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Title: Sub-nanometer-scale measurements of the interaction of ultrafast soft x-ray free-electron-laser pulses with matter

Abstract

Femtosecond pulses from soft-x-ray free-electron lasers (FELs) [1] are ideal for directly probing matter at atomic length scales and timescales of atomic motion. An important component of understanding ultrafast phenomena of light-matter interactions is concerned with the onset of atomic motion which is impeded by the atoms inertia. This delay of structural changes will enable atomic-resolution flash-imaging [2-3] to be performed at upcoming x-ray FELs [4-5] with pulses intense enough to record the x-ray scattering from single molecules [6]. We explored this ultrafast high-intensity regime with the FLASH soft-x-ray FEL [7-8] by measuring the reflectance of nanostructured multilayer mirrors using pulses with fluences far in excess of the mirrors damage threshold. Even though the nanostructures were ultimately completely destroyed, we found that they maintained their integrity and reflectance characteristics during the 25-fs-long pulse, with no evidence for any structural changes during that time over lengths greater than 3 {angstrom}. In the recently built FLASH FEL [7], x-rays are produced from short electron pulses oscillating in a periodic magnet array, called an undulator, by the principle of self-amplification of spontaneous emission [9-10]. The laser quality of the x-ray pulses can be quantified by the peak spectral brilliance of the source, whichmore » is 10{sup 28} photons/(s mm2 mrad2 0.1% bandwidth) [8]; this is up to seven orders of magnitude higher than modern third-generation synchrotron sources. For our studies, the machine operated with pulses of 25 fs duration at a wavelength of 32.5 nm and energies up to 21 {micro}J. We focused these pulses to 3 x 10{sup 14} W/cm{sup 2} onto our nanostructured samples, resulting in an the unprecedented heating rate of 5 x 10{sup 18} K/s, while probing the irradiated structures at the nanometer length scale. The x-ray reflectivity of periodic nanometer-scale multilayers [11] is very sensitive to changes in the atomic positions and the refractive indices of the constituent materials, making them an ideal choice to study structural changes induced by ultrashort FEL pulses. The large multilayer reflectivity results from the cooperative interaction of the x-ray field with many layers of precisely fabricated thicknesses, each less than the x-ray wavelength. This Bragg or resonant reflection from the periodic structure is easily disrupted by any imperfection of the layers. The characteristics of the structure, such as periodicity or layer intermixing, can be precisely determined from the measurement of the Bragg reflectivity as a function of incidence angle. These parameters can be easily measured to a small fraction of the probe wavelength, as is well known in x-ray crystallography where average atomic positions of minerals or proteins are found to less than 0.01{angstrom}. Thus, we can explore ultrafast phenomena at length scales less than the wavelength, and investigate the conditions to overcome the effects of radiation damage by using ultrafast pulses.« less

Authors:
; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
907850
Report Number(s):
UCRL-JRNL-223562
Journal ID: ISSN 0031-9007; PRLTAO; TRN: US0703333
DOE Contract Number:  
W-7405-ENG-48
Resource Type:
Journal Article
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 98; Journal ID: ISSN 0031-9007
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUMM MECHANICS, GENERAL PHYSICS; 36 MATERIALS SCIENCE; 42 ENGINEERING; ATOMS; CRYSTALLOGRAPHY; DEFECTS; ELECTRONS; HEATING RATE; INCIDENCE ANGLE; LASERS; MAGNETS; MIRRORS; NANOSTRUCTURES; PERIODICITY; PROBES; PROTEINS; RADIATIONS; REFLECTION; REFLECTIVITY; SCATTERING; SYNCHROTRONS; WAVELENGTHS

