Abstract

X-ray powder diffraction with a femtosecond time resolution is introduced to map ultrafast structural dynamics of polycrystalline condensed matter. Our pump-probe approach is based on photoexcitation of a powder sample with a femtosecond optical pulse and probing changes of its structure by diffracting a hard X-ray pulse generated in a laser-driven plasma source. We discuss the key aspects of this scheme including an analysis of detection sensitivity and angular resolution. Applying this technique to the prototype molecular material ammonium sulfate, up to 20 powder diffraction rings are recorded simultaneously with a time resolution of 100 fs. We describe how to derive transient charge density maps of the material from the extensive set of diffraction data in a quantitative way.

© 2010 Optical Society of America

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  1. A. Rousse, C. Rischel, and J. C. Gauthier "Femtosecond X-ray crystallography," Rev. Mod. Phys. 73, 17-31 (2001).
    [CrossRef]
  2. C. Rose-Petruck, R. Jiminez, T. Guo, A. Cavalleri, C. Siders, F. Raksi, J. A. Squier, B. C. Walker, K. R. Wilson, and C. P. J. Barty "Picosecond-milliangstrom lattice dynamics measured by ultrafast X-ray diffraction," Nature 398, 310-312 (1999).
    [CrossRef]
  3. K. Sokolowski-Tinten, C. Blome, J. Blums, A. Cavalleri, C. Dietrich, A. Tarasevitch, I. Uschmann, E. F¨orster, 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]
  4. 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]
  5. A. M. Lindenberg, J. Larsson, K. Sokolowski-Tinten, K. J. Gaffney, C. Blome, O. Synnergren, J. Sheppard, C. Caleman, A. G. MacPhee, D. Weinstein, and  others, "Atomic-Scale Visualization of Inertial Dynamics," Science 308, 392-395 (2005).
    [CrossRef] [PubMed]
  6. M. Braun, C. v. Korff Schmising, M . Kiel, N . Zhavoronkov, J . Dreyer, M . Bargheer, T . Elsaesser, C . Root, T. E . Schrader, P. Gilch, W . Zinth, and M . Woerner, "Ultrafast changes of molecular crystal structure induced by dipole solvation," Phys. Rev. Lett. 98, 248301 (2007).
    [CrossRef] [PubMed]
  7. N. C. Woolsey, J. S. Wark, and D. Riley, "Sub-nanosecond X-ray powder diffraction," J. Appl. Cryst. 23, 441-443 (1990).
    [CrossRef]
  8. S. Techert, F. Schotte, and M. Wulff, "Picosecond X-ray diffraction probed transient structural changes in organic solids," Phys. Rev. Lett. 86, 2030-2033 (2001).
    [CrossRef] [PubMed]
  9. S. Techert and K. A. Zachariasse, "Structure determination of the intramolecular charge transfer state in crystalline 4-(diisopropylamino) benzonitrile from picosecond X-ray diffraction," J. Am. Chem. Soc 126, 5593-5600 (2004).
    [CrossRef] [PubMed]
  10. P. Debye and P. Scherrer, "Interferenzen an regellos orientierten Teilchen im Rontgenlicht," Phys. Z. 17, 277-283 (1916).
  11. B. E. Warren, "X-ray Diffraction," (Courier Dover Publications, 1990).
  12. C. Blome, T. Tschentscher, J. Davaasambuu, P. Durand, and S. Techert, "Femtosecond time-resolved powder diffraction experiments using hard X-ray free-electron lasers," J. Sync. Rad. 11, 483-489 (2005).
  13. F. Zamponi, Z. Ansari, C. v . Korff Schmising, P . Rothhardt, N . Zhavoronkov, M . Woerner, T . Elsaesser, M . Bargheer, T . Trobitzsch-Ryll, and M . Haschke, "Femtosecond hard X-ray plasma sources with a kilohertz repetition rate," Appl. Phys. A 96, 51-58 (2009).
    [CrossRef]
  14. N. Zhavoronkov, Y. Gritsai, M. Bargheer, M. Woerner, T. Elsaesser, F. Zamponi, I. Uschmann, and E. F¨orster, "Microfocus Cu K〈 source for femtosecond X-ray science," Opt. Lett. 30, 1737-1739 (2005).
    [CrossRef] [PubMed]
  15. P. Gibbon and E. Forster, "Short-pulse laser-plasma interactions," Plasma Phys. Control. Fusion 38, 769-793 (1996).
    [CrossRef]
  16. F. Brunel, "Not-so-resonant, resonant absorption," Phys. Rev. Lett. 59, 52-55 (1987).
    [CrossRef] [PubMed]
  17. E. O. Schlemper and W. C. Hamilton, "Neutron-Diffraction Study of the Structures of Ferroelectric and Paraelectric Ammonium Sulfate," J. Chem. Phys. 44, 4498-4509 (1966).
    [CrossRef]
  18. S. Ahmed, A. M. Shamah, A. Ibrahim, and F. Hanna, "X-ray studies of the high temperature phase transition of ammonium sulphate crystals," Phys. Status Solidi(a) 115, K149-K153 (1989).
    [CrossRef]
  19. H. Rietveld, "A profile refinement method for nuclear and magnetic structures," J. Appl. Cryst. 2, 65-71 (1969).
    [CrossRef]
  20. R. Brun and F. Rademakers, "ROOT-An object oriented data analysis framework," Nucl. Instrum. Methods A 389, 81-86 (1997).
    [CrossRef]
  21. C. G. Ryan, E. J. Clayton, W. L. Griffin, S. H. Sie, and D. R. Cousens, "SNIP, a statistics-sensitive background treatment for the quantitative analysis of PIXE spectra in geoscience applications," Nucl. Instrum. Methods B 34, 396-402 (1988).
    [CrossRef]

2009 (1)

F. Zamponi, Z. Ansari, C. v . Korff Schmising, P . Rothhardt, N . Zhavoronkov, M . Woerner, T . Elsaesser, M . Bargheer, T . Trobitzsch-Ryll, and M . Haschke, "Femtosecond hard X-ray plasma sources with a kilohertz repetition rate," Appl. Phys. A 96, 51-58 (2009).
[CrossRef]

2007 (1)

M. Braun, C. v. Korff Schmising, M . Kiel, N . Zhavoronkov, J . Dreyer, M . Bargheer, T . Elsaesser, C . Root, T. E . Schrader, P. Gilch, W . Zinth, and M . Woerner, "Ultrafast changes of molecular crystal structure induced by dipole solvation," Phys. Rev. Lett. 98, 248301 (2007).
[CrossRef] [PubMed]

2005 (3)

A. M. Lindenberg, J. Larsson, K. Sokolowski-Tinten, K. J. Gaffney, C. Blome, O. Synnergren, J. Sheppard, C. Caleman, A. G. MacPhee, D. Weinstein, and  others, "Atomic-Scale Visualization of Inertial Dynamics," Science 308, 392-395 (2005).
[CrossRef] [PubMed]

C. Blome, T. Tschentscher, J. Davaasambuu, P. Durand, and S. Techert, "Femtosecond time-resolved powder diffraction experiments using hard X-ray free-electron lasers," J. Sync. Rad. 11, 483-489 (2005).

