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Stimulated Raman adiabatic passage (STIRAP) allows to efficientlytransferring the populations between two discrete quantum states and has beenused to prepare molecules in their rovibrational ground state. In realisticmolecules, a well-resolved intermediate state is usually selected to implementthe resonant STIRAP. Due to the complex molecular level structures, the detunedSTIRAP always coexists with the resonant STIRAP and may cause unexpectedinterference phenomenon. However, it is generally accepted that the detunedSTIRAP can be neglected if compared with the resonant STIRAP. Here we report onthe first observation of interference between the resonant and detuned STIRAPin the adiabatic creation of $^{23}$Na$^{40}$K ground-state molecules. Theinterference is identified by observing that the number of Feshbach moleculesafter a round-trip STIRAP oscillates as a function of the hold time, with avisibility of about 90\%. This occurs even if the intermediate excited statesare well resolved, and the single-photon detuning of the detuned STIRAP isabout one order of magnitude larger than the linewidth of the excited state andthe Rabi frequencies of the STIRAP lasers. Moreover, the observed interferenceindicates that if more than one hyperfine level of the ground state ispopulated, the STIRAP prepares a coherent superposition state among them, butnot an incoherent mixed state. Further, the purity of the hyperfine levels ofthe created ground state can be quantitatively determined by the visibility ofthe oscillation.

Observation of interference between resonant and detuned STIRAP in the adiabatic creation of $^{23}$Na$^{40}$K molecules