Femtosecond electronic response of atoms to ultra-intense X-rays

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.

[1]  M. Richter,et al.  Photon-matter interaction at short wavelengths and ultra-high intensity - Gas-phase experiments at FLASH , 2008 .

[2]  C. Bhalla,et al.  Theoretical K-Shell Auger Rates, Transition Energies, and Fluorescence Yields for Multiply Ionized Neon , 1973 .

[3]  W. Weber,et al.  KL2,3 ionization in neon by electron impact in the range 1.5–50 keV: cross sections and alignment , 1990 .

[4]  C. Bostedt,et al.  Multistep ionization of argon clusters in intense femtosecond extreme ultraviolet pulses. , 2008, Physical review letters.

[5]  H. Wabnitz,et al.  Multiple ionization of atom clusters by intense soft X-rays from a free-electron laser , 2002, Nature.

[6]  Mau H. Chen,et al.  Double K-shell photoionization of neon , 2003 .

[7]  M. Richter,et al.  Photoelectric effect at ultrahigh intensities. , 2007, Physical review letters.

[8]  P. Nicolosi,et al.  First operation of a free-electron laser generating GW power radiation at 32 nm wavelength , 2006 .

[9]  J. Cooper,et al.  Photo-Ionization in the Soft x-Ray Range: 1 Z Dependence in a Central-Potential Model , 1968 .

[10]  P Emma,et al.  Measurements and simulations of ultralow emittance and ultrashort electron beams in the linac coherent light source. , 2009, Physical review letters.

[11]  R. Santra,et al.  X-ray nonlinear optical processes using a self-amplified spontaneous emission free-electron laser , 2007 .

[12]  D. Meyerhofer,et al.  Tunneling ionization of noble gases in a high-intensity laser field. , 1989, Physical review letters.

[13]  R. London,et al.  Characteristics of focused soft X-ray free-electron laser beam determined by ablation of organic molecular solids. , 2007, Optics express.

[14]  Pellegrini,et al.  Spectrum, temporal structure, and fluctuations in a high-gain free-electron laser starting from noise. , 1994, Physical review letters.

[15]  J. Hajdu,et al.  Potential for biomolecular imaging with femtosecond X-ray pulses , 2000, Nature.

[16]  A. Falkowski,et al.  Multielectron ionization of Ne/sup +n/ in ultrastrong laser fields: rescattering and the role of the magnetic field , 2005, 2005 Quantum Electronics and Laser Science Conference.

[17]  E. Chowdhury,et al.  Ultrastrong Field Ionization of Ne{sup n+} (n{<=}8): Rescattering and the Role of the Magnetic Field , 2005 .

[18]  O. Landen,et al.  Finite temperature dense matter studies on next-generation light sources , 2003 .

[19]  Lee,et al.  Double Auger decay in atoms: Probability and angular distribution. , 1992, Physical review. A, Atomic, molecular, and optical physics.

[20]  Claudio Pellegrini,et al.  Collective instabilities and high-gain regime in a free electron laser , 1984 .

[21]  Mikhail Yurkov,et al.  Statistical properties of radiation from VUV and X-ray free electron laser , 1998 .

[22]  R. Henderson The potential and limitations of neutrons, electrons and X-rays for atomic resolution microscopy of unstained biological molecules , 1995, Quarterly Reviews of Biophysics.

[23]  Anton Barty,et al.  Predicting the coherent X-ray wavefront focal properties at the Linac Coherent Light Source (LCLS) X-ray free electron laser. , 2009, Optics express.

[24]  Chen,et al.  Auger transition rates and fluorescence yields for the double-K-hole state. , 1991, Physical review. A, Atomic, molecular, and optical physics.

[25]  M. Martins,et al.  Extreme ultraviolet laser excites atomic giant resonance. , 2009, Physical review letters.

[26]  M. Krause,et al.  Atomic radiative and radiationless yields for K and L shells , 1979 .

