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Theory of Ultralong‐Range Rydberg Molecule Formation Incorporating Spin‐Dependent Relativistic Effects: Cs(6s)–Cs(np) as Case Study
Author(s) -
Markson Samuel,
Rittenhouse Seth T.,
Schmidt Richard,
Shaffer James P.,
Sadeghpour H. R.
Publication year - 2016
Publication title -
chemphyschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.016
H-Index - 140
eISSN - 1439-7641
pISSN - 1439-4235
DOI - 10.1002/cphc.201600932
Subject(s) - rydberg formula , atomic physics , hyperfine structure , rydberg matter , physics , singlet state , spin (aerodynamics) , rydberg constant , rydberg atom , rydberg state , dipole , chemistry , ground state , excited state , scattering , quantum mechanics , ionization , ion , thermodynamics
Abstract We calculate vibrational spectra of ultralong‐range Cs(32p) Rydberg molecules that form in an ultracold gas of Cs atoms. We account for the partial‐wave scattering of the Rydberg electrons from the 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 state electron hyperfine interactions. Excellent agreement with observed data in Saßmannshausen et al. [ Phys. Rev. Lett . 2015 , 113 , 133201] 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 for which all of the relativistic contributions are accounted.