Observation of Cesium (nD 5/2+6S 1/2) Ultralong-Range Rydberg-Ground MoleculesSupported by the National Key R&D Program of China (Grant No. 2017YFA0304203), the National Natural Science Foundation of China (Grant Nos. 11434007, 61835007, 61675123, 61775124, and 11904215), Changjiang Scholars and Innovative Research Team in Universities of Ministry of Education of China (Grant No. IRT 17R70), and the 1331 Project.

Abstract

Ultralong-range Cs2 Rydberg-ground molecules (nD 5/2 + 6S 1/2 F) (33 ≤ n ≤ 39, F = 3 or 4) are investigated by a two-photon photo-association spectroscopy of an ultracold Cs gas. Two vibrational ground molecular spectra of triplet 3 Σ and hyperfine mixed singlet-triplet 1,3 Σ molecular states and their corresponding binding energies are attained. The experimental observations are simulated by an effective Hamiltonian including low energy electron scattering pseudopotentials, the spin-orbit interaction of the Rydberg atom, and the hyperfine interaction of the ground-state atom. The zero-energy singlet and triplet s-wave scattering lengths are extracted by comparing the experimental observations and calculations. Dependences of the measured binding energies on the effective principal quantum number, n eff = n − δD (δD is the quantum defect of Rydberg D state), yield the scaling of , for deep triplet potential and , for shallow mixed singlet-triplet potential well. The simulations of low-energy Rydberg electron scattering show agreement well with the experimental measurements.