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arXiv · 2308.02692

Green's function treatment of Rydberg molecules with spins

Chris H. Greene·Matthew T. Eiles
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Abstract

The determination of ultra-long-range molecular potential curves has been reformulated using the Coulomb Greens function to give a solution in terms of the roots of an analytical determinantal equation. For a system consisting of one Rydberg atom with fine structure and a neutral perturbing ground state atom with hyperfine structure, the solution yields potential energy curves and wavefunctions in terms of the quantum defects of the Rydberg atom and the electron-perturber scattering phaseshifts and hyperfine splittings. This method provides a promising alternative to the standard currently utilized method of diagonalization, which suffers from problematic convergence issues and nonuniqueness, and can potentially yield a more quantitative relationship between Rydberg molecule spectroscopy and electron-atom scattering phaseshifts.

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Chris H. Greene, Matthew T. Eiles. 2023-08-04. Green's function treatment of Rydberg molecules with spins. https://doi.org/10.1103/physreva.108.042805

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