Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

arXiv:2401.09618 · Physical Review A

Ultralong-range Cs-RbCs Rydberg molecules: Nonadiabaticity of dipole moments

David Mellado-Alcedo, Alexander Guttridge, Simon L. Cornish, H. R. Sadeghpour, Rosario González‐Férez

Published Jul 15, 2024• 4 citations
arXivHTMLPDF

Abstract

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 $\mathrm{Cs}(ns)$ 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.

DOI
10.1103/physreva.110.013314

Related papers

Ultralong-range polyatomic Rydberg molecules formed by a polar perturber

Seth T. Rittenhouse, Michael Mayle, Peter Schmelcher +1 more

The internal electric field of a Rydberg atom electron can bind a polar molecule to form a giant ultralong-range stable polyatomic molecule. Such molecules not only share their properties with Rydberg atoms (such as long lifetimes and large sizes) but they also possess huge permanent electric dipole moments and in addition allow for coherent control of the polar molecule orientation. In this work, we include additional Rydberg manifolds which couple to the nearly degenerate set of Rydberg states employed in the previous work (S T Rittenhouse and H R Sadeghpour 2010 Phys. Rev. Lett. 104 243002). The coupling of a set of ( n + 3)s Rydberg states with the n ( l > 2) nearly degenerate Rydberg manifolds in alkali metal atoms leads to pronounced avoided crossings in the Born–Oppenheimer potentials. Ultimately, these avoided crossings enable the formation of the giant polyatomic Rydberg molecules with standard two-photon laser photoassociation techniques.

arXiv:1101.5353•Journal of Physics B Atomic Molecular and Optical Physics•Sep 14, 2011•24 citations

Observation of Blueshifted Ultralong-Range Cs 2 Rydberg Molecules

J. Tallant, Seth T. Rittenhouse, Donald W. Booth +2 more

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.

arXiv:1205.4974•Physical Review Letters•Oct 23, 2012•103 citations

Polyatomic ultralong-range Rydberg molecules in external fields

Javier Aguilera-Fernández, Rosario González‐Férez

We consider an ultralong-range polytonic Rydberg molecule formed by a Rydberg atom and two heteronuclear diatomic molecules. We focus here on the interaction of a Rb( n = 24, l ≥ 3) Rydberg atom with two KRb diatomic polar molecules in their rotational ground state. The polar diatomic molecules are allowed to rotate in the electric fields generated by the Rydberg electron and core. We investigate the electronic structure of this ultralong-range polytomic Rydberg molecule, and rovibrational properties of the two polar dimers as an additional external field is applied.

Journal of Physics Conference Series•Sep 7, 2015•0 citations

Production of trilobite Rydberg molecule dimers with kilo-Debye permanent electric dipole moments

Donald W. Booth, Seth T. Rittenhouse, J. Yang +2 more

Permanent electric dipole moments are important for understanding symmetry breaking in molecular physics, control of chemical reactions, and realization of strongly correlated many-body quantum systems. However, large molecular permanent electric dipole moments are challenging to realize experimentally. We report the observation of ultralong-range Rydberg molecules with bond lengths of ~100 nanometers and kilo-Debye permanent electric dipole moments that form when an ultracold ground-state cesium (Cs) atom becomes bound within the electronic cloud of an extended Cs electronic orbit. The electronic character of this hybrid class of "trilobite" molecules is dominated by degenerate Rydberg manifolds, making them difficult to produce by conventional photoassociation. We used detailed coupled-channel calculations to reproduce their properties quantitatively. Our findings may lead to progress in ultracold chemistry and strongly correlated many-body physics.

arXiv:1411.5291•Science•Apr 2, 2015•154 citations

Experimental Study of Cs Isotropic and Anisotropic Polyatomic Rydberg Molecules

Jin Long Yang

In this thesis, we investigate few-body physics and many-body physics of ultralong-range Rydberg molecules. Ultralong-range Rydberg molecules are formed through scattering processes between Rydberg electrons and ground state atoms. The huge size of the Rydberg electron's orbit makes the Rydberg electron able to interact with more than one ground state atom in cold atomic gases with atom number densities from 10$^{12}$ cm$^{-3}$ to 10$^{14}$ cm$^{-3}$. In cold atomic gases, the ground state atoms on average are far away from each other. They are weakly interacting. Depending on the angular momentum state of the Rydberg electron, two types of polyatomic Rydberg molecules have been studied. When the Rydberg electron is in an $ns$ state, the isotropic probability distribution of the Rydberg electron makes the Rydberg electron interact with different ground state atoms equally. The total binding energy is a summation of the binding energy from each scattering process. These additive interactions have been studied using Cs $6s+83s$ and $6s+90s$ polyatomic Rydberg molecules in this thesis. When the Rydberg electron is in an $l>0$ angular momentum state, spatial correlations between different ground state atoms are established through the anisotropic probability distribution of the Rydberg electron. The total binding energy depends on the relative positions of different ground state atoms. These nonadditive interactions are studied using Cs $6s+6s+34d$ and $6s+6s+36d$ triatomic Rydberg molecules in this thesis.

