IDENTIFICATION OF BORN-OPPENHEIMER POTENTIAL-ENERGY SURFACES OF DIATOMIC-MOLECULES FROM OPTIMIZED CHIRPED PULSES

The optimal control of molecules has been widely studied in recent years. In this paper we explore the feasibility of applying adaptive feedback optimal control to determine Born-Oppenheimer (BO) surfaces, If the molecular wave packet is well localized, laser pulses optimized to transfer population between two surfaces contain information on the potential energy difference in the region scanned by the wave packet in the duration of the pulse. By iterating the experiment with the different values of the nuclear separation large regions of the unknown BO surface can be measured if one of the surfaces is known. The method is simulated with a model experiment on CsI. The results show that the BO surface can be determined with reasonable accuracy. Some limitations and possible extensions of the method are discussed.