In this work we model and realize stimulated Raman adiabatic passage (STIRAP) in the diatomic 23 Na 40 K molecule from weakly bound Feshbach molecules to the rovibronic ground state via the |v d = 5, J = Ω = 1 excited state in the d 3 Π electronic potential. We demonstrate how to set up a quantitative model for polar molecule production by taking into account the rich internal structure of the molecules and the coupling laser phase noise. We find excellent agreement between the model predictions and the experiment, demonstrating the applicability of the model in the search of an ideal STIRAP transfer path. In total we produce 5000 fermionic groundstate molecules. The typical phase-space density of the sample is 0.03 and induced dipole moments of up to 0.54 Debye could be observed.Dipolar quantum gases allow for the realization of intriguing new quantum many-body systems and associated phenomena due to their anisotropic and long-range interactions. Among these are the roton driven fluid to crystalline quantum phase transition [1], dipolar droplet formation [2,3], insulators with fractional filling and supersolid phases of dipoles in optical lattices [4] to name only a few. Ultracold polar molecules promise particularly large dipolar interactions due to their large dipole moments.The standard procedure for creating molecules at high phase-space density starts with a mixture of two atomic species close to quantum degeneracy. The two species are then initially adiabatically associated into a weakly bound Feshbach molecular state |F B [5]. From there they can be transferred into the final, electronic, vibrational and rotational (rovibronic) ground state using stimulated Raman adiabatic passage (STIRAP) [6,7]. This last step involves coupling the initial and final state to a common intermediate, electronically excited molecular state. Both |F B and the intermediate state need to be chosen with care in order to allow for a high efficiency in the transfer and thus to preserve the phase space density of the ultracold mixture. This approach has been applied successfully to dipolar KRb [8] to the ground state compared to the STIRAP scheme employed in [11]. We develop a Hamiltonian model to describe the adiabatic transfer in all required details to achieve a quantitative description. In addition to the molecular structure analysis done for different bialkali systems [14,15] we include the complex light coupling into the analysis. This results in a multi-level, crosscoupled model that is intimately related to the work of the Bergmann group on STIRAP in multilevel systems [16] but is specific to the alkali-alkali molecule formation. We investigate how to maximize the STIRAP transfer efficiency for a given intermediate state manifold by optimizing pulse durations and one-photon detuning. We find excellent agreement between simulation and experiment. Finally, we demonstrate ground state molecule creation with a large electric dipole moment of up to 0.54 Debye. I. MOLECULAR LEVEL STRUCTURE AND HAMILTONIAN MODELIn our model we us...

Superpositions of rotational states in polar molecules induce strong, long-range dipolar interactions. Here we extend the rotational coherence by nearly one order of magnitude to 8.7(6) ms in a dilute gas of polar 23 Na 40 K molecules in an optical trap. We demonstrate spin-decoupled magic trapping, which cancels first-order and reduces second-order differential light shifts. The latter is achieved with a dc electric field that decouples nuclear spin, rotation, and trapping light field. We observe density-dependent coherence times, which can be explained by dipolar interactions in the bulk gas.Interacting particles with long coherence times are a key ingredient for entanglement generation and quantum engineering. Cold and ultracold polar molecules [1][2][3][4][5][6][7][8][9][10][11] are promising systems for exploring such quantum manybody physics with long-range interactions [12,13] due to their strong and tunable electric dipole moment and long single-particle lifetime [14,15]. The manipulation of their rich internal degrees of freedom has been studied for different molecular species [16][17][18][19]. First observations include ultracold chemistry and collisions [20,21]. Nuclear spin states in the rovibronic ground state further promise exciting prospects for quantum computation due to their extremely long coherence times [22].Rotation is a particularly appealing degree of freedom for molecules because it is directly linked to their dipolar interactions. It can be manipulated by microwave (MW) fields and superpositions of rotational states with opposite parity exhibit an oscillating dipole moment with a magnitude close to the permanent electric dipole moment d 0 . Consequently, using rotating polar molecules has been proposed for quantum computation [23], to emulate exotic spin models [24] or to create topological superfluids [25].In order to make use of the rotational transition dipole in a spatially inhomogeneous optical trap, the coupling of the rotation to the trap field needs to be canceled. To first order this may be achieved by choosing an appropriate angle between the angular momentum of the molecule and the trapping field polarization ε [26] or a special trap light intensity [19] such that the differential polarizability between rotational ground and excited states is canceled. The trap is then referred to as "magic". Coherence times of about 1 ms have been achieved in bulk gases of polar molecules using these techniques [19,27]. However, this is much shorter than the dipolar interaction time, preventing observation of many-body spin dynamics.The coherence time in such a magic trap is limited by the intensity dependence of the molecular polarizabil-ity, which originates from the coupling between rotation, nuclear spins, and the trapping light field. It has been suggested to apply large magnetic [28] or electric fields [29] to reduce these couplings and thus simplify the polarizabilities of the involved states.In this work, we realize a spin-decoupled magic trap, i.e. a magic polarization angle trap wit...