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Physical Review A

Dephasing of resonant energy transfer in a cold Rydberg gas

W. R. Anderson, Michael Robinson, J. D. D. Martin, Thomas F. Gallagher

Published Jun 5, 2002• 78 citations
Publisher

Abstract

When the dipole-dipole energy transfer, $\mathrm{Rb} {25s}_{1/2}+\mathrm{Rb} {33s}_{1/2}\ensuremath{\rightarrow}\mathrm{Rb} {24p}_{1/2}+\mathrm{Rb} {34p}_{3/2},$ resonant at fields of 3.0 and 3.4 V/cm, is observed in a cold Rydberg gas, the resonances are broader than expected for this dipole-dipole interaction alone. Using a variant of the Ramsey interference method, in which the system is detuned from the resonance, we observe a density-dependent dephasing which we attribute to the inhomogeneities in the always resonant dipole-dipole excitation exchange interactions $\mathrm{Rb} {25s}_{1/2}+\mathrm{Rb} {24p}_{1/2}\ensuremath{\rightarrow}\mathrm{Rb} {24p}_{1/2}+\mathrm{Rb} {25s}_{1/2}$ and $\mathrm{Rb} {33s}_{1/2}+\mathrm{Rb} {34p}_{3/2}\ensuremath{\rightarrow}\mathrm{Rb} {34p}_{3/2}+\mathrm{Rb} {33s}_{1/2}.$ Since the dephasing rate is comparable to the observed widths, it appears that all of these interactions contribute to the observed linewidths.

DOI
10.1103/physreva.65.063404

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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.
The dipole-dipole interaction strongly couples ultracold highly excited atoms, known as Rydberg atoms, and is the dominant mechanism for energy exchange among such atoms on microsecond time scales. I present the results of experiments that investigate this interaction using rubidium atoms excited to Rydberg states with an all-diode laser system. In the first of these, high resolution dipole-dipole interaction spectra for different magnetic sublevels of the 32d5/2 state are collected and analyzed. In the second experiment, ultracold rubidium atoms are implusively excited to coherent superpositions of three closely spaced |mj|sublevels of the 32d5/2 state in a weak electric field. The magnitude of the field sets the energy level spacing between these states, and hence the frequency of the phase dependent oscillations resulting from interference in resonant energy exchange processes. In the third experiment, the dipole-dipole interaction induced resonant energy exchange between columns of ultracold rubidium Rydberg atoms is imaged using a new technique involving selective field ionization with a spatially sensitive ion detector.
We have studied the decay of Rydberg excitations in a cold Rb gas. A 10 ns, pulsed-dye-amplified diode laser excites Rb atoms at $70\phantom{\rule{0.28em}{0ex}}\ensuremath{\mu}\mathrm{K}$ in a magneto-optical trap to nsnsns or npnpnp Rydberg states with principal quantum numbers $26\ensuremath{\le}n\ensuremath{\le}40$. Time-delayed state-selective field ionization is used to directly monitor the population in the initial and neighboring Rydberg levels. The measured time dependence of the Rydberg population is well described by numerical simulations which consider only spontaneous emission and population transfer by blackbody radiation. No evidence for collective decay is found at atom densities up to $3\ifmmode\times\else\texttimes\fi{}{10}^{9}\phantom{\rule{0.16em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$. This result is in contrast to a previous study [Wang et al., Phys. Rev. A 75, 033802 (2007)], in which superradiant decay was theoretically predicted and experimentally inferred for atom density and laser focal volume conditions very similar to those considered here. Suppression of collective emission is likely due to variations in transition energies within the atom sample, dominated by inhomogeneities in dipole-dipole exchange interactions for initial sss states, or by a combination of dipole-dipole and electric field inhomogeneities for the initial ppp states.
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.
Previous resonant dipole-dipole energy-transfer experiments of cold Rydberg gases [Anderson et al., Phys. Rev. Lett. 80, 249 (1998); Mourachko et al., Phys. Rev. Lett. 80, 253 (1998)] have been interpreted as providing evidence of many-body, as opposed to purely binary, effects. Here we separate two-body and many-body interactions by introducing an additional Rydberg state, which does not participate directly in the energy-transfer process, but is strongly coupled to one of the final states. We observe broadening of the energy-transfer resonances due to this added Rydberg state, which clearly demonstrates the many-body nature of the dipole-dipole interactions in such a system.