Ionization potentials of the alkali diatomic molecules KRb, Rb2, and K2 have been investigated and experimental methods for exploring triplet Rydberg states from the metastable a3Σ+ state of ultracold KRb molecules are proposed.
Convenient state-selective detection methods are proposed for exploring triplet Rydberg states from the metastable a 3 Σ + state of ultracold KRb molecules by resonance-enhanced two-photon ionization and time-of-flight (TOF) mass spectroscopy. This would allow the first accurate determination of the ionization potential. Particularly suitable resonant intermediate states include the 2 3 Π Ω , 3 3 Σ + and 4 3 Σ + states, and we report spectroscopic studies of these states. For the 2 3 Π Ω state, the spin–orbit components (Ω = 0 + , 0 − , 1 and 2) have been investigated and a shallow long-range state (5(0 + )) at ∼ 9.3 Å has been observed. We compare our observations of these three states with predictions based on ab initio potential energy curves. Such studies may also permit the direct observation of autoionizing resonances leading to efficient formation of low-lying rovibrational levels of the 2 Σ + ground state of KRb + , ideally in the v + = 0, N + = 0 level.
We investigate the structure and features of an ultralong-range triatomic Rydberg molecule formed by a Rb Rydberg atom and a KRb diatomic molecule. In our numerical description, we perform a realistic treatment of the internal rotational motion of the diatomic molecule, and take into account the Rb( n , l ≥ 3) Rydberg degenerate manifold and the energetically closest neighboring levels with principal quantum numbers n ' > n and orbital quantum number l ≤ 2. We focus here on the adiabatic electronic potentials evolving from the Rb( n,l ≥ 3) and Rb( n = 26, l = 2) manifolds. The directional properties of the KRb diatomic molecule within the Rb-KRb triatomic Rydberg molecule are also analyzed in detail.
In this thesis I report precision spectroscopy with ultracold 87Rb2 triplet molecules where we use lasers to couple the states in different molecular potentials. We study in detail the lowest triplet states of Rb2. These states are of great importance for transferring weakly bound molecules to the ro-vibrational triplet ground state via states of the excited potential. As most experiments start from molecules in their singlet ground state, the triplet states were hard to access via dipole transitions and remained largely unexplored. The measurements presented in this thesis are the first detailed study of diatomic 87Rb2 molecules in these states.