Experimental systems: (a) fs laser and x-ray pulse generating systems showing the collimating polycapillary lens, dispersive spectrometer, detector, and sample. (b) Focusing polycapillary lens.
X-ray spectra emitted by Cu, Mo, and W wire.
X-ray intensity as a function of the delay time between the pump optical pulse and the probe x-ray pulse.
Broadening of the rocking curve, (FWHM), plotted as a function of time delay. Solid line is calculated fit to experimental data.
Change in x-ray diffraction intensity as a function of time. Steep decrease in intensity designates melting. Dots experimental, line simulation. Reproduced with permission from J. Chen, W.-K. Chen, J. Tang, P. M. Rentzepis, PNAS 108, 18887–18892 (2011). Copyright © 2011.
Femtosecond transient absorption spectra of ferrioxalate in water excited by 400 nm pulses. Insert: Energy dependence of the transient optical density at 430 nm.
Picosecond transient absorption spectra of 1.0 × 10−3 M cobaltoxalate in water using 266 nm excitation. Inset: transient kinetics at 720 nm (solid square points) and the 45 ps pulse width (open circle points fitted with solid line).
Nanosecond transient absorption spectra of 2.3 × 10−3 M ferrioxalate in water (266 nm excitation).
Time resolved transient kinetics of Ferrioxalate in water at different concentrations after 266/267 nm excitation (square: 0.044 M, circle: 0.088 M and triangle: 0.177 M). The solid lines are exponential decay fits to the experimental data. Inset: the reaction rate constant at different concentration and the solid line is a linear fit to the experimental data.
Fe K-edge x-ray absorption spectra of ferrioxalate/water solution before (solid, −20 ps) and after (point, +25 ps) UV radiation.
EXAFS spectra in R space of ferrioxalate/water solution before (solid, −20 ps) and after (point, +25 ps) UV radiation.
Schematic diagram of intramolecular electron transfer and intermolecular electron transfer via dissociation mechanism of M(III) complex (L-ligand).
Schematic representation of x-ray absorption spectra.
Fe K-edge XANES spectrum of the LS state of aqueous [FeII(bpy)3]2+ (black trace) and of the HS quintet state (red dots). (B) Transient XANES spectrum (difference in x-ray absorption between the laser-excited sample and the unexcited sample) recorded 50 ps after laser excitation at 400 nm (red dots) (11). The blue stars represent the transient spectrum recorded at a time delay of 300 fs in the present work. Reprinted with permission from C. Bressler, C. Milne, V. T. Pham, A. ElNahhas, R. M. van der Veen, W. Gawelda, S. Johnson, P. Beaud, G. Grolimund, M. Kaiser, C. N. Borca, G. Ingold, R. Abela, M. Chergui, Science 323, 489–92 (2009). Copyright © 2009. 16
XANES spectra of RuN3 adsorbed to TiO2 nanoparticle surface measured at Ru K-edge. The black and green curves are spectra without the laser and with laser excitation at nominally 50 ps, respectively. The red curve is the spectrum for the charge separate state, RuN3+, extracted from the green curve with a 20% conversion at the 50 ps delay. Inset: schematic of MLCT excitation of RuN3, followed by interfacial electron injection from excited RuN3 to TiO2 nanoparticle. Reprinted with permission from X.Zhang, G. Smolentsev, J. Guo, K. Attenkofer, C. Kurtz, G. Jennings, J.V. Lockard, A. B. Stickrath, L. X. Chen, J. Phys. Chem. Lett. 2, 628–632 (2011). Copyright © 2011. 122
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