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arXiv:1205.4974 · Physical Review Letters

Observation of Blueshifted Ultralong-Range Cs 2 Rydberg Molecules

J. Tallant, Seth T. Rittenhouse, Donald W. Booth, H. R. Sadeghpour, James P. Shaffer

Published Oct 23, 2012• 103 citations
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Abstract

We observe ultralong-range blueshifted Cs(2) molecular states near ns(1/2) Rydberg states in an optical dipole trap, where 31≤n≤34. The accidental near degeneracy of (n-4)l and ns Rydberg states for l>2 in Cs, due to the small fractional ns quantum defect, leads to nonadiabatic coupling among these states, producing potential wells above the ns thresholds. Two important consequences of admixing high angular momentum states with ns states are the formation of large permanent dipole moments, ~15-100 Debye, and accessibility of these states via two-photon association. The observed states are in excellent agreement with theory.

DOI
10.1103/physrevlett.109.173202

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We observe ultralong-range blueshifted Cs(2) molecular states near ns(1/2) Rydberg states in an optical dipole trap, where 31≤n≤34. The accidental near degeneracy of (n-4)l and ns Rydberg states for l>2 in Cs, due to the small fractional ns quantum defect, leads to nonadiabatic coupling among these states, producing potential wells above the ns thresholds. Two important consequences of admixing high angular momentum states with ns states are the formation of large permanent dipole moments, ~15-100 Debye, and accessibility of these states via two-photon association. The observed states are in excellent agreement with theory.
We consider ultralong-range polyatomic Rydberg molecules formed by combining a Rydberg cesium atom and a ground-state RbCs molecule. We explore the regime where the charge-dipole interaction due to the Rydberg electron with the diatomic polar molecule couples the quantum defect Rydberg states Cs(ns)\mathrm{Cs}(ns)Cs(ns) to the nearest degenerate hydrogenic manifold. We consider polyatomic Rydberg molecules in states which are amenable to production in optical tweezers and study the influence of nonadiabatic coupling on the likelihood of their formation. The decay rates of the vibrational states reflect the interference signature of wave function spread in different coupled potential wells.
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The ultralong-range Cs2 Rydberg molecules consisting of a Rydberg, nD5/2 ( principal quantum number n =35-38), and a ground state atom, 6S1/2 (F=4) are prepared by a two-photon photoassociation spectroscopy in an ultracold Cs gas. This kind of molecule is bound with the low energy scattering and has a permanent dipole moment. We observe two Rydberg-ground state molecular spectra, one is deep-bound molecule, TΣ state, bound by triplet s-wave scattering length and the other one is shallow-bound molecule, S,TΣ state, bound by mixed singlet-triplet s-wave scattering length. The binding energy of Rydberg-ground molecules are attained by analyzing the two photon photoassociation spectrum, corresponding permanent dipole moment is measured by applying an external electric field, which is compared to the calculation.
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.
Vibrational properties of ultralong Rydberg Cs2_22​ molecules are investigated on corresponding potential curves obtained by perturbation theory. The Rydberg Cs2_22​ molecules are associated by a Rydberg Cs(nS/nPnS/nPnS/nP) atom (n=30−70)(n=30-70)(n=30−70) and a ground state Cs(6s6s6s) atom. The starting point for the perturbation treatment of corresponding Rydberg molecular potential curves is to generate accurate atomic Rydberg states from realistic {\it ab initio} effective core potential. The calculated results have similar characteristics with available experimental and theoretical investigations on Rydberg Rb2_22​ molecules. And this is the first time that Rydberg molecules are studied at the {\it ab initio} level.