Abstract
An era of exploring the interactions of high-intensity, hard X-rays with matter has begun with the start-up of a hard-X-ray free-electron laser, the Linac Coherent Light Source (LCLS). Understanding how electrons in matter respond to ultra-intense X-ray radiation is essential for all applications. Here we reveal the nature of the electronic response in a free atom to unprecedented high-intensity, short-wavelength, high-fluence radiation (respectively 1018 W cm−2, 1.5–0.6 nm, ∼105 X-ray photons per Å2). At this fluence, the neon target inevitably changes during the course of a single femtosecond-duration X-ray pulse—by sequentially ejecting electrons—to produce fully-stripped neon through absorption of six photons. Rapid photoejection of inner-shell electrons produces ‘hollow’ atoms and an intensity-induced X-ray transparency. Such transparency, due to the presence of inner-shell vacancies, can be induced in all atomic, molecular and condensed matter systems at high intensity. Quantitative comparison with theory allows us to extract LCLS fluence and pulse duration. Our successful modelling of X-ray/atom interactions using a straightforward rate equation approach augurs favourably for extension to complex systems.
This is a preview of subscription content, access via your institution
Access options
Subscribe to this journal
Receive 51 print issues and online access
$199.00 per year
only $3.90 per issue
Buy this article
- Purchase on Springer Link
- Instant access to full article PDF
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
References
Emma, P. First lasing of the LCLS X-ray FEL at 1.5 Å. In Proc. 2009 Particle Accelerator Conf. (IEEE, in the press).
Neutze, R., Wouts, R., van der Spoel, D., Weckert, E. & Hajdu, J. Potential for biomolecular imaging with femtosecond X-ray pulses. Nature 406, 752–757 (2000)
Nagler, B. et al. Turning solid aluminium transparent by intense soft X-ray photoionization. Nature Phys. 5, 693–696 (2009)
Lee, R. W. et al. Finite temperature dense matter studies on next-generation light sources. J. Opt. Soc. Am. B 20, 770–778 (2003)
Gaffney, K. J. & Chapman, H. N. Imaging atomic structure and dynamics with ultrafast X-ray scattering. Science 316, 1444–1448 (2007)
Stephenson, G. B., Robert, A. & Grubel, G. Revealing the atomic dance. Nature Mater. 8, 702–703 (2009)
Ostermeier, C. & Michel, H. Crystallization of membrane proteins. Curr. Opin. Struct. Biol. 7, 697–701 (1997)
Henderson, R. The potential and limitation of neutrons, electrons and X-rays for atomic resolution microscopy of unstained biological molecules. Q. Rev. Biophys. 28, 171–193 (1995)
Chapman, H. N. et al. Femtosecond diffractive imaging with a soft-X-ray free-electron laser. Nature Phys. 2, 839–843 (2006)
Hau-Riege, S. P. X-ray atomic scattering factors of low-Z ions with a core hole. Phys. Rev. A 76, 042511 (2007)
Veigele, W. J. Photon cross sections from 0.1 keV to 1 MeV for elements Z = 1 to Z = 94. At. Data Tables 5, 51–111 (1973)
Rohringer, N. & Santra, R. X-ray nonlinear optical processes using a self-amplified spontaneous emission free-electron laser. Phys. Rev. A 76, 033416 (2007)
Augst, S., Strickland, D., Meyerhofer, D. D., Chin, S. L. & Eberly, J. H. Tunneling ionization of noble gases in a high-intensity laser field. Phys. Rev. Lett. 63, 2212–2215 (1989)
Palaniyappan, S. et al. Ultrastrong field ionization of Nen+ (n ≤ 8): rescattering and the role of the magnetic field. Phys. Rev. Lett. 94, 243003 (2005)
Ackermann, W. et al. Operation of a free-electron laser from the extreme ultraviolet to the water window. Nature Photon. 1, 336–342 (2007)
Sorokin, A. A. et al. Photoelectric effect at ultrahigh intensities. Phys. Rev. Lett. 99, 213002 (2007)
Makris, M. G., Lambropoulos, P. & Mihelic, A. Theory of multiphoton multielectron ionization of xenon under strong 93-eV radiation. Phys. Rev. Lett. 102, 033002 (2009)
Richter, M. et al. Extreme ultraviolet laser excites atomic giant resonance. Phys. Rev. Lett. 102, 163002 (2009)
Bostedt, C. et al. Multistep ionization of argon clusters in intense femtosecond extreme ultraviolet pulses. Phys. Rev. Lett. 100, 133401 (2008)
Wabnitz, H. et al. Multiple ionization of atom clusters by intense soft X-rays from a free-electron laser. Nature 420, 482–485 (2002)
Ziaja, B., Wabnitz, H., Wang, F., Weckert, E. & Möller, T. Energetics, ionization, and expansion dynamics of atomic clusters irradiated with short intense vacuum-ultraviolet pulses. Phys. Rev. Lett. 102, 205002 (2009)
