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Physical Review A

Millimeter-wave rubidium Rydberg van der Waals spectroscopy

Jianing Han, Thomas F. Gallagher

Published May 12, 2009• 34 citations
Publisher

Abstract

We have observed the diatomic $nsns\ensuremath{\rightarrow}ns(n+1)s\ensuremath{\rightarrow}(n+1)s(n+1)s$ microwave transitions of pairs of cold Rb Rydberg atoms for $36<n<48$. The $ns(n+1)s$ state has by far the largest van der Waals shift due to its near degeneracy with the nearby $n{p}_{3/2}n{p}_{3/2}$ state. In fact, the energy difference and the van der Waals shift change sign at $n=38$ and we observe shifts of both signs. The combined excitation of the $ns(n+1)s$ and $(n+1)s(n+1)s$ states leads to an unusual line shape which can be described by a three-level Floquet model.

DOI
10.1103/physreva.79.053409

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We have observed the diatomic nsns\ensuremath→ns(n+1)s\ensuremath→(n+1)s(n+1)snsns\ensuremath{\rightarrow}ns(n+1)s\ensuremath{\rightarrow}(n+1)s(n+1)snsns\ensuremath→ns(n+1)s\ensuremath→(n+1)s(n+1)s microwave transitions of pairs of cold Rb Rydberg atoms for 36<n<4836<n<4836<n<48. The ns(n+1)sns(n+1)sns(n+1)s state has by far the largest van der Waals shift due to its near degeneracy with the nearby np3/2np3/2n{p}_{3/2}n{p}_{3/2}np3/2​np3/2​ state. In fact, the energy difference and the van der Waals shift change sign at n=38n=38n=38 and we observe shifts of both signs. The combined excitation of the ns(n+1)sns(n+1)sns(n+1)s and (n+1)s(n+1)s(n+1)s(n+1)s(n+1)s(n+1)s states leads to an unusual line shape which can be described by a three-level Floquet model.
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 report on the observation of long range interaction in the second-harmonic generation from rubidium Rydberg atoms. The asymmetric spectral broadening of the resonant lines provides evidence of the van der Waals interaction between pairs of Rydberg atoms. This effect is investigated when the two-photon transition is resonant with ndndnd levels for $n\ensuremath{\approx}13$.
We have observed the ionization of a cold gas of Rb Rydberg atoms which occurs when nsnsnsnsnsns van der Waals pairs of nsnsns atoms of $n\ensuremath{\approx}$ 40 on a weakly repulsive potential are transferred to an attractive dipole-dipole nsnpnsnpnsnp potential by a microwave transition. Comparing the measurements to a simple model shows that the initial 300-$\ensuremath{\mu}$K thermal velocity of the atoms plays an important role. Excitation to a repulsive dipole-dipole potential does not lead to more ionization on a 15-$\ensuremath{\mu}$s time scale than leaving the atoms in the weakly repulsive nsnsnsnsnsns state. This observation is slightly surprising since a radiative transition must occur to allow ionization in the latter case. Finally, by power broadening of the microwave transition, to allow transitions from the initial nsnsnsnsnsns state to the nsnpnsnpnsnp state over a broad range of internuclear spacings, it is possible to accelerate markedly the evolution to a plasma.
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.