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The preceding paper describes a strategy for externally influencing thecourse of short-time electronic excitation transfer (EET) in molecular dimersand observing the process by nonlinear wave-packet interferometry (nl-WPI).Within a sample of isotropically oriented dimers having a specified internalgeometry, a vibrational mode internal to the acceptor chromophore can bepreferentially driven by electronically nonresonant impulsive stimulated Raman(or resonant infrared) excitation with a short polarized control pulse. Asubsequent electronically resonant polarized pump then preferentially excitesthe donor, and EET ensues. Here we test both the control strategy and itsspectroscopic investigation-with some sacrifice of amplitude-level detail-bycalculating the pump-probe difference signal. That signal is the limiting caseof the control-influenced nl-WPI signal in which the two pulses in the pumppulse-pair coincide, as do the two pulses in the probe pulse-pair. We presentcalculated pump-probe difference signals for (1) a model excitation-transfercomplex in which two equal-energy monomers each support one moderatelyFranck-Condon active intramolecular vibration; (2) a simplified model of thecovalent dimer dithia-anthracenophane, representing its EET dynamics followingselective impulsive excitation of the weakly Franck-Condon active anthracenevibration at 385 cm-1; and (3) a model complex featuring moderateelectronic-vibrational coupling in which the site energy of the acceptorchromophore is lower than that of the donor.

journal of chemical physics online/the journal of chemical physics/journal of chemical physics

Calculations of Nonlinear Wave-Packet Interferometry Signals in the  Pump-Probe Limit as Tests for Vibrational Control over Electronic Excitation  Transfer