Hau-Riege, S. P., Bionta, R. M., Ryutov, D. D. & Drzywinski, J. Measurement of x-ray free-electron-laser pulse energies by photoluminescence in nitrogen gas. J. Appl. Phys. 103, 053306 (2008)
Richter, M., Bobashev, S. V., Sorokin, A. A. & Tiedtke, K. Photon-matter interaction at short wavelengths and ultra-high intensity — gas-phase experiments at FLASH. J. Phys. Conf. Ser. 141, 012014 (2008)
Chalupsky, J. et al. Characteristics of focused soft X-ray free-electron laser beam determined by ablation of organic molecular solids. Opt. Express 15, 6036–6043 (2007)
Krause, M. O., Vestal, M. L., Johnson, W. H. & Carlson, T. A. Readjustment of the neon atom ionized in the K shell by X rays. Phys. Rev. 133, A385–A390 (1964)
Amusia, M., Ya, Lee, I. S. & Kilin, V. A. Double Auger decay in atoms: probability and angular distribution. Phys. Rev. A 45, 4576–4587 (1992)
Saito, N. & Suzuki, I. H. Multiple photoionization of Ne in the K-shell ionization region. Phys. Scr. 45, 253–256 (1992)
Barty, A. et al. Predicting the coherent X-ray wavefront focal properties at the Linac Coherent Light Source (LCLS) X-ray free electron laser. Opt. Express 17, 15508–15519 (2009)
Novikov, S. A. & Hopersky, A. N. Two-photon excitation/ionization of atomic inner shells. J. Phys. At. Mol. Opt. Phys. 33, 2287–2294 (2000)
Bane, K. L. F. et al. Measurements and modeling of coherent synchrotron radiation and its impact on the Linac Coherent Light Source electron beam. Phys. Rev. Spec. Top. Accel. Beams 12, 030704 (2009)
Milonni, P. & Eberly, J. H. Lasers (Wiley & Sons, 1988)
Krause, M. O. Atomic radiative and radiationless yields for K and L shells. J. Phys. Chem. Ref. Data 8, 307–327 (1979)
Bhalla, C. P., Folland, N. O. & Hein, M. A. Theoretical K-shell Auger rates, transition energies, and fluorescence yields for multiply ionized neon. Phys. Rev. A 8, 649–657 (1973)
Reiche, S., Musumeci, P., Pellegrini, C. & Rosenzweig, J. B. Development of ultra-short pulse, single coherent spike for SASE X-ray FELs. Nucl. Instrum. Methods A 593, 45–48 (2008)
Emma, P. et al. Femtosecond and subfemtosecond X-ray pulses from a self-amplified spontaneous-emission-based free electron laser. Phys. Rev. Lett. 92, 074801 (2004)
Southworth, S. H. et al. Double K-shell photoionization of neon. Phys. Rev. A 67, 062712 (2003)
Albiez, A., Thoma, M., Weber, W. & Mehlhorn, W. KL23 ionization in neon by electron impact in the range 1.5–50 keV: cross sections and alignment. Z. Phys. D 16, 97–106 (1990)
Kanngießer, B. et al. Simultaneous determination of radiative and nonradiative decay channels in the neon K shell. Phys. Rev. A 62, 014702 (2000)
Chen, M. H. Auger transition rates and fluorescence yields for the double-K-hole state. Phys. Rev. A 44, 239–242 (1991)
Ayvazyan, V. et al. First operation of a free-electron laser generating GW power radiation at 32 nm wavelength. Eur. Phys. J. D 37, 297–303 (2006)
Sorokin, A. A. et al. Method based on atomic photoionization for spot-size measurement on focused soft x-ray free electron laser beams. Appl. Phys. Lett. 89, 221114 (2006)
Krainov, V. P. Inverse stimulated bremsstrahlung of slow electrons under Coulomb scattering. J. Phys. At. Mol. Opt. Phys. 33, 1585–1595 (2000)
Föhlisch, A. et al. Direct observation of electron dynamics in the attosecond domain. Nature 436, 373–376 (2005)
Hoener, M. et al. Phys. Rev. Lett. Ultra-intense X-ray induced ionization, dissociation and frustrated absorption in molecular nitrogen. (submitted)
Ding, Y. et al. Measurements and simulations of ultralow emittance and ultrashort electron beams in the Linac coherent light source. Phys. Rev. Lett. 102, 254801 (2009)
Frisch, J. et al. in Proc. BIW08 paper MOIOTIO02, 17–26 (2008) 〈http://accelconf.web.cern.ch/AccelConf/BIW2008/papers/moiotio02.pdf〉
Bozek, J. D. AMO instrumentation for the LCLS X-ray FEL. Eur. Phys. J. Spec. Top. 169, 129–132 (2009)
Paul, H. & Schinner, A. Empirical stopping power tables for ions from 3Li to 18Ar and from 0.001 to 1000 MeV/nucleon in solids and gases. At. Data Nucl. Data Tables 85, 377–452 (2003)
Manson, S. T. & Cooper, J. W. Photo-ionization in the soft x-ray range: Z dependence in a central-potential model. Phys. Rev. 165, 126–138 (1968)
McNeil, B. First light from hard X-ray laser. Nature Photon. 3, 375–377 (2009)
Bonifacio, R., De Salvo, L., Pierini, P., Piovella, N. & Pellegrini, C. Spectrum, temporal structure, and fluctuations in a high-gain free-electron laser starting from noise. Phys. Rev. Lett. 73, 70–73 (1994)
Kelez, N. et al. in Proc. FEL2009 paper WEPC20 546–549 (2009); 〈http://accelconf.web.cern.ch/AccelConf/FEL2009/papers/wepc20.pdf〉.
