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The Journal of Chemical Physics

Dissociation of ultracold cesium Rydberg-ground molecules

Jingxu Bai, Yuechun Jiao, Rong Song, Xijun Li, Jianming Zhao, Suotang Jia

Published Nov 15, 2023• 2 citations
Publisher

Abstract

We report the experimental measurements of the decay rate of polar cesium nD5/2 - 6S1/2 Rydberg-ground molecules with a large principal quantum number range of 35 ≤ n ≤ 40. Rydberg molecules are prepared employing the method of two-photon photoassociation and the molecular (atomic) ions, due to autoionization (blackbody photoionization), are detected with a microchannel plate detector. The decay rate Γ of the vibrational ground state of the deep and shadow bound molecules for triplet (TΣ) and mixed singlet-triplet (S,TΣ) are measured by fitting the molecular population with the exponential function. Comparing with the parent atom, the decay rate of the polar Rydberg-ground molecule shows an obvious increase with a magnitude of a few μs. The possible dissociation mechanism of polar Rydberg-ground molecules including a collisional decay, blackbody induced decay, and coupling of adjacent Rydberg states and tunneling decay are discussed in detail. The theoretical model is induced to simulate the measurements, showing agreement.

DOI
10.1063/5.0175109

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We report the experimental measurements of the decay rate of polar cesium nD5/2 - 6S1/2 Rydberg-ground molecules with a large principal quantum number range of 35 ≤ n ≤ 40. Rydberg molecules are prepared employing the method of two-photon photoassociation and the molecular (atomic) ions, due to autoionization (blackbody photoionization), are detected with a microchannel plate detector. The decay rate Γ of the vibrational ground state of the deep and shadow bound molecules for triplet (TΣ) and mixed singlet-triplet (S,TΣ) are measured by fitting the molecular population with the exponential function. Comparing with the parent atom, the decay rate of the polar Rydberg-ground molecule shows an obvious increase with a magnitude of a few μs. The possible dissociation mechanism of polar Rydberg-ground molecules including a collisional decay, blackbody induced decay, and coupling of adjacent Rydberg states and tunneling decay are discussed in detail. The theoretical model is induced to simulate the measurements, showing agreement.
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.
We present an experimental observation of 37D5/2 + 6S1/2 Cs2 Rydberg-ground molecules by employing a two-photon photoassociation method. Two distinct Rydberg-ground molecular signals, deep and shallow bound molecules, are observed at the red detuning of atomic line. In theory, the model of scattering interaction between the Rydberg electron and ground-state atom is used to simulate the experiments. Two potential energy curves with energy minimum, deep pure triplet 3Σ and shallow hyperfine-mixed singlet–triplet 1,3Σ potentials, refer to the attained Rydberg-ground molecular signals, respectively. Calculations of the binding energy of triplet 3Σ and mixed 1,3Σv = 0 states are compared with the measurements. The agreement between the calculated and measured values of the binding energy yields zero-energy scattering lengths asT(0) = −19.2a0 and asS(0) = −1.3a0, respectively.
Long-range metastable molecules consisting of two cesium atoms in high Rydberg states have been observed in an ultracold gas. A sequential three-photon two-color photoassociation scheme is employed to form these molecules in states, which correlate to np(n+1)s dissociation asymptotes. Spectral signatures of bound molecular states are clearly resolved at the positions of avoided crossings between long-range van der Waals potential curves. The experimental results are in agreement with simulations based on a detailed model of the long-range multipole-multipole interactions of Rydberg-atom pair states. We show that a full model is required to accurately predict the occurrence of bound Rydberg macrodimers. The macrodimers are distinguished from repulsive molecular states by their behavior with respect to spontaneous ionization and possible decay channels are discussed.
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.
The lifetimes of nS1/2 and nD5/2 (n = 60–83) cesium Rydberg states are measured accurately in a magneto-optical trap using the field ionization technique and analyzed with the existing theoretical model. The room temperature blackbody radiation (BBR) and interaction between Rydberg atoms can enhance the decay rate and reduce the spontaneous lifetime of the given Rydberg atom. The measured lifetime shows a good agreement with the calculation accounting a room temperature BBR at low enough Rydberg atomic density. The dependence of measured lifetime on atomic density shows that the collision and interaction between Rydberg atoms have a large effect on the lifetime at higher Rydberg atomic density. The scaling laws of n2.55±0.02 for nD5/2 state and n2.30±0.01 for nS1/2 state within n = 60–83 range are obtained and agreement with the model calculation with a relative deviation less than 3%.