N. Zhavoronkov, Y. Gritsai, M. Bargheer, M. Woerner, T. Elsaesser, F. Zamponi, I. Uschmann, and E. F¨orster, "Microfocus Cu K〈 source for femtosecond X-ray science," Opt. Lett. 30, 1737-1739 (2005).
[CrossRef] [PubMed]

2004 (2)

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]

S. Techert and K. A. Zachariasse, "Structure determination of the intramolecular charge transfer state in crystalline 4-(diisopropylamino) benzonitrile from picosecond X-ray diffraction," J. Am. Chem. Soc 126, 5593-5600 (2004).
[CrossRef] [PubMed]

2003 (1)

K. Sokolowski-Tinten, C. Blome, J. Blums, A. Cavalleri, C. Dietrich, A. Tarasevitch, I. Uschmann, E. F¨orster, 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 (2)

A. Rousse, C. Rischel, and J. C. Gauthier "Femtosecond X-ray crystallography," Rev. Mod. Phys. 73, 17-31 (2001).
[CrossRef]

S. Techert, F. Schotte, and M. Wulff, "Picosecond X-ray diffraction probed transient structural changes in organic solids," Phys. Rev. Lett. 86, 2030-2033 (2001).
[CrossRef] [PubMed]

1999 (1)

C. Rose-Petruck, R. Jiminez, T. Guo, A. Cavalleri, C. Siders, F. Raksi, J. A. Squier, B. C. Walker, K. R. Wilson, and C. P. J. Barty "Picosecond-milliangstrom lattice dynamics measured by ultrafast X-ray diffraction," Nature 398, 310-312 (1999).
[CrossRef]

1997 (1)

R. Brun and F. Rademakers, "ROOT-An object oriented data analysis framework," Nucl. Instrum. Methods A 389, 81-86 (1997).
[CrossRef]

1996 (1)

P. Gibbon and E. Forster, "Short-pulse laser-plasma interactions," Plasma Phys. Control. Fusion 38, 769-793 (1996).
[CrossRef]

1990 (1)

N. C. Woolsey, J. S. Wark, and D. Riley, "Sub-nanosecond X-ray powder diffraction," J. Appl. Cryst. 23, 441-443 (1990).
[CrossRef]

1989 (1)

S. Ahmed, A. M. Shamah, A. Ibrahim, and F. Hanna, "X-ray studies of the high temperature phase transition of ammonium sulphate crystals," Phys. Status Solidi(a) 115, K149-K153 (1989).
[CrossRef]

1988 (1)

C. G. Ryan, E. J. Clayton, W. L. Griffin, S. H. Sie, and D. R. Cousens, "SNIP, a statistics-sensitive background treatment for the quantitative analysis of PIXE spectra in geoscience applications," Nucl. Instrum. Methods B 34, 396-402 (1988).
[CrossRef]

1987 (1)

F. Brunel, "Not-so-resonant, resonant absorption," Phys. Rev. Lett. 59, 52-55 (1987).
[CrossRef] [PubMed]

1969 (1)

H. Rietveld, "A profile refinement method for nuclear and magnetic structures," J. Appl. Cryst. 2, 65-71 (1969).
[CrossRef]

1966 (1)

E. O. Schlemper and W. C. Hamilton, "Neutron-Diffraction Study of the Structures of Ferroelectric and Paraelectric Ammonium Sulfate," J. Chem. Phys. 44, 4498-4509 (1966).
[CrossRef]

1916 (1)

P. Debye and P. Scherrer, "Interferenzen an regellos orientierten Teilchen im Rontgenlicht," Phys. Z. 17, 277-283 (1916).

Ahmed, S.

S. Ahmed, A. M. Shamah, A. Ibrahim, and F. Hanna, "X-ray studies of the high temperature phase transition of ammonium sulphate crystals," Phys. Status Solidi(a) 115, K149-K153 (1989).
[CrossRef]

Ansari, Z.

F. Zamponi, Z. Ansari, C. v . Korff Schmising, P . Rothhardt, N . Zhavoronkov, M . Woerner, T . Elsaesser, M . Bargheer, T . Trobitzsch-Ryll, and M . Haschke, "Femtosecond hard X-ray plasma sources with a kilohertz repetition rate," Appl. Phys. A 96, 51-58 (2009).
[CrossRef]

Bargheer, M

F. Zamponi, Z. Ansari, C. v . Korff Schmising, P . Rothhardt, N . Zhavoronkov, M . Woerner, T . Elsaesser, M . Bargheer, T . Trobitzsch-Ryll, and M . Haschke, "Femtosecond hard X-ray plasma sources with a kilohertz repetition rate," Appl. Phys. A 96, 51-58 (2009).
[CrossRef]

M. Braun, C. v. Korff Schmising, M . Kiel, N . Zhavoronkov, J . Dreyer, M . Bargheer, T . Elsaesser, C . Root, T. E . Schrader, P. Gilch, W . Zinth, and M . Woerner, "Ultrafast changes of molecular crystal structure induced by dipole solvation," Phys. Rev. Lett. 98, 248301 (2007).
[CrossRef] [PubMed]

Bargheer, M.

N. Zhavoronkov, Y. Gritsai, M. Bargheer, M. Woerner, T. Elsaesser, F. Zamponi, I. Uschmann, and E. F¨orster, "Microfocus Cu K〈 source for femtosecond X-ray science," Opt. Lett. 30, 1737-1739 (2005).
[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]

Barty, C. P. J.