Citation Formats

Hau-Riege, S, Chapman, H, Krzywinski, J, Sobierajski, R, London, R, Bionta, R, Bergh, M, Caleman, C, Nietubyc, R, Juha, L, Kuba, J, Bajt, S, Spiller, E, Baker, S, Kjornrattanawanich, B, Gullikson, E, Tschentscher, T, Plonjes, E, and Toleikis, S. Sub-nanometer-scale measurements of the interaction of ultrafast soft x-ray free-electron-laser pulses with matter. United States: N. p., 2006. Web.
Hau-Riege, S, Chapman, H, Krzywinski, J, Sobierajski, R, London, R, Bionta, R, Bergh, M, Caleman, C, Nietubyc, R, Juha, L, Kuba, J, Bajt, S, Spiller, E, Baker, S, Kjornrattanawanich, B, Gullikson, E, Tschentscher, T, Plonjes, E, & Toleikis, S. Sub-nanometer-scale measurements of the interaction of ultrafast soft x-ray free-electron-laser pulses with matter. United States.
Hau-Riege, S, Chapman, H, Krzywinski, J, Sobierajski, R, London, R, Bionta, R, Bergh, M, Caleman, C, Nietubyc, R, Juha, L, Kuba, J, Bajt, S, Spiller, E, Baker, S, Kjornrattanawanich, B, Gullikson, E, Tschentscher, T, Plonjes, E, and Toleikis, S. Wed . "Sub-nanometer-scale measurements of the interaction of ultrafast soft x-ray free-electron-laser pulses with matter". United States. https://www.osti.gov/servlets/purl/907850.
@article{osti_907850,
title = {Sub-nanometer-scale measurements of the interaction of ultrafast soft x-ray free-electron-laser pulses with matter},
author = {Hau-Riege, S and Chapman, H and Krzywinski, J and Sobierajski, R and London, R and Bionta, R and Bergh, M and Caleman, C and Nietubyc, R and Juha, L and Kuba, J and Bajt, S and Spiller, E and Baker, S and Kjornrattanawanich, B and Gullikson, E and Tschentscher, T and Plonjes, E and Toleikis, S},
abstractNote = {Femtosecond pulses from soft-x-ray free-electron lasers (FELs) [1] are ideal for directly probing matter at atomic length scales and timescales of atomic motion. An important component of understanding ultrafast phenomena of light-matter interactions is concerned with the onset of atomic motion which is impeded by the atoms inertia. This delay of structural changes will enable atomic-resolution flash-imaging [2-3] to be performed at upcoming x-ray FELs [4-5] with pulses intense enough to record the x-ray scattering from single molecules [6]. We explored this ultrafast high-intensity regime with the FLASH soft-x-ray FEL [7-8] by measuring the reflectance of nanostructured multilayer mirrors using pulses with fluences far in excess of the mirrors damage threshold. Even though the nanostructures were ultimately completely destroyed, we found that they maintained their integrity and reflectance characteristics during the 25-fs-long pulse, with no evidence for any structural changes during that time over lengths greater than 3 {angstrom}. In the recently built FLASH FEL [7], x-rays are produced from short electron pulses oscillating in a periodic magnet array, called an undulator, by the principle of self-amplification of spontaneous emission [9-10]. The laser quality of the x-ray pulses can be quantified by the peak spectral brilliance of the source, which is 10{sup 28} photons/(s mm2 mrad2 0.1% bandwidth) [8]; this is up to seven orders of magnitude higher than modern third-generation synchrotron sources. For our studies, the machine operated with pulses of 25 fs duration at a wavelength of 32.5 nm and energies up to 21 {micro}J. We focused these pulses to 3 x 10{sup 14} W/cm{sup 2} onto our nanostructured samples, resulting in an the unprecedented heating rate of 5 x 10{sup 18} K/s, while probing the irradiated structures at the nanometer length scale. The x-ray reflectivity of periodic nanometer-scale multilayers [11] is very sensitive to changes in the atomic positions and the refractive indices of the constituent materials, making them an ideal choice to study structural changes induced by ultrashort FEL pulses. The large multilayer reflectivity results from the cooperative interaction of the x-ray field with many layers of precisely fabricated thicknesses, each less than the x-ray wavelength. This Bragg or resonant reflection from the periodic structure is easily disrupted by any imperfection of the layers. The characteristics of the structure, such as periodicity or layer intermixing, can be precisely determined from the measurement of the Bragg reflectivity as a function of incidence angle. These parameters can be easily measured to a small fraction of the probe wavelength, as is well known in x-ray crystallography where average atomic positions of minerals or proteins are found to less than 0.01{angstrom}. Thus, we can explore ultrafast phenomena at length scales less than the wavelength, and investigate the conditions to overcome the effects of radiation damage by using ultrafast pulses.},
doi = {},
url = {https://www.osti.gov/biblio/907850}, journal = {Physical Review Letters},
issn = {0031-9007},
number = ,
volume = 98,
place = {United States},
year = {2006},
month = {8}
}