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Physical Review Letters

Splitting of Spin-Unitary Spin Multiplets.

M. A. B. Bég, Virendra Pratap Singh

Published Oct 12, 1964• 11 citations
Publisher
DOI
10.1103/physrevlett.13.501

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Observation of spin-structure of ultralong-range Rydberg molecules

Markus Deiß, Shinsuke Haze, Joschka Wolf +6 more

We present an experimental and theoretical study of the spin- and vibrational states of $16P-5S$ ultralong-range Rb$_2$ Rydberg molecules that are bound in the second outermost potential well. Due to resonant $p$-wave interaction, the admixture of a butterfly state, and the combination of spin-spin and spin-orbit couplings these molecules feature non-trivial spin state energy level manifolds. By carrying out Rydberg spectroscopy we observe several vibrational ladders. Each ladder exhibits a characteristic multiplet substructure which facilitates assigning a spin state to each level. Our calculations show that a specific type of spin-orbit interaction can significantly contribute to the multiplet line splittings. This spin-orbit interaction is given by the coupling between the total electron spin and the orbital angular momentum of the Rydberg electron in the reference frame of the ground state atom. Furthermore, we find that the diabaticity of the molecular motion across an avoided crossing in the potential energy curve has a strong impact on the vibrational level structure. Our investigation paves the way for further in-depth studies of subtle interaction mechanisms in Rydberg molecules.

•Jan 25, 2019•0 citations
Investigations have been made of the energy and temporal characteristics of the 3066.2 and 3011.1 nm stimulated emission lines of a strontium vapor laser as a function of the discharge conditions. Experimental data are presented which confirm the hypothesis that the mechanism for depopulation of the lower active level of the lines under study is collisional spin-orbit relaxation in the 3Pj0 multiplet. It is concluded that the search for collisional laser action in atoms and ions exhibiting large multiplet splitting is promising.
Analytical dependences on a static electric field F 0 are derived for the wave functions, matrix elements and probabilities of radiation transitions between multiplet substates interacting in field in pairs, ranging from ordinary doublet states with spin S =1/2, pair-wise interacting sublevels of triplet and quintet states with the magnetic quantum number M =0, to the most general case of states with arbitrary angular L and spin S momenta and maximal magnitude of the magnetic quantum number | M |= L + S -1. Equalization of doublet line intensities in the anticrossing field region and vanishing of one of the two doublet lines in the high-field regime are demonstrated. A general relation is determined between the anticrossing field F A , multiplet splitting and tensor polarizability.
We present an experimental and theoretical study of the spin- and vibrational states of 16P−5S16P-5S16P−5S ultralong-range Rb2_22​ Rydberg molecules that are bound in the second outermost potential well. Due to resonant ppp-wave interaction, the admixture of a butterfly state, and the combination of spin-spin and spin-orbit couplings these molecules feature non-trivial spin state energy level manifolds. By carrying out Rydberg spectroscopy we observe several vibrational ladders. Each ladder exhibits a characteristic multiplet substructure which facilitates assigning a spin state to each level. Our calculations show that a specific type of spin-orbit interaction can significantly contribute to the multiplet line splittings. This spin-orbit interaction is given by the coupling between the total electron spin and the orbital angular momentum of the Rydberg electron in the reference frame of the ground state atom. Furthermore, we find that the diabaticity of the molecular motion across an avoided crossing in the potential energy curve has a strong impact on the vibrational level structure. Our investigation paves the way for further in-depth studies of subtle interaction mechanisms in Rydberg molecules.