Picosecond and femtosecond X-ray absorption spectroscopy of molecular systems

Author(s):  
Majed Chergui

The need to visualize molecular structure in the course of a chemical reaction, a phase transformation or a biological function has been a dream of scientists for decades. The development of time-resolved X-ray and electron-based methods is making this true. X-ray absorption spectroscopy is ideal for the study of structural dynamics in liquids, because it can be implemented in amorphous media. Furthermore, it is chemically selective. Using X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) in laser pump/X-ray probe experiments allows the retrieval of the local geometric structure of the system under study, but also the underlying photoinduced electronic structure changes that drive the structural dynamics. Recent developments in picosecond and femtosecond X-ray absorption spectroscopy applied to molecular systems in solution are reviewed: examples on ultrafast photoinduced processes such as intramolecular electron transfer, low-to-high spin change, and bond formation are presented.

Author(s):  
Matthew R. Ross ◽  
Benjamin E Van Kuiken ◽  
Matthew L. Strader ◽  
Hana Cho ◽  
Amy Cordones-Hahn ◽  
...  

2002 ◽  
Vol 116 (7) ◽  
pp. 2955-2966 ◽  
Author(s):  
Christian Bressler ◽  
Melanie Saes ◽  
Majed Chergui ◽  
Daniel Grolimund ◽  
Rafael Abela ◽  
...  

Author(s):  
Matthew Ross ◽  
Benjamin E. Van Kuiken ◽  
Mathew L. Strader ◽  
Amy Cordones-Hahn ◽  
Hana Cho ◽  
...  

2008 ◽  
Vol 16 (1) ◽  
pp. 110-115 ◽  
Author(s):  
Tokushi Sato ◽  
Shunsuke Nozawa ◽  
Kohei Ichiyanagi ◽  
Ayana Tomita ◽  
Matthieu Chollet ◽  
...  

2004 ◽  
Vol 75 (1) ◽  
pp. 24-30 ◽  
Author(s):  
Melanie Saes ◽  
Frank van Mourik ◽  
Wojciech Gawelda ◽  
Maik Kaiser ◽  
Majed Chergui ◽  
...  

2022 ◽  
Vol 29 (1) ◽  
Author(s):  
Yujin Kim ◽  
Daewoong Nam ◽  
Rory Ma ◽  
Sangsoo Kim ◽  
Myung-jin Kim ◽  
...  

Understanding the ultrafast dynamics of molecules is of fundamental importance. Time-resolved X-ray absorption spectroscopy (TR-XAS) is a powerful spectroscopic technique for unveiling the time-dependent structural and electronic information of molecules that has been widely applied in various fields. Herein, the design and technical achievement of a newly developed experimental apparatus for TR-XAS measurements in the tender X-ray range with X-ray free-electron lasers (XFELs) at the Pohang Accelerator Laboratory XFEL (PAL-XFEL) are described. Femtosecond TR-XAS measurements were conducted at the Ru L 3-edge of well known photosensitizer tris(bipyridine)ruthenium(II) chloride ([Ru(bpy)3]2+) in water. The results indicate ultrafast photoinduced electron transfer from the Ru center to the ligand, which demonstrates that the newly designed setup is applicable for monitoring ultrafast reactions in the femtosecond domain.


2009 ◽  
Vol 96 (1) ◽  
pp. 11-18 ◽  
Author(s):  
G. Gavrila ◽  
K. Godehusen ◽  
C. Weniger ◽  
E. T. J. Nibbering ◽  
T. Elsaesser ◽  
...  

2016 ◽  
Vol 49 (2) ◽  
pp. 385-388 ◽  
Author(s):  
Kanokwan Kanchiang ◽  
Atipong Bootchanont ◽  
Janyaporn Witthayarat ◽  
Sittichain Pramchu ◽  
Panjawan Thanasuthipitak ◽  
...  

Chrysoberyl is one of the most interesting minerals for laser applications, widely used for medical purposes, as it exhibits higher laser performance than other materials. Although its utilization has been vastly expanded, the location of transition metal impurities, especially the iron that is responsible for chrysoberyl's special optical properties, is not completely understood. The full understanding and control of these optical properties necessitates knowledge of the precise location of the transition metals inside the structure. Therefore, synchrotron X-ray absorption spectroscopy (XAS), a local structural probe sensitive to the different local geometries, was employed in this work to determine the site occupation of the Fe3+ cation in the chrysoberyl structure. An Fe K-edge X-ray absorption near-edge structure (XANES) simulation was performed in combination with density functional theory calculations of Fe3+ cations located at different locations in the chrysoberyl structure. The simulated spectra were then qualitatively compared with the measured XANES features. The comparison indicates that Fe3+ is substituted on the two different Al2+ octahedral sites with the proportion 60% on the inversion site and 40% on the reflection site. The accurate site distribution of Fe3+ obtained from this work provides useful information on the doping process for improving the efficiency of chrysoberyl as a solid-state laser material.


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