Coherent High Harmonics’ X-ray Supercontinua Enable Ultra-Precise Measurements of structure and dynamics on a Tabletop.

Dimitar Popmintchev, Benjamin R Galloway, Ming-Chang Chen, Franklin Dollar, Christopher A Mancuso, Amelia Hankla, Luis Miaja-Avila, Galen O'Neil, Justin M Shaw, Guangyu Fan, Skirmantas Ališauskas, Giedrius Andriukaitis, Tadas Balčiunas, Oliver D Mücke, Audrius Pugzlys, Andrius Baltuška, Henry C Kapteyn, Tenio Popmintchev, Margaret M Murnane

Overview

Coherent X-rays are an ideal probe of the ultra-fast and ultra-small atomic and molecular world, due to their nature of having extremely short wavelength, short pulse duration, unique ability to penetrate thick and opaque objects combined with elemental specific fingerprints from the atomic absorption edges. While Ultrafast spectroscopies in the visible and infrared (IR) energy regions can probe non-equilibrium dynamics on the ultrafast time scale, they cannot determine the chemical nature of the excited state dynamics with elemental selectivity. Alternatively, coherent X-ray spectroscopies have an important additional advantage of being able to uncover oxidation state, magnetic state, or charge localization to specific elements, giving information about the electronic structures, (i.e., valence, bands and charge), as well as orbital and spin ordering phenomena. Using coherent high harmonic supercontinua laser-like beams, high quality extended edge coherent absorption spectroscopy of materials have been observed in the near-keV region for the first time, to obtain structural and chemical information.

Summary

In the near future, because high harmonic X-ray bursts emerge as an isolated femtosecond-to-attosecond pulses, it will be possible to perform extensive spatio-temporal and chemical imaging of the local atomic structure of materials. The attosecond -picometer resolution metrology science is .. a hand away.

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Published in PRL
http://dx.doi.org/10.1103/PhysRevLett.120.093002

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

Phys Rev Lett 2018 Mar;120(9):093002

JILA, University of Colorado at Boulder, Boulder, Colorado 80309-0440, USA.

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.





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Source
https://link.aps.org/doi/10.1103/PhysRevLett.120.093002
Publisher Site
http://dx.doi.org/10.1103/PhysRevLett.120.093002DOI Listing
March 2018
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