Near- and Extended-Edge X-Ray-Absorption Fine-Structure Spectroscopy Using Ultrafast Coherent High-Order Harmonic Supercontinua.

Recent advances in high-order harmonic generation have made it possible to use a tabletop-scale setup to produce spatially and temporally coherent beams of light with bandwidth spanning 12 octaves, from the ultraviolet up to x-ray photon energies >1.6  keV. Here we demonstrate the use of this light for x-ray-absorption spectroscopy at the K- and L-absorption edges of solids at photon energies near 1 keV. We also report x-ray-absorption spectroscopy in the water window spectral region (284-543 eV) using a high flux high-order harmonic generation x-ray supercontinuum with 10^{9}  photons/s in 1% bandwidth, 3 orders of magnitude larger than has previously been possible using tabletop sources. Since this x-ray radiation emerges as a single attosecond-to-femtosecond pulse with peak brightness exceeding 10^{26}  photons/s/mrad^{2}/mm^{2}/1% bandwidth, these novel coherent x-ray sources are ideal for probing the fastest molecular and materials processes on femtosecond-to-attosecond time scales and picometer length scales.

[1]  J. Biegert,et al.  High-flux table-top soft x-ray source driven by sub-2-cycle, CEP stable, 1.85-μm 1-kHz pulses for carbon K-edge spectroscopy. , 2014, Optics letters.

[2]  J. Seres,et al.  X-ray absorption spectroscopy in the keV range with laser generated high harmonic radiation , 2006 .

[3]  Tenio Popmintchev,et al.  90 GW peak power few-cycle mid-infrared pulses from an optical parametric amplifier. , 2011, Optics letters.

[4]  Abdul Quamar,et al.  ATHENA++ , 2020 .

[5]  P. Eisenberger,et al.  Extended x-ray absorption fine structure—its strengths and limitations as a structural tool , 1981 .

[6]  Tsuyoshi Murata,et al.  {m , 1934, ACML.

[7]  H. van Brug,et al.  A polychromator for (S)EXAFS using a laser generated plasma as soft X-ray source , 1985 .

[8]  Stephen R. Leone,et al.  Femtosecond x-ray spectroscopy of an electrocyclic ring-opening reaction , 2017, Science.

[9]  M Newville,et al.  ATHENA, ARTEMIS, HEPHAESTUS: data analysis for X-ray absorption spectroscopy using IFEFFIT. , 2005, Journal of synchrotron radiation.

[11]  S. Leone,et al.  Efficient table-top dual-wavelength beamline for ultrafast transient absorption spectroscopy in the soft X-ray region , 2019, Scientific Reports.

[12]  Justin M. Shaw,et al.  Probing the timescale of the exchange interaction in a ferromagnetic alloy , 2012, Proceedings of the National Academy of Sciences.

[13]  Justin M. Shaw,et al.  Ultrafast Demagnetization Measurements Using Extreme Ultraviolet Light: Comparison of Electronic and Magnetic Contributions , 2012 .

[14]  C. Spielmann,et al.  Time resolved spectroscopy with femtosecond soft-x-ray pulses , 2009 .

[15]  I. Christov,et al.  Phase matching of high harmonic generation in the soft and hard X-ray regions of the spectrum , 2009, Proceedings of the National Academy of Sciences.

[16]  Bradley K. Alpert,et al.  Ultrafast Time-Resolved Hard X-Ray Emission Spectroscopy on a Tabletop , 2016 .

[17]  M. Murnane,et al.  Distinguishing attosecond electron–electron scattering and screening in transition metals , 2017, Proceedings of the National Academy of Sciences.

[18]  I. Robinson,et al.  Focus on X-ray Beams with High Coherence , 2010 .

[19]  E. Takahashi,et al.  Coherent water window x ray by phase-matched high-order harmonic generation in neutral media. , 2008, Physical review letters.

