title: Theory of Ultralong-Range Rydberg Molecule Formation Incorporating Spin-Dependent Relativistic Effects: Cs(6s)-Cs(np) as Case Study.
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-resolved1,3SJand1,3PJscattering 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.
authors.affiliation: ITAMP, Harvard-Smithsonian Center for Astrophysics, Harvard University, 60 Garden St., Cambridge, MA, 02138, USA.|Physics Department, University of Connecticut, Storrs, CT, 06269-3046, USA.
authors.forename: Samuel
authors.initials: S
authors.lastname: Markson
authors.affiliation: Department of Physics, The United States Naval Academy, Annapolis, Maryland, 21402, USA.
authors.forename: Seth T
authors.initials: ST
authors.lastname: Rittenhouse
authors.affiliation: ITAMP, Harvard-Smithsonian Center for Astrophysics, Harvard University, 60 Garden St., Cambridge, MA, 02138, USA.
authors.forename: Richard
authors.initials: R
authors.lastname: Schmidt
authors.affiliation: University of Oklahoma, Homer L. Dodge Department of Physics and Astronomy, Norman, Oklahoma, 73072, USA.
authors.forename: James P
authors.initials: JP
authors.lastname: Shaffer
authors.affiliation: ITAMP, Harvard-Smithsonian Center for Astrophysics, Harvard University, 60 Garden St., Cambridge, MA, 02138, USA.
authors.forename: H R
authors.initials: HR
authors.lastname: Sadeghpour
keywords: Rydberg systems; cold molecules; dipole moments; relativistic effects; vibrational spectroscopy