Kondratenko, A. M. & Saldin, E. L. Generation of coherent radiation by a relativistic-electron beam in an undulator. Sov. Phys. Dokl. 24, 986–988 (1979)
Bonifacio, R., Pellegrini, C. & Narducci, L. M. Collective instabilities and high-gain regime in a free electron laser. Opt. Commun. 50, 373–378 (1984)
Saldin, E. L., Schneidmiller, E. A. & Yurkov, M. V. Statistical properties of radiation from VUV and X-ray free electron laser. Opt. Commun. 148, 383–403 (1998)
Saldin, E. L., Schneidmiller, E. A. & Yurkov, M. V. The Physics of Free Electron Lasers (Springer, 2000)
Wuilleumier, F. & Krause, M. O. Photoionization of neon between 100 and 2000 eV: single and multiple processes, angular distributions, and subshell cross sections. Phys. Rev. A 10, 242–258 (1974).
Acknowledgements
We thank P. Emma, Z. Huang, R. Iverson, F. J. Decker, J. Frisch, and J. Turner for discussions that allowed us to realize, and subsequently utilize, the flexibility of the LCLS to maximum benefit. We are indebted to the operations staff for the performance of the LCLS in the many modes and energies that we requested throughout the course of this experiment. We thank the software engineers for producing advanced control, data acquisition and analysis capabilities during the experiment. This work was supported by the Chemical Sciences, Geosciences, and Biosciences Division of the Office of Basic Energy Sciences, Office of Science, US Department of Energy (DE-AC02-06CH11357, DE-FG02-04ER15614, DE-FG02-92ER14299). N.R. was supported by the US Department of Energy by Lawrence Livermore National Laboratory (DE-AC52-07NA27344). M.H. thanks the Alexander von Humboldt Foundation for a Feodor Lynen fellowship. P.H.B., J.P.C., S.G., J.M.G. and D.A.R. were supported through the PULSE Institute, which is jointly funded by the Department of Energy, Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division and Division of Materials Science and Engineering. Portions of this research were carried out at the LCLS at the SLAC National Accelerator Laboratory. LCLS is funded by the US Department of Energy’s Office of Basic Energy Sciences.
Author information
Authors and Affiliations
Contributions
L.Y., R.S., S.H.S., E.P.K. and B.K. conceived the experimental plan, acquired and analysed the data, and wrote the paper. R.S. and N.R. performed the theoretical calculations. J.D.B. and C.B. designed, commissioned and operated the AMO instrument. M.M. assisted during the experiment with upstream X-ray diagnostics. Y.L., A.M.M., S.T.P., L.F.D., G.D., C.A.R., N.B., L.F., M.H., P.H.B., J.P.C., S.G., J.M.G. and D.A.R. contributed to the experiment. All authors contributed to the work presented here and to the final paper.
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing financial interests.
Rights and permissions
About this article
Cite this article
Young, L., Kanter, E., Krässig, B. et al. Femtosecond electronic response of atoms to ultra-intense X-rays. Nature 466, 56–61 (2010). https://doi.org/10.1038/nature09177
Received:
Accepted:
Issue Date:
DOI: https://doi.org/10.1038/nature09177
This article is cited by
-
Transient responses of double core-holes generation in all-attosecond pump-probe spectroscopy
Scientific Reports (2024)
-
Shepherd electron effects in multiple ionization of rubidium by circularly polarized intense laser fields
Communications Physics (2023)
-
Multiple-core-hole resonance spectroscopy with ultraintense X-ray pulses
Nature Communications (2023)
-
Artificial intelligence for online characterization of ultrashort X-ray free-electron laser pulses
Scientific Reports (2022)
Comments
By submitting a comment you agree to abide by our Terms and Community Guidelines. If you find something abusive or that does not comply with our terms or guidelines please flag it as inappropriate.