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Physical Review A

Excitonlike exchange in two-photon transitions of pairs of cold Rb Rydberg atoms

Jeonghun Lee, Phatthamon Kongkhambut, Thomas F. Gallagher

Published Dec 26, 2017• 3 citations
Publisher

Abstract

We have observed an excitonlike exchange in two-photon microwave transitions between pairs of cold Rb Rydberg atoms, specifically, transitions in which a $n{s}_{1/2}n{s}_{1/2}$ pair undergoes the transition to the $n{p}_{1/2}n{p}_{3/2}$ and $n{p}_{3/2}n{p}_{1/2}$ states. This transition occurs due to the excitonlike $n{s}_{1/2}n{p}_{j}\ensuremath{\leftrightarrow}n{p}_{j}n{s}_{1/2}$ exchange in the intermediate states, and the process can be thought of as a F\"orster resonant energy transfer between Floquet, or dressed, states. In addition, the measurements provide clear evidence of the importance of the three-dimensional nature of the dipole-dipole interaction.

DOI
10.1103/physreva.96.061401

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Previous measurements of single photon $n{d}_{5/2}n{d}_{5/2}\ensuremath{\rightarrow}(n+1){d}_{j}(n\ensuremath{-}2)f$ transitions by two of us were described as microwave transitions made possible by configuration interaction (CI) between the $n{d}_{5/2}n{d}_{5/2}$ and the nearly degenerate $(n+2){p}_{3/2}(n\ensuremath{-}2)f$ states [Lee and Gallagher, Phys. Rev. A 93, 062509 (2016)]. Here we report the observation of the one photon $n{d}_{5/2}n{d}_{5/2}\ensuremath{\rightarrow}(n+3){s}_{1/2}(n\ensuremath{-}2)f$, two photon $n{d}_{5/2}n{d}_{5/2}\ensuremath{\rightarrow}(n+3){p}_{j}(n\ensuremath{-}2)f$, and three photon $n{d}_{5/2}n{d}_{5/2}\ensuremath{\rightarrow}(n+4){s}_{1/2}(n\ensuremath{-}2)f$ microwave transitions. We show that both single and multiphoton microwave transitions are conveniently described as Forster resonant energy transfers between resonant Floquet states, and we show that the Floquet-Forster model reduces to the CI model used previously. Finally, to show that the transitions observed previously are by no means unique, we report pair transitions with different initial and final states as well as radio instead of microwave frequencies.