C. Rose-Petruck, R. Jiminez, T. Guo, A. Cavalleri, C. Siders, F. Raksi, J. A. Squier, B. C. Walker, K. R. Wilson, and C. P. J. Barty "Picosecond-milliangstrom lattice dynamics measured by ultrafast X-ray diffraction," Nature 398, 310-312 (1999).
[CrossRef]

Blome, C.

C. Blome, T. Tschentscher, J. Davaasambuu, P. Durand, and S. Techert, "Femtosecond time-resolved powder diffraction experiments using hard X-ray free-electron lasers," J. Sync. Rad. 11, 483-489 (2005).

A. M. Lindenberg, J. Larsson, K. Sokolowski-Tinten, K. J. Gaffney, C. Blome, O. Synnergren, J. Sheppard, C. Caleman, A. G. MacPhee, D. Weinstein, and  others, "Atomic-Scale Visualization of Inertial Dynamics," Science 308, 392-395 (2005).
[CrossRef] [PubMed]

K. Sokolowski-Tinten, C. Blome, J. Blums, A. Cavalleri, C. Dietrich, A. Tarasevitch, I. Uschmann, E. F¨orster, 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]

Blums, J.

K. Sokolowski-Tinten, C. Blome, J. Blums, A. Cavalleri, C. Dietrich, A. Tarasevitch, I. Uschmann, E. F¨orster, 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]

Braun, M.

M. Braun, C. v. Korff Schmising, M . Kiel, N . Zhavoronkov, J . Dreyer, M . Bargheer, T . Elsaesser, C . Root, T. E . Schrader, P. Gilch, W . Zinth, and M . Woerner, "Ultrafast changes of molecular crystal structure induced by dipole solvation," Phys. Rev. Lett. 98, 248301 (2007).
[CrossRef] [PubMed]

Brun, R.

R. Brun and F. Rademakers, "ROOT-An object oriented data analysis framework," Nucl. Instrum. Methods A 389, 81-86 (1997).
[CrossRef]

Brunel, F.

F. Brunel, "Not-so-resonant, resonant absorption," Phys. Rev. Lett. 59, 52-55 (1987).
[CrossRef] [PubMed]

Caleman, C.

A. M. Lindenberg, J. Larsson, K. Sokolowski-Tinten, K. J. Gaffney, C. Blome, O. Synnergren, J. Sheppard, C. Caleman, A. G. MacPhee, D. Weinstein, and  others, "Atomic-Scale Visualization of Inertial Dynamics," Science 308, 392-395 (2005).
[CrossRef] [PubMed]

Cavalleri, A.

K. Sokolowski-Tinten, C. Blome, J. Blums, A. Cavalleri, C. Dietrich, A. Tarasevitch, I. Uschmann, E. F¨orster, 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]

C. Rose-Petruck, R. Jiminez, T. Guo, A. Cavalleri, C. Siders, F. Raksi, J. A. Squier, B. C. Walker, K. R. Wilson, and C. P. J. Barty "Picosecond-milliangstrom lattice dynamics measured by ultrafast X-ray diffraction," Nature 398, 310-312 (1999).
[CrossRef]

Clayton, E. J.

C. G. Ryan, E. J. Clayton, W. L. Griffin, S. H. Sie, and D. R. Cousens, "SNIP, a statistics-sensitive background treatment for the quantitative analysis of PIXE spectra in geoscience applications," Nucl. Instrum. Methods B 34, 396-402 (1988).
[CrossRef]

Cousens, D. R.

C. G. Ryan, E. J. Clayton, W. L. Griffin, S. H. Sie, and D. R. Cousens, "SNIP, a statistics-sensitive background treatment for the quantitative analysis of PIXE spectra in geoscience applications," Nucl. Instrum. Methods B 34, 396-402 (1988).
[CrossRef]

Davaasambuu, J.

C. Blome, T. Tschentscher, J. Davaasambuu, P. Durand, and S. Techert, "Femtosecond time-resolved powder diffraction experiments using hard X-ray free-electron lasers," J. Sync. Rad. 11, 483-489 (2005).

Debye, P.

P. Debye and P. Scherrer, "Interferenzen an regellos orientierten Teilchen im Rontgenlicht," Phys. Z. 17, 277-283 (1916).

Dietrich, C.

K. Sokolowski-Tinten, C. Blome, J. Blums, A. Cavalleri, C. Dietrich, A. Tarasevitch, I. Uschmann, E. F¨orster, 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]

Dreyer, J

M. Braun, C. v. Korff Schmising, M . Kiel, N . Zhavoronkov, J . Dreyer, M . Bargheer, T . Elsaesser, C . Root, T. E . Schrader, P. Gilch, W . Zinth, and M . Woerner, "Ultrafast changes of molecular crystal structure induced by dipole solvation," Phys. Rev. Lett. 98, 248301 (2007).
[CrossRef] [PubMed]

Durand, P.

C. Blome, T. Tschentscher, J. Davaasambuu, P. Durand, and S. Techert, "Femtosecond time-resolved powder diffraction experiments using hard X-ray free-electron lasers," J. Sync. Rad. 11, 483-489 (2005).

Elsaesser, T

F. Zamponi, Z. Ansari, C. v . Korff Schmising, P . Rothhardt, N . Zhavoronkov, M . Woerner, T . Elsaesser, M . Bargheer, T . Trobitzsch-Ryll, and M . Haschke, "Femtosecond hard X-ray plasma sources with a kilohertz repetition rate," Appl. Phys. A 96, 51-58 (2009).
[CrossRef]

M. Braun, C. v. Korff Schmising, M . Kiel, N . Zhavoronkov, J . Dreyer, M . Bargheer, T . Elsaesser, C . Root, T. E . Schrader, P. Gilch, W . Zinth, and M . Woerner, "Ultrafast changes of molecular crystal structure induced by dipole solvation," Phys. Rev. Lett. 98, 248301 (2007).
[CrossRef] [PubMed]

Elsaesser, T.

N. Zhavoronkov, Y. Gritsai, M. Bargheer, M. Woerner, T. Elsaesser, F. Zamponi, I. Uschmann, and E. F¨orster, "Microfocus Cu K〈 source for femtosecond X-ray science," Opt. Lett. 30, 1737-1739 (2005).
[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]

F¨orster, E.

