Steill, Jeffrey D., Kay, Jeffrey J., Paterson, Grant, Sharples, Thomas R., KÅos, Jacek, Costen, Matthew L., Strecker, Kevin E., McKendrick, Kenneth G., Alexander, M. H., and Chandler, David W.
Wereport the direct angle-resolved measurement of collision-inducedalignment of short-lived electronically excited molecules using crossedatomic and molecular beams. Utilizing velocity-mapped ion imaging,we measure the alignment of NO in its first electronically excitedstate (A2Σ) following single collisionswith Ne atoms. We prepare A2Σ(v= 0, N= 0, j= 0.5)and by comparing images obtained using orthogonal linear probe laserpolarizations, we experimentally determine the degree of alignmentinduced by collisional rotational excitation for the final rotationalstates NⲠ= 4, 5, 7, and 9. The experimentalresults are compared to theoretical predictions using both a simpleclassical hard-shell model and quantum scattering calculations onan ab initio potential energy surface (PES). The experimental resultsshow overall trends in the scattering-angle dependent polarizationsensitivity that are accounted for by the simple classical model,but structure in the scattering-angle dependence that is not. Thequantum scattering calculations qualitatively reproduce this structure,and we demonstrate that the experimental measurements have the sensitivityto critique the best available potential surfaces. This sensitivityto the PES is in contrast to that predicted for ground-state NO(X)alignment. [ABSTRACT FROM AUTHOR]