2009
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Abstract: Ground-state coherent wavepacket motions arising from intermolecular modes with clustered, first-shell solvent molecules were observed using the femtosecond dynamic absorption technique in polar solutions of Zn(II) meso-tetrakis(N-methylpyridyl)porphyrin (ZnTMPyP) with excitation in the Soret absorption band. As was observed previously in bacteriochlorophyll a solution, the pump-probe transients in ZnTMPyP solutions are weakly modulated by slowly damped (effective damping time gamma > 1 ps) features that are a… Show more

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“…Another possible interpretation of this behavior is the possible involvement of solvent molecules in the dephasing of the vibrational coherence. Indeed, coherent pump–probe studies with isotopically marked solvents suggested that in metalated porphyrins strongly damped low-frequency modes can be interpreted as intermolecular vibrations involving clustered solvent molecules around the metal atom . To verify this possibility, we studied the behavior of clustered solvent in the MD trajectories, calculating the average radial distribution function of the THF molecules around the zinc atoms.…”
Section: Resultsmentioning
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“…Another possible interpretation of this behavior is the possible involvement of solvent molecules in the dephasing of the vibrational coherence. Indeed, coherent pump–probe studies with isotopically marked solvents suggested that in metalated porphyrins strongly damped low-frequency modes can be interpreted as intermolecular vibrations involving clustered solvent molecules around the metal atom . To verify this possibility, we studied the behavior of clustered solvent in the MD trajectories, calculating the average radial distribution function of the THF molecules around the zinc atoms.…”
Section: Resultsmentioning
“…Indeed, coherent pump−probe studies with isotopically marked solvents suggested that in metalated porphyrins strongly damped low-frequency modes can be interpreted as intermolecular vibrations involving clustered solvent molecules around the metal atom. 72 To verify this possibility, we studied the behavior of clustered solvent in the MD trajectories, calculating the average radial distribution function of the THF molecules around the zinc atoms. No significant differences across the three samples were detected (Figure S11 of the SI).…”
Section: ■ Introductionmentioning
“…21 In most cases vibrational coherence is associated with a single electronic state, either the initially populated excited state (so called impulsive absorption) or the ground state (formed via impulsive stimulated Raman scattering). 2,7,33 Indirect vibrational coherence mechanisms have also been identified resulting from photochemistry, 5,11,13,14,37 rapid geometric changes, 21 or formation of some other type of product state. 22,32 Distinct from these processes is so-called retention of vibrational coherence, wherein a vibrational wavepacket is formed on one electronic surface and propagates through a barrier or avoided crossing to populate another electronic state with the wavepacket still intact.…”
Section: Resultsmentioning
“…The damping time observed for a similar groundstate vibration at 138 cm −1 in IR144 is 500 fs. 51 These damping times are still considerably shorter than the >1 ps damping times that are usually characteristic of resonance Raman active modes in π → π* chromophores such as porphyrins, 54 perhaps because of interference between modes of comparable frequency in the low-frequency regime (see the normal mode calculation results discussed in Figure S4 of the Supporting Information). The 3PEPS response (Figure 8) shows that a majority fraction of the nonpolar solvation of Cy5 occurs on the 30 fs timescale.…”
Section: ■ Discussionmentioning