•Jan 1, 2019•0 citations

Spin mixing in Cs ultralong-range Rydberg molecules: a case study

Samuel C. Markson, Seth T. Rittenhouse, Richard Schmidt +2 more

We calculate vibrational spectra of ultralong-range Cs(32p) Rydberg molecules which form in an ultracold gas of Cs atoms. We account for the partial-wave scattering of the Rydberg electrons from the ground Cs perturber atoms by including the full set of spin-resolved ${}^{1,3}S_J$ and ${}^{1,3}P_J$ scattering phase shifts, and allow for the mixing of singlet (S=0) and triplet (S=1) spin states through Rydberg electron spin-orbit and ground electron hyperfine interactions. Excellent agreement with observed data in Saßmannshausen et al. [Phys. Rev. Lett. 113, 133201(2015)] in line positions and profiles is obtained. We also determine the spin-dependent permanent electric dipole moments for these molecules. This is the first such calculation of ultralong-range Rydberg molecules in which all of the relativistic contributions are accounted for.

arXiv:1608.06939•Aug 24, 2016•0 citations
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.
The internal electric field of a Rydberg atom electron can bind a polar molecule to form a giant ultralong-range stable polyatomic molecule. Such molecules not only share their properties with Rydberg atoms (such as long lifetimes and large sizes) but they also possess huge permanent electric dipole moments and in addition allow for coherent control of the polar molecule orientation. In this work, we include additional Rydberg manifolds which couple to the nearly degenerate set of Rydberg states employed in the previous work (S T Rittenhouse and H R Sadeghpour 2010 Phys. Rev. Lett. 104 243002). The coupling of a set of ( n + 3)s Rydberg states with the n ( l > 2) nearly degenerate Rydberg manifolds in alkali metal atoms leads to pronounced avoided crossings in the Born–Oppenheimer potentials. Ultimately, these avoided crossings enable the formation of the giant polyatomic Rydberg molecules with standard two-photon laser photoassociation techniques.
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 an ultralong-range polytonic Rydberg molecule formed by a Rydberg atom and two heteronuclear diatomic molecules. We focus here on the interaction of a Rb( n = 24, l ≥ 3) Rydberg atom with two KRb diatomic polar molecules in their rotational ground state. The polar diatomic molecules are allowed to rotate in the electric fields generated by the Rydberg electron and core. We investigate the electronic structure of this ultralong-range polytomic Rydberg molecule, and rovibrational properties of the two polar dimers as an additional external field is applied.
Permanent electric dipole moments are important for understanding symmetry breaking in molecular physics, control of chemical reactions, and realization of strongly correlated many-body quantum systems. However, large molecular permanent electric dipole moments are challenging to realize experimentally. We report the observation of ultralong-range Rydberg molecules with bond lengths of ~100 nanometers and kilo-Debye permanent electric dipole moments that form when an ultracold ground-state cesium (Cs) atom becomes bound within the electronic cloud of an extended Cs electronic orbit. The electronic character of this hybrid class of "trilobite" molecules is dominated by degenerate Rydberg manifolds, making them difficult to produce by conventional photoassociation. We used detailed coupled-channel calculations to reproduce their properties quantitatively. Our findings may lead to progress in ultracold chemistry and strongly correlated many-body physics.
In this thesis, we investigate few-body physics and many-body physics of ultralong-range Rydberg molecules. Ultralong-range Rydberg molecules are formed through scattering processes between Rydberg electrons and ground state atoms. The huge size of the Rydberg electron's orbit makes the Rydberg electron able to interact with more than one ground state atom in cold atomic gases with atom number densities from 1012^{12}12 cm−3^{-3}−3 to 1014^{14}14 cm−3^{-3}−3. In cold atomic gases, the ground state atoms on average are far away from each other. They are weakly interacting. Depending on the angular momentum state of the Rydberg electron, two types of polyatomic Rydberg molecules have been studied. When the Rydberg electron is in an nsnsns state, the isotropic probability distribution of the Rydberg electron makes the Rydberg electron interact with different ground state atoms equally. The total binding energy is a summation of the binding energy from each scattering process. These additive interactions have been studied using Cs 6s+83s6s+83s6s+83s and 6s+90s6s+90s6s+90s polyatomic Rydberg molecules in this thesis. When the Rydberg electron is in an l>0l>0l>0 angular momentum state, spatial correlations between different ground state atoms are established through the anisotropic probability distribution of the Rydberg electron. The total binding energy depends on the relative positions of different ground state atoms. These nonadditive interactions are studied using Cs 6s+6s+34d6s+6s+34d6s+6s+34d and 6s+6s+36d6s+6s+36d6s+6s+36d triatomic Rydberg molecules in this thesis.
We calculate vibrational spectra of ultralong-range Cs(32p) Rydberg molecules which form in an ultracold gas of Cs atoms. We account for the partial-wave scattering of the Rydberg electrons from the ground Cs perturber atoms by including the full set of spin-resolved 1,3SJ{}^{1,3}S_J1,3SJ​ and 1,3PJ{}^{1,3}P_J1,3PJ​ scattering phase shifts, and allow for the mixing of singlet (S=0) and triplet (S=1) spin states through Rydberg electron spin-orbit and ground electron hyperfine interactions. Excellent agreement with observed data in Saßmannshausen et al. [Phys. Rev. Lett. 113, 133201(2015)] in line positions and profiles is obtained. We also determine the spin-dependent permanent electric dipole moments for these molecules. This is the first such calculation of ultralong-range Rydberg molecules in which all of the relativistic contributions are accounted for.