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We investigate the control of electronic energy transfer in molecular dimersthrough the preparation of specific vibrational coherences prior to electronicexcitation, and its observation by nonlinear wave-packet interferometry.Laser-driven coherent nuclear motion can affect the instantaneous resonancebetween site-excited electronic states and thereby influence short-timeelectronic excitation transfer (EET). We first illustrate this controlmechanism with calculations on a dimer whose constituent monomers undergoharmonic vibrations. We then consider the use of nonlinear wave-packetinterferometry (nl-WPI) experiments to monitor the nuclear dynamicsaccompanying EET in general dimer complexes following impulsive vibrationalexcitation by a sub-resonant control pulse (or control pulse sequence). Inmeasurements of this kind, two pairs of polarized phase-related femtosecondpulses following the control pulse generate superpositions of coherent nuclearwave packets in optically accessible electronic states. Interferencecontributions to the time- and frequency-integrated fluorescence signal due tooverlaps among the superposed wave packets provide amplitude-level informationon the nuclear and electronic dynamics. We derive the basic expression for acontrol-pulse-dependent nl-WPI signal. The electronic transition moments of theconstituent monomers are assumed to have a fixed relative orientation, whilethe overall orientation of the complex is distributed isotropically. We includethe limiting case of coincident arrival by pulses within each phase-relatedpair in which control-influenced nl-WPI reduces to a fluorescence-detectedpump-probe difference experiment. Numerical calculations of pump-probe signalsbased on these theoretical expressions are presented in the following paper.

Using Wave-Packet Interferometry to Monitor the External Vibrational Control of Electronic Excitation Transfer