Journal of Physical Chemistry A, Vol.101, No.50, 9594-9602, 1997
Practical aspects of aligning asymmetric top molecules via single-photon excitation: An application to S-1<-S-0 excitation of glyoxal
The practical aspects of aligning glyoxal (CHO-CHO) via S-1 <--S-0 photoexcitation with a linearly polarized laser are considered, with an emphasis on preparing the aligned molecules to probe for steric effects in crossed beam energy transfer, The degree to which ''broadside'' and ''edge-on'' collision geometries can be obtained for the planar glyoxal molecule is quantified. For a pump laser polarization parallel to the relative collision velocity, an aligned distribution is predicted in which a broadside collision is 2.3 times more likely than an edge-on collision. For the perpendicular laser polarization, an edge-on collision is 1.6 times more likely than a broadside collision, Implementation of alignment via photoexcitation in an actual experiment is described. Concerns when aligning molecules via this method are discussed, including saturation effects and nuclear spin depolarization. The laser-induced fluorescence formalism of Greene and Zare [J. Chem. Phys. 1983, 75, 6741] is used to demonstrate that glyoxal call indeed be aligned to the degree predicted by theory.