[27]  P. Feulner,et al.  Direct observation of electron dynamics in the attosecond domain , 2005, Nature.

[28]  D Rolles,et al.  Ultraintense x-ray induced ionization, dissociation, and frustrated absorption in molecular nitrogen. , 2010, Physical review letters.

[29]  M G Makris,et al.  Theory of multiphoton multielectron ionization of xenon under strong 93-eV radiation. , 2009, Physical review letters.

[30]  P Emma,et al.  Femtosecond and subfemtosecond x-ray pulses from a self-amplified spontaneous-emission-based free-electron laser. , 2004, Physical review letters.

[31]  F. Wuilleumier,et al.  Photoionization of neon between 100 and 2000 eV: Single and multiple processes, angular distributions, and subshell cross sections , 1974 .

[32]  W. Veigele,et al.  Photon cross sections from 0.1 keV to 1 MeV for elements Z = 1 to Z = 94* , 1973 .

[33]  N. Saito,et al.  Multiple photoionization of Ne in the K-shell ionization region , 1992 .

[34]  E. Weckert,et al.  Energetics, ionization, and expansion dynamics of atomic clusters irradiated with short intense vacuum-ultraviolet pulses. , 2008, Physical review letters.

[35]  H. N. Chapman,et al.  Imaging Atomic Structure and Dynamics with Ultrafast X-ray Scattering , 2007, Science.

[36]  B. McNeil,et al.  Free electron lasers: First light from hard X-ray laser , 2009 .

[37]  H. Chapman,et al.  Turning solid aluminium transparent by intense soft X-ray photoionization , 2009 .

[38]  Gerhard Grübel,et al.  X-ray spectroscopy: Revealing the atomic dance. , 2009, Nature materials.

[39]  J. Bozek AMO instrumentation for the LCLS X-ray FEL , 2009 .

[40]  S. Novikov,et al.  Two-photon excitation/ionization of atomic inner shells , 2000 .

[41]  M. Yurkov,et al.  The Physics of Free Electron Lasers , 1999 .

[42]  B. Kanngießer,et al.  Simultaneous determination of radiative and nonradiative decay channels in the neon K shell , 2000 .

[43]  E. Saldin,et al.  Generation of coherent radiation by a relativistic-electron beam in an undulator , 1979 .

[44]  Ryszard S. Romaniuk,et al.  Operation of a free-electron laser from the extreme ultraviolet to the water window , 2007 .

[45]  Sven Reiche,et al.  Development of ultra-short pulse, single coherent spike for SASE X-ray FELs , 2008 .

[46]  Stefan P. Hau-Riege,et al.  X-ray atomic scattering factors of low- Z ions with a core hole , 2007 .

[47]  C. Limborg-Deprey,et al.  Measurements and modeling of coherent synchrotron radiation and its impact on the Linac Coherent Light Source electron beam , 2009 .

[48]  P. Emma First Lasing of the LCLS X-Ray FEL at 1.5 Å , 2010 .

[49]  Andreas Schinner,et al.  Empirical stopping power tables for ions from 3Li to 18Ar and from 0.001 to 1000 MeV/nucleon in solids and gases , 2003 .

[50]  H. Michel,et al.  Crystallization of membrane proteins. , 1983, Current opinion in structural biology.

[51]  V. Krainov Inverse stimulated bremsstrahlung of slow electrons under Coulomb scattering , 2000 .

[52]  W. H. Benner,et al.  Femtosecond diffractive imaging with a soft-X-ray free-electron laser , 2006, physics/0610044.

[53]  Jacek Krzywinski,et al.  Measurement of x-ray free-electron-laser pulse energies by photoluminescence in nitrogen gas , 2008 .

[54]  E. Plönjes,et al.  Method based on atomic photoionization for spot-size measurement on focused soft x-ray free-electron laser beams , 2006 .

[55]  M. Vestal,et al.  Readjustment of the Neon Atom Ionized in the K Shell by X Rays , 1964 .