N. Zhavoronkov, Y. Gritsai, M. Bargheer, M. Woerner, T. Elsaesser, F. Zamponi, I. Uschmann, and E. F¨orster, "Microfocus Cu K〈 source for femtosecond X-ray science," Opt. Lett. 30, 1737-1739 (2005).
[CrossRef] [PubMed]

K. Sokolowski-Tinten, C. Blome, J. Blums, A. Cavalleri, C. Dietrich, A. Tarasevitch, I. Uschmann, E. F¨orster, 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]

Forster, E.

P. Gibbon and E. Forster, "Short-pulse laser-plasma interactions," Plasma Phys. Control. Fusion 38, 769-793 (1996).
[CrossRef]

Gaffney, K. J.

A. M. Lindenberg, J. Larsson, K. Sokolowski-Tinten, K. J. Gaffney, C. Blome, O. Synnergren, J. Sheppard, C. Caleman, A. G. MacPhee, D. Weinstein, and  others, "Atomic-Scale Visualization of Inertial Dynamics," Science 308, 392-395 (2005).
[CrossRef] [PubMed]

Gauthier, J. C.

A. Rousse, C. Rischel, and J. C. Gauthier "Femtosecond X-ray crystallography," Rev. Mod. Phys. 73, 17-31 (2001).
[CrossRef]

Gibbon, P.

P. Gibbon and E. Forster, "Short-pulse laser-plasma interactions," Plasma Phys. Control. Fusion 38, 769-793 (1996).
[CrossRef]

Gilch, P

M. Braun, C. v. Korff Schmising, M . Kiel, N . Zhavoronkov, J . Dreyer, M . Bargheer, T . Elsaesser, C . Root, T. E . Schrader, P. Gilch, W . Zinth, and M . Woerner, "Ultrafast changes of molecular crystal structure induced by dipole solvation," Phys. Rev. Lett. 98, 248301 (2007).
[CrossRef] [PubMed]

Griffin, W. L.

C. G. Ryan, E. J. Clayton, W. L. Griffin, S. H. Sie, and D. R. Cousens, "SNIP, a statistics-sensitive background treatment for the quantitative analysis of PIXE spectra in geoscience applications," Nucl. Instrum. Methods B 34, 396-402 (1988).
[CrossRef]

Gritsai, Y.

N. Zhavoronkov, Y. Gritsai, M. Bargheer, M. Woerner, T. Elsaesser, F. Zamponi, I. Uschmann, and E. F¨orster, "Microfocus Cu K〈 source for femtosecond X-ray science," Opt. Lett. 30, 1737-1739 (2005).
[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]

Guo, T.

C. Rose-Petruck, R. Jiminez, T. Guo, A. Cavalleri, C. Siders, F. Raksi, J. A. Squier, B. C. Walker, K. R. Wilson, and C. P. J. Barty "Picosecond-milliangstrom lattice dynamics measured by ultrafast X-ray diffraction," Nature 398, 310-312 (1999).
[CrossRef]

Hamilton, W. C.

E. O. Schlemper and W. C. Hamilton, "Neutron-Diffraction Study of the Structures of Ferroelectric and Paraelectric Ammonium Sulfate," J. Chem. Phys. 44, 4498-4509 (1966).
[CrossRef]

Hanna, F.

S. Ahmed, A. M. Shamah, A. Ibrahim, and F. Hanna, "X-ray studies of the high temperature phase transition of ammonium sulphate crystals," Phys. Status Solidi(a) 115, K149-K153 (1989).
[CrossRef]

Haschke, M

F. Zamponi, Z. Ansari, C. v . Korff Schmising, P . Rothhardt, N . Zhavoronkov, M . Woerner, T . Elsaesser, M . Bargheer, T . Trobitzsch-Ryll, and M . Haschke, "Femtosecond hard X-ray plasma sources with a kilohertz repetition rate," Appl. Phys. A 96, 51-58 (2009).
[CrossRef]

Horn-von-Hoegen, M.

K. Sokolowski-Tinten, C. Blome, J. Blums, A. Cavalleri, C. Dietrich, A. Tarasevitch, I. Uschmann, E. F¨orster, 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]

Ibrahim, A.

S. Ahmed, A. M. Shamah, A. Ibrahim, and F. Hanna, "X-ray studies of the high temperature phase transition of ammonium sulphate crystals," Phys. Status Solidi(a) 115, K149-K153 (1989).
[CrossRef]

Jiminez, R.

C. Rose-Petruck, R. Jiminez, T. Guo, A. Cavalleri, C. Siders, F. Raksi, J. A. Squier, B. C. Walker, K. R. Wilson, and C. P. J. Barty "Picosecond-milliangstrom lattice dynamics measured by ultrafast X-ray diffraction," Nature 398, 310-312 (1999).
[CrossRef]

Kammler, M.

K. Sokolowski-Tinten, C. Blome, J. Blums, A. Cavalleri, C. Dietrich, A. Tarasevitch, I. Uschmann, E. F¨orster, 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]

Kiel, M

M. Braun, C. v. Korff Schmising, M . Kiel, N . Zhavoronkov, J . Dreyer, M . Bargheer, T . Elsaesser, C . Root, T. E . Schrader, P. Gilch, W . Zinth, and M . Woerner, "Ultrafast changes of molecular crystal structure induced by dipole solvation," Phys. Rev. Lett. 98, 248301 (2007).
[CrossRef] [PubMed]

Kim, D. S.

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]

Korff Schmising, C. v

F. Zamponi, Z. Ansari, C. v . Korff Schmising, P . Rothhardt, N . Zhavoronkov, M . Woerner, T . Elsaesser, M . Bargheer, T . Trobitzsch-Ryll, and M . Haschke, "Femtosecond hard X-ray plasma sources with a kilohertz repetition rate," Appl. Phys. A 96, 51-58 (2009).
[CrossRef]

Korff Schmising, C. v.

M. Braun, C. v. Korff Schmising, M . Kiel, N . Zhavoronkov, J . Dreyer, M . Bargheer, T . Elsaesser, C . Root, T. E . Schrader, P. Gilch, W . Zinth, and M . Woerner, "Ultrafast changes of molecular crystal structure induced by dipole solvation," Phys. Rev. Lett. 98, 248301 (2007).
[CrossRef] [PubMed]

Larsson, J.

A. M. Lindenberg, J. Larsson, K. Sokolowski-Tinten, K. J. Gaffney, C. Blome, O. Synnergren, J. Sheppard, C. Caleman, A. G. MacPhee, D. Weinstein, and  others, "Atomic-Scale Visualization of Inertial Dynamics," Science 308, 392-395 (2005).
[CrossRef] [PubMed]

Lindenberg, A. M.

