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@ARTICLE{Rudenko:323844,
author = {Rudenko, A. and Inhester, L. and Hanasaki, K. and Li, X.
and Robatjazi, S. J. and Erk, B. and Boll, R. and Toyota, K.
and Hao, Y. and Vendrell, O. and Bomme, C. and Savelyev, E.
and Rudek, B. and Foucar, L. and Southworth, S. H. and
Lehmann, C. S. and Kraessig, B. and Marchenko, T. and Simon,
M. and Ueda, K. and Ferguson, K. R. and Bucher, M. and
Gorkhover, T. and Carron, S. and Alonso-Mori, R. and Koglin,
J. E. and Correa, J. and Williams, G. J. and Boutet, S. and
Young, L. and Bostedt, C. and Son, S.-K. and Santra, R. and
Rolles, D.},
title = {{F}emtosecond response of polyatomic molecules to
ultra-intense hard {X}-rays},
journal = {Nature},
volume = {546},
number = {7656},
issn = {1476-4687},
address = {London [u.a.]},
publisher = {Macmillan},
reportid = {PUBDB-2017-04151},
pages = {129 - 132},
year = {2017},
note = {© Macmillan Publishers Limited, part of Springer Nature ;
Post referee fulltext in progress; Embargo 6 months from
publication},
abstract = {X-ray free-electron lasers enable the investigation of the
structure and dynamics of diverse systems, including atoms,
molecules, nanocrystals and single bioparticles, under
extreme conditions1, 2, 3, 4, 5, 6, 7. Many imaging
applications that target biological systems and complex
materials use hard X-ray pulses with extremely high peak
intensities (exceeding 1020 watts per square centimetre)3,
5. However, fundamental investigations have focused mainly
on the individual response of atoms and small molecules
using soft X-rays with much lower intensities8, 9, 10, 11,
12, 13, 14, 15, 16, 17. Studies with intense X-ray pulses
have shown that irradiated atoms reach a very high degree of
ionization, owing to multiphoton absorption8, 12, 13, 18,
which in a heteronuclear molecular system occurs
predominantly locally on a heavy atom (provided that the
absorption cross-section of the heavy atom is considerably
larger than those of its neighbours) and is followed by
efficient redistribution of the induced charge14, 15, 16,
17, 19, 20. In serial femtosecond crystallography of
biological objects—an application of X-ray free-electron
lasers that greatly enhances our ability to determine
protein structure2, 3—the ionization of heavy atoms
increases the local radiation damage that is seen in the
diffraction patterns of these objects21, 22 and has been
suggested as a way of phasing the diffraction data23, 24. On
the basis of experiments using either soft or less-intense
hard X-rays14, 15, 16, 17, 18, 19, 25, it is thought that
the induced charge and associated radiation damage of atoms
in polyatomic molecules can be inferred from the charge that
is induced in an isolated atom under otherwise comparable
irradiation conditions. Here we show that the femtosecond
response of small polyatomic molecules that contain one
heavy atom to ultra-intense (with intensities approaching
1020 watts per square centimetre), hard (with photon
energies of 8.3 kiloelectronvolts) X-ray pulses is
qualitatively different: our experimental and modelling
results establish that, under these conditions, the
ionization of a molecule is considerably enhanced compared
to that of an individual heavy atom with the same absorption
cross-section. This enhancement is driven by ultrafast
charge transfer within the molecule, which refills the core
holes that are created in the heavy atom, providing further
targets for inner-shell ionization and resulting in the
emission of more than 50 electrons during the X-ray pulse.
Our results demonstrate that efficient modelling of
X-ray-driven processes in complex systems at ultrahigh
intensities is feasible.},
cin = {FS-SCS / FS-FLASH-O / FS-CFEL-3 / CFEL-DESYT / MPG /
CFEL-DRD},
ddc = {070},
cid = {I:(DE-H253)FS-SCS-20131031 / I:(DE-H253)FS-FLASH-O-20160930
/ I:(DE-H253)FS-CFEL-3-20120731 /
I:(DE-H253)CFEL-DESYT-20160930 / I:(DE-H253)MPG-20120806 /
I:(DE-H253)CFEL-DRD-20160910},
pnm = {6211 - Extreme States of Matter: From Cold Ions to Hot
Plasmas (POF3-621)},
pid = {G:(DE-HGF)POF3-6211},
experiment = {EXP:(DE-MLZ)NOSPEC-20140101},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000402372800041},
pubmed = {pmid:28569799},
doi = {10.1038/nature22373},
url = {https://bib-pubdb1.desy.de/record/323844},
}