Ultrafast X-ray measurements of the glass-like, high-frequency stiffness of aqueous solutions

2017 ◽  
Vol 19 (31) ◽  
pp. 21095-21100 ◽  
Author(s):  
Yishuo Jiao ◽  
Bernhard Adams ◽  
Christoph Rose-Petruck

The ultrafast dynamics of the domains surrounding solutes in aqueous solution were measured using laser-generating GHz phonons in 30 mM ferrocyanide solutions and the resulting molecular motions of the solutes and their hydrogen-bonded solvation shells were detected using ultrafast X-ray absorption spectroscopy (UXAS).

2014 ◽  
Vol 140 (24) ◽  
pp. 244506 ◽  
Author(s):  
Iradwikanari Waluyo ◽  
Dennis Nordlund ◽  
Uwe Bergmann ◽  
Daniel Schlesinger ◽  
Lars G. M. Pettersson ◽  
...  

2019 ◽  
Vol 21 (18) ◽  
pp. 9239-9245 ◽  
Author(s):  
Zoltán Németh ◽  
Éva G. Bajnóczi ◽  
Bogdán Csilla ◽  
György Vankó

Aqueous solutions of the ternary system Ni(ii)–EDTA–CN− are investigated with X-ray Absorption Spectroscopy (XAS) as a function of cyanide concentration with an enhanced laboratory von Hámos X-ray spectrometer.


2018 ◽  
Vol 10 (1) ◽  
pp. 52-58 ◽  
Author(s):  
Carlo Kleine ◽  
Maria Ekimova ◽  
Gildas Goldsztejn ◽  
Sebastian Raabe ◽  
Christian Strüber ◽  
...  

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.


2005 ◽  
Vol 109 (27) ◽  
pp. 5995-6002 ◽  
Author(s):  
Lars-Åke Näslund ◽  
David C. Edwards ◽  
Philippe Wernet ◽  
Uwe Bergmann ◽  
Hirohito Ogasawara ◽  
...  

2018 ◽  
Vol 232 (5-6) ◽  
pp. 705-722 ◽  
Author(s):  
Masanari Nagasaka ◽  
Hayato Yuzawa ◽  
Nobuhiro Kosugi

Abstract Intermolecular interactions of pyridine in liquid and in aqueous solution are studied by using soft X-ray absorption spectroscopy (XAS) at the C, N, and O K-edges. XAS of liquid pyridine shows that the N 1s→π* peak is blue shifted and the C 1s→π* peak of the meta and para sites is red shifted, respectively, as compared with XAS of pyridine gas. These shifts in liquid are smaller than those in clusters, indicating that the intermolecular interaction of liquid pyridine is weaker than that of pyridine cluster, as supported by the combination of quantum chemical calculations of the core excitation and molecular dynamics simulations of the liquid structure. On the other hand, XAS spectra of aqueous pyridine solutions (C5H5N)x(H2O)1−x measured at different molar fractions show that in the pyridine rich region, x>0.7, the C and N 1s→π* peak energies are not so different from pure liquid pyridine (x=1.0). In this region, antiparallel displaced structures of pyridine molecules are dominant as in pure pyridine liquid. In the O K-edge XAS, the pre-edge peaks sensitive to the hydrogen bond (HB) network of water molecules show the red shift of −0.15 eV from that of bulk water, indicating that small water clusters with no large-scale HB network are formed in the gap space of structured pyridine molecules. In the water rich region, 0.7>x, the N 1s→π* peaks and the O 1s pre-edge peaks are blue shifted, and the C 1s→π* peaks of the meta and para sites are red-shifted by increasing molar fraction of water. The HB network of bulk water is dominant, but quantum chemical calculations indicate that small pyridine clusters with the HB interaction between the H atom in water and the N atom in pyridine are still existent even in very dilute pyridine solutions.


Fuel ◽  
2012 ◽  
Vol 102 ◽  
pp. 156-161 ◽  
Author(s):  
Hiroyuki Akiho ◽  
Tohru Yamamoto ◽  
Yoshihisa Tochihara ◽  
Naoki Noda ◽  
Shinichi Noguchi ◽  
...  

2021 ◽  
Vol 21 (4) ◽  
pp. 2881-2894
Author(s):  
Georgia Michailoudi ◽  
Jack J. Lin ◽  
Hayato Yuzawa ◽  
Masanari Nagasaka ◽  
Marko Huttula ◽  
...  

Abstract. Glyoxal (CHOCHO) and methylglyoxal (CH3C(O)CHO) are well-known components of atmospheric particles and their properties can impact atmospheric chemistry and cloud formation. To get information on their hydration states in aqueous solutions and how they are affected by the addition of inorganic salts (sodium chloride (NaCl) and sodium sulfate (Na2SO4)), we applied carbon and oxygen K-edge X-ray absorption spectroscopy (XAS) in transmission mode. The recorded C K-edge spectra show that glyoxal is completely hydrated in the dilute aqueous solutions, in line with previous studies. For methylglyoxal, supported by quantum chemical calculations we identified not only C–H, C=O and C–OH bonds, but also fingerprints of C–OH(CH2) and C=C bonds. The relatively low intensity of C=O transitions implies that the monohydrated form of methylglyoxal is not favored in the solutions. Instead, the spectral intensity is stronger in regions where products of aldol condensation and enol tautomers of the monohydrates contribute. The addition of salts was found to introduce only very minor changes to absorption energies and relative intensities of the observed absorption features, indicating that XAS in the near-edge region is not very sensitive to these intermolecular organic–inorganic interactions at the studied concentrations. The identified structures of glyoxal and methylglyoxal in an aqueous environment support the uptake of these compounds to the aerosol phase in the presence of water and their contribution to secondary organic aerosol formation.


Sign in / Sign up

Export Citation Format

Share Document