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International Symposium on Molecular Spectroscopy (ISMS)•Jun 23, 2015•0 citations
We have observed an excitonlike exchange in two-photon microwave transitions between pairs of cold Rb Rydberg atoms, specifically, transitions in which a ns1/2ns1/2n{s}_{1/2}n{s}_{1/2}ns1/2​ns1/2​ pair undergoes the transition to the np1/2np3/2n{p}_{1/2}n{p}_{3/2}np1/2​np3/2​ and np3/2np1/2n{p}_{3/2}n{p}_{1/2}np3/2​np1/2​ states. This transition occurs due to the excitonlike ns1/2npj\ensuremath↔npjns1/2n{s}_{1/2}n{p}_{j}\ensuremath{\leftrightarrow}n{p}_{j}n{s}_{1/2}ns1/2​npj​\ensuremath↔npj​ns1/2​ exchange in the intermediate states, and the process can be thought of as a F"orster resonant energy transfer between Floquet, or dressed, states. In addition, the measurements provide clear evidence of the importance of the three-dimensional nature of the dipole-dipole interaction.
Previous measurements of single photon $n{d}_{5/2}n{d}_{5/2}\ensuremath{\rightarrow}(n+1){d}_{j}(n\ensuremath{-}2)f$ transitions by two of us were described as microwave transitions made possible by configuration interaction (CI) between the nd5/2nd5/2n{d}_{5/2}n{d}_{5/2}nd5/2​nd5/2​ and the nearly degenerate $(n+2){p}_{3/2}(n\ensuremath{-}2)f$ states [Lee and Gallagher, Phys. Rev. A 93, 062509 (2016)]. Here we report the observation of the one photon $n{d}_{5/2}n{d}_{5/2}\ensuremath{\rightarrow}(n+3){s}_{1/2}(n\ensuremath{-}2)f$, two photon $n{d}_{5/2}n{d}_{5/2}\ensuremath{\rightarrow}(n+3){p}_{j}(n\ensuremath{-}2)f$, and three photon $n{d}_{5/2}n{d}_{5/2}\ensuremath{\rightarrow}(n+4){s}_{1/2}(n\ensuremath{-}2)f$ microwave transitions. We show that both single and multiphoton microwave transitions are conveniently described as Forster resonant energy transfers between resonant Floquet states, and we show that the Floquet-Forster model reduces to the CI model used previously. Finally, to show that the transitions observed previously are by no means unique, we report pair transitions with different initial and final states as well as radio instead of microwave frequencies.
This dissertation consists of three microwave spectroscopy experiments performed with cold Rb Rydberg atoms in Magneto Optical Trap.The first experiment is a systematic study of a particular type of transition which was first observed in 2012 that involves a pair of Rydberg atoms.In this transition, even though only one microwave photon is absorbed, both atoms in the pair change states.In particular, we describe the transition with the configuration interaction (CI) model and experimentally verify the scaling of fractional population transfer predicted by the CI model.The second experiment builds on the first experiment and reports observations of additional single and multi photon microwave transitions that are allowed due to the same CI as in the first experiment.The observations show clearly that this type of transition involving a pair of Rydberg atoms are a lot more common than initially thought.We show that the transitions can be conveniently described as Forster resonances of Floquet states.The last experiment reports on the technique we used to measure the ng and nh series quantum defects and the ionic dipole and quadrupole polarizabilities of 85 Rb.The technique allows us to obtain zero field intervals of (n + 1)d 5/2 → ng and (n + 1)d 5/2 → nh intervals despite the fact that we can only control the stray electric field in one direction.Using the technique, the quantum defects of ng and nh were determined to be 0.0039741(16) and 0.0014066(57), respectively.The ionic II dipole and quadrupole polarizabilities were determined to be 9.12(2)a 3 0 and 14(3)a 5 0 , respectively.
We have observed the process $\mathrm{Rb}ns+\mathrm{Rb}\phantom{\rule{4pt}{0ex}}ns+2h\ensuremath{\nu}\ensuremath{\rightarrow}\mathrm{Rb}\phantom{\rule{4pt}{0ex}}n{p}_{1/2}+\mathrm{Rb}\phantom{\rule{4pt}{0ex}}n{p}_{3/2}$ from n=34n=34n=34 to n=40n=40n=40 in a frozen gas of Rb Rydberg atoms. It is resonant when the microwave frequency is halfway between the $ns\phantom{\rule{0.16em}{0ex}}\ensuremath{\rightarrow}\phantom{\rule{0.16em}{0ex}}n{p}_{1/2}$ and $ns\ensuremath{\rightarrow}n{p}_{3/2}$ frequencies, which range from 57 to 106 GHz. The process cannot occur in isolated atoms, nor can it occur if the magnetic quantum numbers are unchanged, an implicit assumption of one-dimensional models. A Floquet-Forster model shows that the coupling between the initial and final states involves the absorption of two microwave photons and the dipole-dipole interaction, which leads to a coupling proportional to the product of the density, the microwave field squared, and n∗14{n}^{*14}n∗14, where n∗{n}^{*}n∗ is the effective quantum number of the np3/2n{p}_{3/2}np3/2​ state. We have experimentally verified these dependences. The observed resonances are asymmetric, with a low-frequency tail, which we attribute to the van der Waals shift of the final np1/2np3/2n{p}_{1/2}n{p}_{3/2}np1/2​np3/2​ state due to its dipole-dipole interaction with the nearby ns(n+1)sns(n+1)sns(n+1)s state. While the van der Waals shift is negligible for most of the atoms in the Rydberg gas, it is not for the pairs of close atoms which undergo this transition.
We have observed microwave transitions between pairs of cold Rb atoms, specifically, transitions between the molecular nd(5/2)nd(5/2) and (n+1)d(j)(n-2)f states for 41≤n≤44. (We use the separated atom limits as labels.) The transition is allowed because the dipole-dipole induced configuration interaction between the nd(5/2)nd(5/2) state and the energetically close (n+2)p(3/2)(n-2)f state leads to an admixture of the latter into the former. Such transitions may provide a way of selecting closely spaced pairs of atoms.
Long-range interactions between cold Rydberg atoms, which are used in many important applications, can be enhanced using F\"orster resonances between collective many-body states controlled by an external electric field. Here we report on the first experimental observation of highly resolved radio-frequency-assisted F\"orster resonances in a few cold Rb Rydberg atoms. We also observed radio-frequency-induced F\"orster resonances which cannot be tuned by a dc electric field. They imply an efficient transition from van der Waals to resonant dipole-dipole interaction due to Floquet sidebands of Rydberg levels appearing in the rf field. This method can be applied to enhance the interactions of almost arbitrary Rydberg atoms with large principal quantum numbers.
Microwave transitions between pair states composed of two Rb Rydberg atoms in a magneto-optical trap are investigated. Our current interest is the transition from ndnd to (n+1)d(n-2)f states. This transition is allowed because the dipole-dipole induced configuration interaction between the ndnd state and the energetically close (n+2)p(n-2)f state admixes some of the latter state into the former. The resonance frequencies of the ndnd-(n+1)d(n-2)f transitions for n=35 to 42 have been measured and found to agree well with the calculated values. In addition, the power shifts of the resonance frequencies have been measured for n=35 to 42. The dependence of the fractional population transfer from the ndnd to (n+1)d(n-2)f states on the microwave field strength and atomic density has been measured and can be compared to a simple theoretical model. This work has been supported by the Air Force Office of Scientific Research.