A. M. Lindenberg, J. Larsson, K. Sokolowski-Tinten, K. J. Gaffney, C. Blome, O. Synnergren, J. Sheppard, C. Caleman, A. G. MacPhee, D. Weinstein, and  others, "Atomic-Scale Visualization of Inertial Dynamics," Science 308, 392-395 (2005).
[CrossRef] [PubMed]

MacPhee, A. G.

A. M. Lindenberg, J. Larsson, K. Sokolowski-Tinten, K. J. Gaffney, C. Blome, O. Synnergren, J. Sheppard, C. Caleman, A. G. MacPhee, D. Weinstein, and  others, "Atomic-Scale Visualization of Inertial Dynamics," Science 308, 392-395 (2005).
[CrossRef] [PubMed]

Rademakers, F.

R. Brun and F. Rademakers, "ROOT-An object oriented data analysis framework," Nucl. Instrum. Methods A 389, 81-86 (1997).
[CrossRef]

Raksi, F.

C. Rose-Petruck, R. Jiminez, T. Guo, A. Cavalleri, C. Siders, F. Raksi, J. A. Squier, B. C. Walker, K. R. Wilson, and C. P. J. Barty "Picosecond-milliangstrom lattice dynamics measured by ultrafast X-ray diffraction," Nature 398, 310-312 (1999).
[CrossRef]

Rietveld, H.

H. Rietveld, "A profile refinement method for nuclear and magnetic structures," J. Appl. Cryst. 2, 65-71 (1969).
[CrossRef]

Riley, D.

N. C. Woolsey, J. S. Wark, and D. Riley, "Sub-nanosecond X-ray powder diffraction," J. Appl. Cryst. 23, 441-443 (1990).
[CrossRef]

Rischel, C.

A. Rousse, C. Rischel, and J. C. Gauthier "Femtosecond X-ray crystallography," Rev. Mod. Phys. 73, 17-31 (2001).
[CrossRef]

Root, C

M. Braun, C. v. Korff Schmising, M . Kiel, N . Zhavoronkov, J . Dreyer, M . Bargheer, T . Elsaesser, C . Root, T. E . Schrader, P. Gilch, W . Zinth, and M . Woerner, "Ultrafast changes of molecular crystal structure induced by dipole solvation," Phys. Rev. Lett. 98, 248301 (2007).
[CrossRef] [PubMed]

Rose-Petruck, C.

C. Rose-Petruck, R. Jiminez, T. Guo, A. Cavalleri, C. Siders, F. Raksi, J. A. Squier, B. C. Walker, K. R. Wilson, and C. P. J. Barty "Picosecond-milliangstrom lattice dynamics measured by ultrafast X-ray diffraction," Nature 398, 310-312 (1999).
[CrossRef]

Rothhardt, P

F. Zamponi, Z. Ansari, C. v . Korff Schmising, P . Rothhardt, N . Zhavoronkov, M . Woerner, T . Elsaesser, M . Bargheer, T . Trobitzsch-Ryll, and M . Haschke, "Femtosecond hard X-ray plasma sources with a kilohertz repetition rate," Appl. Phys. A 96, 51-58 (2009).
[CrossRef]

Rousse, A.

A. Rousse, C. Rischel, and J. C. Gauthier "Femtosecond X-ray crystallography," Rev. Mod. Phys. 73, 17-31 (2001).
[CrossRef]

Ryan, C. G.

C. G. Ryan, E. J. Clayton, W. L. Griffin, S. H. Sie, and D. R. Cousens, "SNIP, a statistics-sensitive background treatment for the quantitative analysis of PIXE spectra in geoscience applications," Nucl. Instrum. Methods B 34, 396-402 (1988).
[CrossRef]

Scherrer, P.

P. Debye and P. Scherrer, "Interferenzen an regellos orientierten Teilchen im Rontgenlicht," Phys. Z. 17, 277-283 (1916).

Schlemper, E. O.

E. O. Schlemper and W. C. Hamilton, "Neutron-Diffraction Study of the Structures of Ferroelectric and Paraelectric Ammonium Sulfate," J. Chem. Phys. 44, 4498-4509 (1966).
[CrossRef]

Schotte, F.

S. Techert, F. Schotte, and M. Wulff, "Picosecond X-ray diffraction probed transient structural changes in organic solids," Phys. Rev. Lett. 86, 2030-2033 (2001).
[CrossRef] [PubMed]

Schrader, T. E

M. Braun, C. v. Korff Schmising, M . Kiel, N . Zhavoronkov, J . Dreyer, M . Bargheer, T . Elsaesser, C . Root, T. E . Schrader, P. Gilch, W . Zinth, and M . Woerner, "Ultrafast changes of molecular crystal structure induced by dipole solvation," Phys. Rev. Lett. 98, 248301 (2007).
[CrossRef] [PubMed]

Shamah, A. M.

S. Ahmed, A. M. Shamah, A. Ibrahim, and F. Hanna, "X-ray studies of the high temperature phase transition of ammonium sulphate crystals," Phys. Status Solidi(a) 115, K149-K153 (1989).
[CrossRef]

Sheppard, J.

A. M. Lindenberg, J. Larsson, K. Sokolowski-Tinten, K. J. Gaffney, C. Blome, O. Synnergren, J. Sheppard, C. Caleman, A. G. MacPhee, D. Weinstein, and  others, "Atomic-Scale Visualization of Inertial Dynamics," Science 308, 392-395 (2005).
[CrossRef] [PubMed]

Siders, C.

C. Rose-Petruck, R. Jiminez, T. Guo, A. Cavalleri, C. Siders, F. Raksi, J. A. Squier, B. C. Walker, K. R. Wilson, and C. P. J. Barty "Picosecond-milliangstrom lattice dynamics measured by ultrafast X-ray diffraction," Nature 398, 310-312 (1999).
[CrossRef]

Sie, S. H.

C. G. Ryan, E. J. Clayton, W. L. Griffin, S. H. Sie, and D. R. Cousens, "SNIP, a statistics-sensitive background treatment for the quantitative analysis of PIXE spectra in geoscience applications," Nucl. Instrum. Methods B 34, 396-402 (1988).
[CrossRef]

Sokolowski-Tinten, K.

