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. |