Figure 2
Illustration of the photoselection process. Before the arrival of the laser pump ( ), the molecules are randomly oriented in solution. The laser pulse preferentially excites the molecules with the transition dipole moments parallel to the laser polarization axis. Thus, the excited-state population is created as an aligned ensemble (at t = 0 the distribution of the transition dipole moment in molecules being excited is a cosine-squared distribution with respect to the laser polarization axis) yielding anisotropic difference scattering patterns. After the excitation event ( ), the rotation of both the excited and unexcited populations causes rotational dephasing of the alignment. |