A. M. Lindenberg, J. Larsson, K. Sokolowski-Tinten, K. J. Gaffney, C. Blome, O. Synnergren, J. Sheppard, C. Caleman, A. G. MacPhee, D. Weinstein, and  others, "Atomic-Scale Visualization of Inertial Dynamics," Science 308, 392-395 (2005).
[CrossRef] [PubMed]

K. Sokolowski-Tinten, C. Blome, J. Blums, A. Cavalleri, C. Dietrich, A. Tarasevitch, I. Uschmann, E. F¨orster, 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]

Squier, J. A.

C. Rose-Petruck, R. Jiminez, T. Guo, A. Cavalleri, C. Siders, F. Raksi, J. A. Squier, B. C. Walker, K. R. Wilson, and C. P. J. Barty "Picosecond-milliangstrom lattice dynamics measured by ultrafast X-ray diffraction," Nature 398, 310-312 (1999).
[CrossRef]

Synnergren, O.

A. M. Lindenberg, J. Larsson, K. Sokolowski-Tinten, K. J. Gaffney, C. Blome, O. Synnergren, J. Sheppard, C. Caleman, A. G. MacPhee, D. Weinstein, and  others, "Atomic-Scale Visualization of Inertial Dynamics," Science 308, 392-395 (2005).
[CrossRef] [PubMed]

Tarasevitch, A.

K. Sokolowski-Tinten, C. Blome, J. Blums, A. Cavalleri, C. Dietrich, A. Tarasevitch, I. Uschmann, E. F¨orster, 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]

Techert, S.

C. Blome, T. Tschentscher, J. Davaasambuu, P. Durand, and S. Techert, "Femtosecond time-resolved powder diffraction experiments using hard X-ray free-electron lasers," J. Sync. Rad. 11, 483-489 (2005).

S. Techert and K. A. Zachariasse, "Structure determination of the intramolecular charge transfer state in crystalline 4-(diisopropylamino) benzonitrile from picosecond X-ray diffraction," J. Am. Chem. Soc 126, 5593-5600 (2004).
[CrossRef] [PubMed]

S. Techert, F. Schotte, and M. Wulff, "Picosecond X-ray diffraction probed transient structural changes in organic solids," Phys. Rev. Lett. 86, 2030-2033 (2001).
[CrossRef] [PubMed]

Trobitzsch-Ryll, T

F. Zamponi, Z. Ansari, C. v . Korff Schmising, P . Rothhardt, N . Zhavoronkov, M . Woerner, T . Elsaesser, M . Bargheer, T . Trobitzsch-Ryll, and M . Haschke, "Femtosecond hard X-ray plasma sources with a kilohertz repetition rate," Appl. Phys. A 96, 51-58 (2009).
[CrossRef]

Tschentscher, T.

C. Blome, T. Tschentscher, J. Davaasambuu, P. Durand, and S. Techert, "Femtosecond time-resolved powder diffraction experiments using hard X-ray free-electron lasers," J. Sync. Rad. 11, 483-489 (2005).

Uschmann, I.

N. Zhavoronkov, Y. Gritsai, M. Bargheer, M. Woerner, T. Elsaesser, F. Zamponi, I. Uschmann, and E. F¨orster, "Microfocus Cu K〈 source for femtosecond X-ray science," Opt. Lett. 30, 1737-1739 (2005).
[CrossRef] [PubMed]

K. Sokolowski-Tinten, C. Blome, J. Blums, A. Cavalleri, C. Dietrich, A. Tarasevitch, I. Uschmann, E. F¨orster, 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]

von der Linde, D.

K. Sokolowski-Tinten, C. Blome, J. Blums, A. Cavalleri, C. Dietrich, A. Tarasevitch, I. Uschmann, E. F¨orster, 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]

Walker, B. C.

C. Rose-Petruck, R. Jiminez, T. Guo, A. Cavalleri, C. Siders, F. Raksi, J. A. Squier, B. C. Walker, K. R. Wilson, and C. P. J. Barty "Picosecond-milliangstrom lattice dynamics measured by ultrafast X-ray diffraction," Nature 398, 310-312 (1999).
[CrossRef]

Wark, J. S.

N. C. Woolsey, J. S. Wark, and D. Riley, "Sub-nanosecond X-ray powder diffraction," J. Appl. Cryst. 23, 441-443 (1990).
[CrossRef]

Weinstein, D.

A. M. Lindenberg, J. Larsson, K. Sokolowski-Tinten, K. J. Gaffney, C. Blome, O. Synnergren, J. Sheppard, C. Caleman, A. G. MacPhee, D. Weinstein, and  others, "Atomic-Scale Visualization of Inertial Dynamics," Science 308, 392-395 (2005).
[CrossRef] [PubMed]

Wilson, K. R.

C. Rose-Petruck, R. Jiminez, T. Guo, A. Cavalleri, C. Siders, F. Raksi, J. A. Squier, B. C. Walker, K. R. Wilson, and C. P. J. Barty "Picosecond-milliangstrom lattice dynamics measured by ultrafast X-ray diffraction," Nature 398, 310-312 (1999).
[CrossRef]

Woerner, M

F. Zamponi, Z. Ansari, C. v . Korff Schmising, P . Rothhardt, N . Zhavoronkov, M . Woerner, T . Elsaesser, M . Bargheer, T . Trobitzsch-Ryll, and M . Haschke, "Femtosecond hard X-ray plasma sources with a kilohertz repetition rate," Appl. Phys. A 96, 51-58 (2009).
[CrossRef]

M. Braun, C. v. Korff Schmising, M . Kiel, N . Zhavoronkov, J . Dreyer, M . Bargheer, T . Elsaesser, C . Root, T. E . Schrader, P. Gilch, W . Zinth, and M . Woerner, "Ultrafast changes of molecular crystal structure induced by dipole solvation," Phys. Rev. Lett. 98, 248301 (2007).
[CrossRef] [PubMed]

Woerner, M.

N. Zhavoronkov, Y. Gritsai, M. Bargheer, M. Woerner, T. Elsaesser, F. Zamponi, I. Uschmann, and E. F¨orster, "Microfocus Cu K〈 source for femtosecond X-ray science," Opt. Lett. 30, 1737-1739 (2005).
[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]

Woo, J. C.

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]

Woolsey, N. C.