[20]  Martin Aeschlimann,et al.  Ultrafast demagnetization dynamics at the M edges of magnetic elements observed using a tabletop high-harmonic soft x-ray source. , 2009, Physical review letters.

[21]  M. Murnane,et al.  The attosecond nonlinear optics of bright coherent X-ray generation , 2010 .

[22]  P. Argoul,et al.  Continuous Cauchy wavelet transform of XAFS spectra , 2005 .

[23]  Tenio Popmintchev,et al.  Extended phase matching of high harmonics driven by mid-infrared light. , 2008, Optics letters.

[24]  Jean-Pierre Wolf,et al.  Time-resolved x-ray absorption spectroscopy with a water window high-harmonic source , 2017, Science.

[25]  M. Murnane,et al.  Phase-matched generation of coherent soft X-rays , 1998, Science.

[26]  M. Murnane,et al.  Generation of bright isolated attosecond soft X-ray pulses driven by multicycle midinfrared lasers , 2014, Proceedings of the National Academy of Sciences.

[27]  M. Murnane,et al.  Bright Coherent Ultrahigh Harmonics in the keV X-ray Regime from Mid-Infrared Femtosecond Lasers , 2012, Science.

[28]  Edward A. Stern,et al.  New Technique for Investigating Noncrystalline Structures: Fourier Analysis of the Extended X-Ray—Absorption Fine Structure , 1971 .

[29]  Ronggui Yang,et al.  Quasi-ballistic thermal transport from nanoscale interfaces observed using ultrafast coherent soft X-ray beams. , 2010, Nature materials.

[30]  M. Murnane,et al.  Ultrafast magnetization enhancement in metallic multilayers driven by superdiffusive spin current , 2012, Nature Communications.

[31]  P. Corkum,et al.  Symmetry of molecular Rydberg states revealed by XUV transient absorption spectroscopy , 2019, Nature Communications.

[32]  M. Murnane,et al.  High flux coherent supercontinuum soft X-ray source driven by a single-stage 10 mJ, kHz, Ti:sapphire laser amplifier , 2014, 2014 Conference on Lasers and Electro-Optics (CLEO) - Laser Science to Photonic Applications.

[33]  J. Biegert,et al.  0.5-keV Soft X-ray attosecond continua , 2016, Nature Communications.

[34]  D. Popmintchev Quantum and Extreme Nonlinear Optics Design of Coherent Ultrafast X-ray Light and Applications , 2016 .

[35]  Dmitri A. Romanov,et al.  Ultraviolet surprise: Efficient soft x-ray high-harmonic generation in multiply ionized plasmas , 2015, Science.

[36]  Allan S. Johnson,et al.  Attosecond soft X-ray high harmonic generation , 2019, Philosophical Transactions of the Royal Society A.

[37]  Weilun Chao,et al.  A new regime of nanoscale thermal transport: Collective diffusion increases dissipation efficiency , 2014, Proceedings of the National Academy of Sciences.

[38]  W. Marsden I and J , 2012 .

[39]  M M Murnane,et al.  Bright, coherent, ultrafast soft X-ray harmonics spanning the water window from a tabletop light source. , 2010, Physical review letters.

[40]  Jinghua Guo,et al.  Structural and electronic properties of low dielectric constant fluorinated amorphous carbon films , 1998 .

[41]  N. Ishii,et al.  Laser-based soft x-ray light source resolving x-ray absorption near edge structure at the carbon K edge , 2015, 2015 Conference on Lasers and Electro-Optics (CLEO).

[42]  Manos Mavrikakis,et al.  Direct time-domain observation of attosecond final-state lifetimes in photoemission from solids , 2016, Science.

[43]  M. Key,et al.  Spectroscopy of Laser-Produced Plasmas , 1980 .

[44]  Yu Zhang,et al.  Understanding laser beam brightness: A review and new prospective in material processing , 2015 .

[45]  Emrah Turgut,et al.  Controlling the competition between optically induced ultrafast spin-flip scattering and spin transport in magnetic multilayers. , 2013, Physical review letters.