Ultrafast Time-Resolved Hard X-Ray Emission Spectroscopy on a Tabletop

被引:38
作者
Miaja-Avila, Luis [1 ]
O'Neil, Galen C. [1 ]
Joe, Young I. [1 ]
Alpert, Bradley K. [1 ]
Damrauer, Niels H. [2 ]
Doriese, William B. [1 ]
Fatur, Steven M. [2 ]
Fowler, Joseph W. [1 ]
Hilton, Gene C. [1 ]
Jimenez, Ralph [2 ,3 ,4 ]
Reintsema, Carl D. [1 ]
Schmidt, Daniel R. [1 ]
Silverman, Kevin L. [1 ]
Swetz, Daniel S. [1 ]
Tatsuno, Hideyuki [1 ]
Ullom, Joel N. [1 ,5 ]
机构
[1] NIST, 325 Broadway, Boulder, CO 80305 USA
[2] Univ Colorado, Dept Chem & Biochem, Campus Box 215, Boulder, CO 80309 USA
[3] NIST, JILA, 440 UCB, Boulder, CO 80309 USA
[4] Univ Colorado, 440 UCB, Boulder, CO 80309 USA
[5] Univ Colorado, Dept Phys, Boulder, CO 80309 USA
关键词
TRANSITION-METAL-COMPLEXES; EXCITED-STATE DYNAMICS; POLYPYRIDINE COMPLEXES; ELECTRON-TRANSFER; SPIN-TRANSITION; RESOLUTION; IRON(II); LIGHT; MICROCALORIMETER; INTERPLAY;
D O I
10.1103/PhysRevX.6.031047
中图分类号
O4 [物理学];
学科分类号
0702 ;
摘要
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 [Fed2,2'-bipyridine)(3)](2+) 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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页数:13
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