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Ultrafast strong-field dissociative ionization dynamics of probed by femtosecond soft x-ray transient absorption spectroscopy
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10.1063/1.2925268
/content/aip/journal/jcp/128/20/10.1063/1.2925268
http://aip.metastore.ingenta.com/content/aip/journal/jcp/128/20/10.1063/1.2925268

Figures

Image of FIG. 1.
FIG. 1.

Energy level diagram showing the adiabatic correlation of the various ion states to their respective dissociation products.

Image of FIG. 2.
FIG. 2.

Schematic illustration of the experimental setup.

Image of FIG. 3.
FIG. 3.

Pump-probe time traces for (a) the growth of the ion ground state and (b) the depletion of the neutral molecule. These time traces give a Gaussian instrument response function with a FWHM of .

Image of FIG. 4.
FIG. 4.

Soft x-ray transient absorption spectrum collected at a time delay of and an intensity of for the pulse. The spectral peaks at 64.4, 65.1, and correspond to atomic Br transitions from the core level, whereas the peaks at 66.5 and correspond to transitions of parent and fragment in their electronic ground states. The shoulder at corresponds to a transition from the and/or electronically excited state of . The solid line represents the fit of the entire spectrum to a sum of six Gaussian peaks, with each individual component appearing as a dotted line.

Image of FIG. 5.
FIG. 5.

Pump-probe time traces for the appearance of (a) the Br (●) and (○) atoms, and (b) the photofragment ion.

Image of FIG. 6.
FIG. 6.

(a) Soft x-ray transient absorption spectrum collected at a time delay of and an intensity of for the pulse. The peaks at 66.5 and correspond to transitions of parent , whereas the peaks at 68.9 and correspond to transitions of the dication. The depletion of neutral appears at 70.5 and . The solid line represents the fit of the entire spectrum to a sum of six Gaussian peaks (four of which have positive amplitudes and two have negative amplitudes), with each individual component appearing as a dotted line. The inset shows the absence of the atomic Br absorption peak at .

Image of FIG. 7.
FIG. 7.

Pump-probe time trace of the dication species, confirming its significant stability up to .

Image of FIG. 8.
FIG. 8.

Energy level diagram for the Coulomb explosion of , calculated at the level of theory.

Tables

Generic image for table
Table I.

Optimized geometric parameters for the dication ground state and the transition state en route to Coulomb explosion, as well as those for the ground state. Due to the elongation of one of the C–Br bonds in the transition state, two sets of values for the CBr bond length and HCBr bond angle exist for that state.

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/content/aip/journal/jcp/128/20/10.1063/1.2925268
2008-05-23
2014-04-18
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Ultrafast strong-field dissociative ionization dynamics of CH2Br2 probed by femtosecond soft x-ray transient absorption spectroscopy
http://aip.metastore.ingenta.com/content/aip/journal/jcp/128/20/10.1063/1.2925268
10.1063/1.2925268
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