A large optical Stark effect has been observed in the two-photon spectrum X 2 Tl-* A 2 X + in nitric oxide. It is explained as a near-resonant process in which the upper state of the two-photon transition is perturbed by interactions with higher-lying electronic states coupled by the laser field. A theoretical analysis is presented along with Stark parameters determined from ab initio wave functions. The synthetic spectrum reproduces the major experimental features.
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