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Resonant Dipole-Dipole Energy Transfer Dynamics in a Frozen Rydberg Gas

Donald P. Fahey

Published Jan 1, 2014• 0 citations
OpenAlex

Abstract

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.

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Dipole-dipole interaction between rubidium Rydberg atoms

Emily Altiere, Donald P. Fahey, Michael W. Noel +2 more

Ultracold Rydberg atoms in a static electric field can exchange energy via the dipole-dipole interaction. The Stark effect shifts the energy levels of the atoms which tunes the energy exchange into resonance at specific values of the electric field (F\"orster resonances). We excite rubidium atoms to Rydberg states by focusing either a 480 nm beam from a tunable dye laser or a pair of diode lasers into a magneto-optical trap. The trap lies at the center of a configuration of electrodes. We scan the electric field by controlling the voltage on the electrodes while measuring the fraction of atoms that interact. Dipole-dipole interaction spectra are presented for initially excited rubidium $nd$ states for $n=31$ to 46 and for four different pairs of initially excited rubidium $ns$ states. We also present the dipole-dipole interaction spectra for individual rubidium 32$d$ $(j,\phantom{\rule{0.16em}{0ex}}{m}_{j})$ fine structure levels that have been selectively excited. The data are compared to calculated spectra.

Physical Review A•Nov 28, 2011•26 citations

Imaging the dipole-dipole energy exchange between ultracold rubidium Rydberg atoms

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The long-range, anisotropic nature of the interaction among atoms in an ultracold dipolar gas leads to a rich array of possibilities for studying many-body physics. In this work, an ultracold gas of highly excited atoms is used to study energy transport due to the long-range dipole-dipole interaction. A technique is developed to measure both the internal energy states of the interacting Rydberg atoms and their positions in space. This technique is demonstrated by observing energy exchange between two spatially separated groups of Rydberg atoms excited to two different internal states. Simulations confirm the general features of the energy transport in this system and highlight subtleties associated with the homogeneity of the electric field used in this experiment.

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We measure the transport of energy among the internal states of ultracold rubidium Rydberg atoms coupled by dipole-dipole exchange. In a magneto-optical trap, a static electric field of a few V/cm shifts the energy levels of the atoms. For a particular principal quantum number, $n$, the angular momentum eigenstates $\ell > 4$ are nearly degenerate at zero electric field. At nonzero field, a manifold of equally spaced clusters form a ladder with each rung consisting of a set of closely spaced $m$ energy eigenstates. We excite Rydberg atoms to energy levels near the center of the manifold and allow them to exchange energy via resonant dipole-dipole interactions. We measure the time evolution as energy spreads away from the center of the manifold, which reveals that the system may fail to thermalize for long interaction times. A computational model that includes only a few essential features of the system qualitatively agrees with this result.

arXiv:2407.21764•Jul 31, 2024•0 citations

Rydberg-wave-packet evolution in a frozen gas of dipole-dipole-coupled atoms

Tao Zhou, Sha Li, R. R. Jones

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 $ns$ Rydberg eigenstates. A picosecond THz pulse further excites them into coherent superposition states involving the initial-level and neighboring $np$ 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.

Physical Review A•Jun 16, 2014•7 citations

Influence of Dipole-Dipole Interaction on Electron Dynamics in a Cold Rydberg Gas

Tao Zhou

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.

•Apr 27, 2016•0 citations

Spatial and temporal correlations in cold Rydberg gases

Markus Stecker

Rydberg atoms, i.e. atoms with one or more highly excited electrons, show exaggerated properties compared to ground state atoms. For example, their energy levels are very sensitive to external electric fields (Stark effect) and they exhibit strong interatomic interactions, which can lead to a suppression of excitation known as the Rydberg blockade. The latter property makes Rydberg atoms promising candidates for quantum simulation and quantum computing. This work describes the direct observation of the excitation blockade for highly Stark-shifted Rydberg atoms induced by controllable dipole-dipole interactions. We investigate the electric field region around and above the classical ionization threshold, which is typically not considered suitable for blockade experiments. We excite Rydberg atoms in the energy region corresponding to the unperturbed 43S1/2 state at electric fields around 127V/cm out of a magneto-optically trapped cloud of 87Rb atoms with a temperature of 150 μK. We tune the dipole-dipole interaction by the applied electric field thus changing the electric dipole moment of the excited state. The position of the Rydberg atoms is detected by ionization and subsequent ion imaging; the controlled ionization of the atoms is achieved by adiabatic transfer of the Rydberg state to an ionizing state. For the spatially resolved detection of the atoms, a high resolution ion microscope for cold atoms has been developed and experimentally characterized. It features a maximum magnification of 1000 and sub-micrometer spatial resolution. A theoretical treatment of highly Stark-shifted Rydberg states is developed introducing a complex absorbing potential. It is capable of predicting the ionization rates of the Rydberg states for a wide range of electric fields and energies with only one free parameter. Together with the numerical calculations, measurements of the ionization spectra for different Rydberg states are presented. The 43S1/2 state is measured in an electric-field range from 125V/cm to 165V/cm (classical ionization limit 127V/cm), the 70S1/2 state in an electric-field range from 15V/cm to 35V/cm (classical ionization limit 16.1V/cm) and the 100S1/2 state in an electric-field range from 7V/cm to 19V/cm (classical ionization limit 3.7V/cm). Our results show an intricate energy level structure with broad, strongly ionizing states as well as sharp, nearly non-ionizing states. The numerical calculations are also used for the prediction of selective field ionization spectra and the results are used to identify Förster resonances in the Stark spectrum of the 45D5/2 state. Complementary to the spatially resolved measurements in high electric fields, the Rydberg blockade effect is also observed via the excitation number statistics at Förster resonances.

