Document Type

Article

Publication Date

9-27-2016

Publication Title

PHYSICAL REVIEW X

ISSN

2160-3308

Volume

6

Issue

3

DOI

http://dx.doi.org/10.1103/PhysRevX.6.031047

Abstract

Experimental tools capable of monitoring both atomic and electronic structure on ultrafast (femtosecond to picosecond) time scales are needed for investigating photophysical processes fundamental to light harvesting, photocatalysis, energy and data storage, and optical display technologies. Time-resolved hard x-ray (>3 keV) spectroscopies have proven valuable for these measurements due to their elemental specificity and sensitivity to geometric and electronic structures. Here, we present the first tabletop apparatus capable of performing time-resolved x-ray emission spectroscopy. The time resolution of the apparatus is better than 6 ps. By combining a compact laser-driven plasma source with a highly efficient array of microcalorimeter x-ray detectors, we are able to observe photoinduced spin changes in an archetypal polypyridyl iron complex ½Feð2; 20 -bipyridineÞ3 2þ and accurately measure the lifetime of the quintet spin state. Our results demonstrate that ultrafast hard x-ray emission spectroscopy is no longer confined to large facilities and now can be performed in conventional laboratories with 10 times better time resolution than at synchrotrons. Our results are enabled, in part, by a 100- to 1000-fold increase in x-ray collection efficiency compared to current techniques.

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AUTHORS & AFFILIATIONS

Luis Miaja-Avila1,*, Galen C. O’Neil1, Young I. Joe1, Bradley K. Alpert1, Niels H. Damrauer2, William B. Doriese1, Steven M. Fatur2, Joseph W. Fowler1, Gene C. Hilton1, Ralph Jimenez2,3, Carl D. Reintsema1, Daniel R. Schmidt1, Kevin L. Silverman1, Daniel S. Swetz1, Hideyuki Tatsuno1, and Joel N. Ullom1,4,†

  • 1National Institute of Standards and Technology, 325 Broadway, Boulder, Colorado 80305, USA
  • 2Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder, Colorado 80309, USA
  • 3JILA, National Institute of Standards and Technology and University of Colorado Boulder, 440 UCB, Boulder, Colorado 80309, USA
  • 4Department of Physics, University of Colorado Boulder, Boulder, Colorado 80309, USA
  • *Corresponding author. miaja@nist.gov
  • Corresponding author. joel.ullom@nist.gov

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