ} \approx \frac{1}{3}