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Using wave-packet interferometry to monitor the external vibrational control of electronic excitation transfer
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Image of FIG. 1.
FIG. 1.

Top panel: initial trajectories of wave packets launched impulsively to the donor-excited electronic state (shown as elongated ovals for clarity) overlaying contour plots for the harmonic surfaces of two site-excited states, each of which is displaced by from the ground-state potential minimum along the appropriate nuclear coordinate. Bottom panel: population of the donor-excited state for the wave packets whose initial trajectories are shown in the left panel; in this simulation any population lost by the donor is gained by the acceptor and vice versa. Shown are the cases in which the wave packet prior to electronic excitation is the vibrational ground state (solid line) or a coherent state executing harmonic motion along the acceptor vibrational coordinate (dashed line).

Image of FIG. 2.
FIG. 2.

Schematic representation of the pulse sequence for the experiments considered here. The preresonant control pulse precedes the nl-WPI sequence . The absolute phase of any pulse is considered random, while the phase differences and are precisely controlled.


Generic image for table
Table I.

Rotationally averaged values for the direction-cosine terms multiplying the wave-packet overlaps that compose the signals considered here. For the case of “parallel probing,” we take the four WPI pulses (, , , and ) polarized parallel to each other and perpendicular to the control pulse . is the angle between the monomer transition-dipole moments.

Generic image for table
Table II.

The same as Table I, but in this case the “probe pulse pair” ( and ) is polarized parallel to the control pulse and perpendicular to the “pump pulse pair” ( and ).


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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Using wave-packet interferometry to monitor the external vibrational control of electronic excitation transfer