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Physical Review Letters

Probing Electronic Coherence in a Gas of Dipole-Dipole Coupled Rydberg Atoms

Mary R. Kutteruf, R. R. Jones

Published Jan 3, 2012• 14 citations
Publisher

Abstract

We demonstrate a novel time-domain method to probe electronic coherence in ensembles of cold Rydberg atoms coupled via nearly resonant dipole-dipole interactions. Short laser pulses create coherent superpositions of few-electron eigenstates which evolve under the influence of pulsed electric fields. The pulses steer the dynamics, enhancing the probability for finding atoms in np, rather than initially excited ns states. The enhancement reflects the underlying electronic coherence which persists for >10 μs, 2 orders of magnitude longer than previously measured dephasing times in the same system. Simulations suggest that atom motion is responsible for the eventual decoherence.

DOI
10.1103/physrevlett.108.013001

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Resonant electric dipole-dipole interactions between cold Rydberg atoms were observed using microwave spectroscopy. Laser-cooled 85Rb atoms in a magneto-optical trap were optically excited to 45d(5/2) Rydberg states using a pulsed laser. A microwave pulse transferred a fraction of these Rydberg atoms to the 46p(3/2) state. A second microwave pulse then drove atoms in the 45d(5/2) state to the 46d(5/2) state, and was used as a probe of interatomic interactions. The spectral width of this two-photon probe transition was found to depend on the presence of the 46p(3/2) atoms, and is due to the resonant electric dipole-dipole interaction between 45d(5/2) and 46p(3/2) Rydberg atoms.

arXiv:physics/0411076•Physical Review Letters•Nov 30, 2004•126 citations
We demonstrate a novel time-domain method to probe electronic coherence in ensembles of cold Rydberg atoms coupled via nearly resonant dipole-dipole interactions. Short laser pulses create coherent superpositions of few-electron eigenstates which evolve under the influence of pulsed electric fields. The pulses steer the dynamics, enhancing the probability for finding atoms in np, rather than initially excited ns states. The enhancement reflects the underlying electronic coherence which persists for >10 μs, 2 orders of magnitude longer than previously measured dephasing times in the same system. Simulations suggest that atom motion is responsible for the eventual decoherence.
We have studied the evolution of Rydberg wave packets in the presence of interatomic dipole-dipole interactions in a frozen Rb gas. Rb atoms in a magneto-optical trap (MOT) are first laser excited to nsnsns Rydberg eigenstates. A picosecond THz pulse further excites them into coherent superposition states involving the initial-level and neighboring npnpnp states. A second, identical, time-delayed THz pulse probes the wave-packet dynamics. As the wave packets evolve they are influenced by dipole-dipole interactions, predominantly pairwise excitation-exchange processes of the form $|s\ensuremath{\rangle}|p\ensuremath{\rangle}\ensuremath{\leftrightarrow}|p\ensuremath{\rangle}|s\ensuremath{\rangle}$. The coherent electronic evolution of the ensemble dephases due to the variation in dipole-dipole coupling strength between atom pairs in the MOT. The experimental results are in good agreement with numerical calculations that simulate the interactions between nearest neighbors in a frozen gas.
Coupling by the resonant dipole-dipole energy transfer between cold cesium Rydberg atoms is investigated using time-resolved narrow-band de-excitation spectroscopy. This technique combines the advantage of efficient Rydberg excitation with high-resolution spectroscopy at variable interaction times. The coherent character of the process is studied by back and forth transfer in the np+np <--> ns+(n+1)s reaction. The evolution of coherence is mostly due to the motion between the atoms induced by the dipole-dipole interaction. Dipole-dipole interaction is observed spectroscopically as avoided level crossing.
Coupling by the resonant dipole-dipole energy transfer between cold cesium Rydberg atoms is investigated using time-resolved narrow-band deexcitation spectroscopy. This technique combines the advantage of efficient Rydberg excitation with high-resolution spectroscopy at variable interaction times. Dipole-dipole interaction is observed spectroscopically as avoided level crossing. The coherent character of the process is linked to back and forth transfer in the np + np <--> ns + (n + 1)s reaction. Decoherence in the ensemble has two different origins: the atom motion induced by dipole-dipole interaction and the migration of the s-Rydberg excitation in the environment of p-Rydberg atoms.
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.
Resonant electric dipole-dipole interactions between cold Rydberg atoms were observed using microwave spectroscopy. Laser-cooled 85Rb atoms in a magneto-optical trap were optically excited to 45d(5/2) Rydberg states using a pulsed laser. A microwave pulse transferred a fraction of these Rydberg atoms to the 46p(3/2) state. A second microwave pulse then drove atoms in the 45d(5/2) state to the 46d(5/2) state, and was used as a probe of interatomic interactions. The spectral width of this two-photon probe transition was found to depend on the presence of the 46p(3/2) atoms, and is due to the resonant electric dipole-dipole interaction between 45d(5/2) and 46p(3/2) Rydberg atoms.