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Physical Review A

Microwave pump-probe spectroscopy of the dipole-dipole interaction in a cold Rydberg gas

Hyunwook Park, Thomas F. Gallagher, P. Pillet

Published May 2, 2016• 11 citations
Publisher

Abstract

Microwave pump-probe experiments starting with a cold gas of Rb $34s$ atoms confirm that cusped line shapes observed in dipole-dipole broadened microwave transitions are due to atoms which are widely separated and exhibit small dipole-dipole energy shifts. When the experiments are interpreted in terms of a nearest-neighbor model, they demonstrate that it is possible to select pairs of atoms based on their separation and orientation.

DOI
10.1103/physreva.93.052501

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•Apr 27, 2016•0 citations
Microwave pump-probe experiments starting with a cold gas of Rb 34s34s34s atoms confirm that cusped line shapes observed in dipole-dipole broadened microwave transitions are due to atoms which are widely separated and exhibit small dipole-dipole energy shifts. When the experiments are interpreted in terms of a nearest-neighbor model, they demonstrate that it is possible to select pairs of atoms based on their separation and orientation.
The dipole-dipole broadening of $ns\ensuremath{-}np$ microwave transitions of cold Rb Rydberg atoms in a magneto-optical trap has been recorded for $28\ensuremath{\leqslant}n\ensuremath{\leqslant}51$. Since the electric dipole transition matrix elements scale as n2{n}^{2}n2, a broadening rate scaling as n4{n}^{4}n4 is expected and a broadening rate of $8.2\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}15}{n}^{4}$ MHz cm3{}^{3}3 is observed. The observed broadening is smaller than expected from a classical picture due to the spin-orbit interaction in the npnpnp atoms. The broadened resonances are asymmetric and cusp shaped, and their line shapes can be reproduced by a diatomic model which takes into account the dipole-dipole interaction, including the spin-orbit interaction, the strengths of the allowed microwave transitions, and the distribution of the atomic spacings in the trap.
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.
We have explored the dipole-dipole mediated, resonant energy transfer reaction, $32{p}_{3/2}+32{p}_{3/2}\ensuremath{\rightarrow}32s+33s$, in an ensemble of cold 85Rb^{85}\mathrm{Rb}85Rb Rydberg atoms. Stark tuning is employed to measure the population transfer probability as a function of the total electronic energy difference between the initial and final atom-pair states over a range of Rydberg densities, $2\ifmmode\times\else\texttimes\fi{}{10}^{8}\ensuremath{\le}\ensuremath{\rho}\ensuremath{\le}3\ifmmode\times\else\texttimes\fi{}{10}^{9} {\mathrm{cm}}^{\ensuremath{-}3}$. The observed line shapes provide information on the role of beyond nearest-neighbor interactions, the range of Rydberg atom separations, and the electric field inhomogeneity in the sample. The widths of the resonance line shapes increase approximately linearly with the Rydberg density and are only a factor of 2 larger than expected for two-body, nearest-neighbor interactions alone. These results are in agreement with the prediction [B. Sun and F. Robicheaux, Phys. Rev. A 78, 040701(R) (2008)] that beyond nearest-neighbor exchange interactions should not influence the population transfer process to the degree once thought. At low densities, Gaussian rather than Lorentzian line shapes are observed due to electric field inhomogeneities, allowing us to set an upper limit for the field variation across the Rydberg sample. At higher densities, non-Lorentzian, cusplike line shapes characterized by sharp central peaks and broad wings reflect the random distribution of interatomic distances within the magneto-optical trap (MOT). These line shapes are well reproduced by an analytic expression derived from a nearest-neighbor interaction model and may serve as a useful fingerprint for characterizing the position correlation function for atoms within the MOT.
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.
Electron dynamics in dipole-dipole (DD) coupled Rydberg atoms show some unique properties that do not exist in individual atoms.The goal of the research in this dissertation is to reveal and control the electron dynamics influenced by DD interaction in cold Rydberg gases.We have studied the decay of Rydberg excitations in a cold Rb gas and find no evidence for superradiance.The decay rates and population redistribution we observe are consistent with a model that considers only spontaneous emission from, and blackbody redistribution within, isolated atoms.Suppression of superradiant emission is likely due to variations in transition energies across the cold Rydberg atom sample.For initial s states, these variations are dominated by inhomogeneities in DD exchange interactions within the random ensemble.Such inhomogeneities will necessarily be present in any measurement involving a large number of atoms where the separation between atoms is not well defined.For initial p states, the suppression is likely due to a combination of DD exchange and electric field inhomogeneities.We have also explored the evolution of Rydberg wavepackets in the presence of strong dipole-dipole interactions in a frozen gas.The distribution of atom separations results in an inhomogeneity in the strength of the exchange coupling between neighboring atoms, causing a dephasing of the macroscopic coherence.We have also explored the mechanism of wavepacket coherence transfer from one Rydberg atom to a neighboring Rydberg atom via DD interactions utilizing the resonant DD coupling transition 25s33s↔24p34p.The phase-shift of the observed interference modulations in the 34p signal, relative to that in 25s, is a signature of wavepacket coherence transfer between atoms driven by electron correlations resulting from the controlled DD coupling between them.I would like to thank my advisor Professor Bob Jones for his guidance and help, not only in the detailed research performance but also in scientific ethics and methodology.He taught me how to operate most of the instruments as well as helped me fix failing apparatus.His rigorous, yet optimistic, working attitude always inspires me in my research.I don't remember how many times I have felt frustrated after getting nothing from a several days' experiment.At those times, I was always motivated and energetic from his guidance, constructive criticism and sincere encouragement, after even a short talk with him.The accomplishment of this dissertation involved a lot of his help, ranging from grammar checking, to language polishing, to error correction.I really feel grateful and fortunate to have worked with him for more than 5 years.Thanks also goes to my colleagues who have helped me in the research.Brian Richards worked with me a lot to fix failing instruments.He also programmed the data collection software.Sha Li taught me how to build setups to generate the THz radiation and build dye lasers.Kisra Nayomal Egodapitiya helped me adjust lasers and amplifiers many times.I also got invaluable inspiration from daily talks with them.