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Bulletin of the American Physical Society

Singlet-triplet electron scattering admixture due to fine- and hyper-fine interactions in Cs Rydberg molecules

Samuel C. Markson, Seth T. Rittenhouse, H. R. Sadeghpour

Published May 24, 2016• 0 citations
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Ultralong-range Cs 2 Rydberg-ground molecules ( nD 5/2 + 6 S 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 − δ D ( δ D is the quantum defect of Rydberg D state), yield the scaling of n eff − 5.60 ± 0.16 ( 3 ​ Σ , F = 3 ) , n eff − 5.62 ± 0.16 ( 3 ​ Σ , F = 4 ) for deep triplet potential and n eff − 5.65 ± 0.38 ( 1 , 3 ​ Σ , F = 3 ) , n eff − 6.19 ± 0.14 ( 1 , 3 ​ Σ , F = 4 ) for shallow mixed singlet-triplet potential well. The simulations of low-energy Rydberg electron scattering show agreement well with the experimental measurements.
We observe the formation of long-range Cs2 Rydberg molecules consisting of a Rydberg and a ground-state atom by photoassociation spectroscopy in an ultracold Cs gas near 6s1/2(F=3,4)→np3/2 resonances (n=26-34). The spectra reveal two types of molecular states recently predicted by D. A. Anderson, S. A. Miller, and G. Raithel [Phys. Rev. A 90, 062518 (2014)]: states bound purely by triplet s-wave scattering with binding energies ranging from 400 MHz at n=26 to 80 MHz at n=34, and states bound by mixed singlet-triplet s-wave scattering with smaller and F-dependent binding energies. The experimental observations are accounted for by an effective Hamiltonian including s-wave scattering pseudopotentials, the hyperfine interaction of the ground-state atom, and the spin-orbit interaction of the Rydberg atom. The analysis enables the characterization of the role of singlet scattering in the formation of long-range Rydberg molecules and the determination of an effective singlet s-wave scattering length for low-energy-electron-Cs collisions.
We report on the observation of long-range Cs 2 Rydberg molecules consisting of a p-state Rydberg atom and a ground-state atom. Two types of molecular states are visible in the photoassociation spectra: states bound purely by triplet s -wave scattering and states bound by mixed singlet-triplet s -wave scattering. An effective Hamiltonian including s -wave scattering pseudopotentials, the hyperfine interaction of the ground-state atom, and the spin-orbit interaction of the Rydberg atom reproduces the experimental observations. The detailed analysis reveals the important role of singlet scattering in long-range Rydberg molecules and yields an effective singlet s-wave scattering length for low-energy e − -Cs collisions.