N. C. Woolsey, J. S. Wark, and D. Riley, "Sub-nanosecond X-ray powder diffraction," J. Appl. Cryst. 23, 441-443 (1990).
[CrossRef]

Wulff, M.

S. Techert, F. Schotte, and M. Wulff, "Picosecond X-ray diffraction probed transient structural changes in organic solids," Phys. Rev. Lett. 86, 2030-2033 (2001).
[CrossRef] [PubMed]

Zachariasse, K. A.

S. Techert and K. A. Zachariasse, "Structure determination of the intramolecular charge transfer state in crystalline 4-(diisopropylamino) benzonitrile from picosecond X-ray diffraction," J. Am. Chem. Soc 126, 5593-5600 (2004).
[CrossRef] [PubMed]

Zamponi, F.

F. Zamponi, Z. Ansari, C. v . Korff Schmising, P . Rothhardt, N . Zhavoronkov, M . Woerner, T . Elsaesser, M . Bargheer, T . Trobitzsch-Ryll, and M . Haschke, "Femtosecond hard X-ray plasma sources with a kilohertz repetition rate," Appl. Phys. A 96, 51-58 (2009).
[CrossRef]

N. Zhavoronkov, Y. Gritsai, M. Bargheer, M. Woerner, T. Elsaesser, F. Zamponi, I. Uschmann, and E. F¨orster, "Microfocus Cu K〈 source for femtosecond X-ray science," Opt. Lett. 30, 1737-1739 (2005).
[CrossRef] [PubMed]

Zhavoronkov, N

F. Zamponi, Z. Ansari, C. v . Korff Schmising, P . Rothhardt, N . Zhavoronkov, M . Woerner, T . Elsaesser, M . Bargheer, T . Trobitzsch-Ryll, and M . Haschke, "Femtosecond hard X-ray plasma sources with a kilohertz repetition rate," Appl. Phys. A 96, 51-58 (2009).
[CrossRef]

M. Braun, C. v. Korff Schmising, M . Kiel, N . Zhavoronkov, J . Dreyer, M . Bargheer, T . Elsaesser, C . Root, T. E . Schrader, P. Gilch, W . Zinth, and M . Woerner, "Ultrafast changes of molecular crystal structure induced by dipole solvation," Phys. Rev. Lett. 98, 248301 (2007).
[CrossRef] [PubMed]

Zhavoronkov, N.

N. Zhavoronkov, Y. Gritsai, M. Bargheer, M. Woerner, T. Elsaesser, F. Zamponi, I. Uschmann, and E. F¨orster, "Microfocus Cu K〈 source for femtosecond X-ray science," Opt. Lett. 30, 1737-1739 (2005).
[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]

Zinth, W

M. Braun, C. v. Korff Schmising, M . Kiel, N . Zhavoronkov, J . Dreyer, M . Bargheer, T . Elsaesser, C . Root, T. E . Schrader, P. Gilch, W . Zinth, and M . Woerner, "Ultrafast changes of molecular crystal structure induced by dipole solvation," Phys. Rev. Lett. 98, 248301 (2007).
[CrossRef] [PubMed]

Appl. Phys. A (1)

F. Zamponi, Z. Ansari, C. v . Korff Schmising, P . Rothhardt, N . Zhavoronkov, M . Woerner, T . Elsaesser, M . Bargheer, T . Trobitzsch-Ryll, and M . Haschke, "Femtosecond hard X-ray plasma sources with a kilohertz repetition rate," Appl. Phys. A 96, 51-58 (2009).
[CrossRef]

J. Am. Chem. Soc (1)

S. Techert and K. A. Zachariasse, "Structure determination of the intramolecular charge transfer state in crystalline 4-(diisopropylamino) benzonitrile from picosecond X-ray diffraction," J. Am. Chem. Soc 126, 5593-5600 (2004).
[CrossRef] [PubMed]

J. Appl. Cryst. (2)

N. C. Woolsey, J. S. Wark, and D. Riley, "Sub-nanosecond X-ray powder diffraction," J. Appl. Cryst. 23, 441-443 (1990).
[CrossRef]

H. Rietveld, "A profile refinement method for nuclear and magnetic structures," J. Appl. Cryst. 2, 65-71 (1969).
[CrossRef]

J. Chem. Phys. (1)

E. O. Schlemper and W. C. Hamilton, "Neutron-Diffraction Study of the Structures of Ferroelectric and Paraelectric Ammonium Sulfate," J. Chem. Phys. 44, 4498-4509 (1966).
[CrossRef]

J. Sync. Rad. (1)

C. Blome, T. Tschentscher, J. Davaasambuu, P. Durand, and S. Techert, "Femtosecond time-resolved powder diffraction experiments using hard X-ray free-electron lasers," J. Sync. Rad. 11, 483-489 (2005).

Nature (2)

C. Rose-Petruck, R. Jiminez, T. Guo, A. Cavalleri, C. Siders, F. Raksi, J. A. Squier, B. C. Walker, K. R. Wilson, and C. P. J. Barty "Picosecond-milliangstrom lattice dynamics measured by ultrafast X-ray diffraction," Nature 398, 310-312 (1999).
[CrossRef]

K. Sokolowski-Tinten, C. Blome, J. Blums, A. Cavalleri, C. Dietrich, A. Tarasevitch, I. Uschmann, E. F¨orster, 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]

Nucl. Instrum. Methods A (1)

R. Brun and F. Rademakers, "ROOT-An object oriented data analysis framework," Nucl. Instrum. Methods A 389, 81-86 (1997).
[CrossRef]

Nucl. Instrum. Methods B (1)

C. G. Ryan, E. J. Clayton, W. L. Griffin, S. H. Sie, and D. R. Cousens, "SNIP, a statistics-sensitive background treatment for the quantitative analysis of PIXE spectra in geoscience applications," Nucl. Instrum. Methods B 34, 396-402 (1988).
[CrossRef]

Opt. Lett. (1)

Phys. Rev. Lett. (3)

S. Techert, F. Schotte, and M. Wulff, "Picosecond X-ray diffraction probed transient structural changes in organic solids," Phys. Rev. Lett. 86, 2030-2033 (2001).
[CrossRef] [PubMed]

M. Braun, C. v. Korff Schmising, M . Kiel, N . Zhavoronkov, J . Dreyer, M . Bargheer, T . Elsaesser, C . Root, T. E . Schrader, P. Gilch, W . Zinth, and M . Woerner, "Ultrafast changes of molecular crystal structure induced by dipole solvation," Phys. Rev. Lett. 98, 248301 (2007).
[CrossRef] [PubMed]

F. Brunel, "Not-so-resonant, resonant absorption," Phys. Rev. Lett. 59, 52-55 (1987).
[CrossRef] [PubMed]

Phys. Status Solidi (1)

S. Ahmed, A. M. Shamah, A. Ibrahim, and F. Hanna, "X-ray studies of the high temperature phase transition of ammonium sulphate crystals," Phys. Status Solidi(a) 115, K149-K153 (1989).
[CrossRef]

Phys. Z. (1)

P. Debye and P. Scherrer, "Interferenzen an regellos orientierten Teilchen im Rontgenlicht," Phys. Z. 17, 277-283 (1916).

Plasma Phys. Control. Fusion (1)

P. Gibbon and E. Forster, "Short-pulse laser-plasma interactions," Plasma Phys. Control. Fusion 38, 769-793 (1996).
[CrossRef]

Rev. Mod. Phys. (1)

A. Rousse, C. Rischel, and J. C. Gauthier "Femtosecond X-ray crystallography," Rev. Mod. Phys. 73, 17-31 (2001).
[CrossRef]

Science (2)

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]

A. M. Lindenberg, J. Larsson, K. Sokolowski-Tinten, K. J. Gaffney, C. Blome, O. Synnergren, J. Sheppard, C. Caleman, A. G. MacPhee, D. Weinstein, and  others, "Atomic-Scale Visualization of Inertial Dynamics," Science 308, 392-395 (2005).
[CrossRef] [PubMed]

Other (1)

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

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Figures (9)

Fig. 1.
Fig. 1.

Upper panel: sketch of the Debye-Scherrer method. Lower panel: possible laser-induced crystal changes, adapted from [1]. The black and the red dots mimic two different kinds of atoms in a crystal. The lower plots show how the powder pattern would look like for two arbitrary reflections. (a) unperturbed crystal. (b) expansion (contraction) due, e.g., to an increase (decrease) of the temperature; the peaks shift correspondingly. (c) propagation of acoustical phonon, compression followed by expansion; the peaks get broader. (d) optical-phonon-like excitation of the crystal; only the ratio of the peak intensity is changed. This process can be very fast in low-Z materials.

Fig. 2.
Fig. 2.

(a) Schematic of the experimental set-up for femtosecond powder diffraction. Explanation in the main text. (b) Sample geometry used in the femtosecond experiments. (c) Debye-Scherrer diffraction pattern from an ammonium sulfate powder sample recorded with a large-area CCD detector. The exposure time was 420 s.

Fig. 3.
Fig. 3.

Powder pattern in the measured angular range. Black solid line: measured powder pattern with 420 s exposure time. Blue dashed line: calculated powder pattern based on measurements reported in [17]. Red dotted line: synthetic spectrum used to optimize the parameters needed in the 2D-1D data reduction; note that only the exact positions are needed, not the relative intensities as discussed in the text.

Fig. 4.
Fig. 4.

In (a) the different contributions to the measured line broadening are sketched. The whole X-ray probe beam can be thought of as composed of many beamlets, each with the divergence of the full beam. Each incoming beamlet (in red) along the path through the powder is diffracted at different depths. Both the divergence of the incoming beam and the finite extension of the probe beam on the sample contributes to the measured line broadening. In (b) the line broadening is modeled by taking into account the probed volume and the X-ray beam divergence. The solid black line is the line width from the unpumped sample as calculated for a sample thickness of 250 μm. The data points are the measured line widths of (200) and (212) reflections. The red dashed line is the line width as calculated by considering a sample thickness of 25 μm, to be compared with the measured line width of time-resolved changes of (200) at t = 50 fs.

Fig. 5.
Fig. 5.

Time-resolved signal. (a) 2θ-delay scan. The diffracted X-ray intensity is plotted as a function of the diffraction angle 2θ and the pump-probe delay. (b) Intensity changes (time cut along the red line in plot a) normalized to the intensity of the strongest diffracted peak before excitation, 〈I(θ 111, -∞)〉. Inset: Intensity change around time delay zero. The numerical fit gives a cross-correlation width of about 120 fs.

Fig. 6.
Fig. 6.

(a) Measured intensity changes at time t = +50 fs, corresponding to the vertical lineout of Fig. 5a (blue line). (b) Static structure factor values calculated from [17]. (c) Difference between static and transient structure factor values. Note that the magnitude of ΔF is strongly influenced by the multiplicity.

Fig. 7.
Fig. 7.

2D projection of the electron density in AS. (a) Unit cell of AS. The shaded plane is parallel to the z-axis, goes through (0.5 a, 0.5 b, 0.5 c) and is tilted by 60° with respect to the x-axis. (b) Electron density as calculated from [17] for this plane. (c) electron density map of the changes Δρ(x,y,z,t) = ρ(x,y,z,t) - ρ(x,y,z, - ∞) are shown at time t = +50 fs.

Fig. 8.
Fig. 8.

Δρ(x,y,z,t) for the same plane depicted in Fig. 7a is given for different time delays. This plane is parallel to the z-axis and includes the line connecting the hydrogen atoms of opposite NH+ 4 groups, marked with a dashed circle.

Tables (1)

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Table 1. Femtosecond X-ray plasma source

Equations (7)

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P scatt = I 0 r e 2 V λ 3 M ( hkl ) F hkl 2 4 v a 2 ( 1 + cos 2 ( 2 θ ) 2 sin θ ) ,
Δ I ( θ hkl , t ) I ( θ 111 , ) = I ( θ hkl , t ) I ( θ hkl , ) I ( θ 111 , ) ,
Δ I ( θ hkl , t ) I ( θ 111 , ) = η F hkl ex + ( 1 η ) F hkl gr 2 F hkl gr 2 I ( θ 111 , ) C .
η Δ F hkl = η ( F hkl ex F hkl gr ) Δ I ( θ hkl , t ) 2 C F hkl gr .
η Δ ρ ( x , y , z , t ) = η abc hkl Δ F hkl ( t ) exp ( i ϕ hkl ) cos [ 2 π ( hx a + ky b + lz c ) ]
V CT η Δ ρ ( x , y , z , t ) dxdydz = N e ,
Q = i = 0 N P synth ( θ i ) In ( P meas ( θ i ) ) ,

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