•Jan 1, 2018•0 citations
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.
Ultracold Rydberg atoms in a static electric field can exchange energy via the dipole-dipole interaction. The Stark effect shifts the energy levels of the atoms which tunes the energy exchange into resonance at specific values of the electric field (F\"orster resonances). We excite rubidium atoms to Rydberg states by focusing either a 480 nm beam from a tunable dye laser or a pair of diode lasers into a magneto-optical trap. The trap lies at the center of a configuration of electrodes. We scan the electric field by controlling the voltage on the electrodes while measuring the fraction of atoms that interact. Dipole-dipole interaction spectra are presented for initially excited rubidium ndndnd states for n=31n=31n=31 to 46 and for four different pairs of initially excited rubidium nsnsns states. We also present the dipole-dipole interaction spectra for individual rubidium 32ddd (j,mj)(j,\phantom{\rule{0.16em}{0ex}}{m}_{j})(j,mj​) fine structure levels that have been selectively excited. The data are compared to calculated spectra.
The long-range, anisotropic nature of the interaction among atoms in an ultracold dipolar gas leads to a rich array of possibilities for studying many-body physics. In this work, an ultracold gas of highly excited atoms is used to study energy transport due to the long-range dipole-dipole interaction. A technique is developed to measure both the internal energy states of the interacting Rydberg atoms and their positions in space. This technique is demonstrated by observing energy exchange between two spatially separated groups of Rydberg atoms excited to two different internal states. Simulations confirm the general features of the energy transport in this system and highlight subtleties associated with the homogeneity of the electric field used in this experiment.
We measure the transport of energy among the internal states of ultracold rubidium Rydberg atoms coupled by dipole-dipole exchange. In a magneto-optical trap, a static electric field of a few V/cm shifts the energy levels of the atoms. For a particular principal quantum number, nnn, the angular momentum eigenstates ℓ>4\ell > 4ℓ>4 are nearly degenerate at zero electric field. At nonzero field, a manifold of equally spaced clusters form a ladder with each rung consisting of a set of closely spaced mmm energy eigenstates. We excite Rydberg atoms to energy levels near the center of the manifold and allow them to exchange energy via resonant dipole-dipole interactions. We measure the time evolution as energy spreads away from the center of the manifold, which reveals that the system may fail to thermalize for long interaction times. A computational model that includes only a few essential features of the system qualitatively agrees with this result.
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.
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.
Rydberg atoms, i.e. atoms with one or more highly excited electrons, show exaggerated properties compared to ground state atoms. For example, their energy levels are very sensitive to external electric fields (Stark effect) and they exhibit strong interatomic interactions, which can lead to a suppression of excitation known as the Rydberg blockade. The latter property makes Rydberg atoms promising candidates for quantum simulation and quantum computing. This work describes the direct observation of the excitation blockade for highly Stark-shifted Rydberg atoms induced by controllable dipole-dipole interactions. We investigate the electric field region around and above the classical ionization threshold, which is typically not considered suitable for blockade experiments. We excite Rydberg atoms in the energy region corresponding to the unperturbed 43S1/2 state at electric fields around 127V/cm out of a magneto-optically trapped cloud of 87Rb atoms with a temperature of 150 μK. We tune the dipole-dipole interaction by the applied electric field thus changing the electric dipole moment of the excited state. The position of the Rydberg atoms is detected by ionization and subsequent ion imaging; the controlled ionization of the atoms is achieved by adiabatic transfer of the Rydberg state to an ionizing state. For the spatially resolved detection of the atoms, a high resolution ion microscope for cold atoms has been developed and experimentally characterized. It features a maximum magnification of 1000 and sub-micrometer spatial resolution. A theoretical treatment of highly Stark-shifted Rydberg states is developed introducing a complex absorbing potential. It is capable of predicting the ionization rates of the Rydberg states for a wide range of electric fields and energies with only one free parameter. Together with the numerical calculations, measurements of the ionization spectra for different Rydberg states are presented. The 43S1/2 state is measured in an electric-field range from 125V/cm to 165V/cm (classical ionization limit 127V/cm), the 70S1/2 state in an electric-field range from 15V/cm to 35V/cm (classical ionization limit 16.1V/cm) and the 100S1/2 state in an electric-field range from 7V/cm to 19V/cm (classical ionization limit 3.7V/cm). Our results show an intricate energy level structure with broad, strongly ionizing states as well as sharp, nearly non-ionizing states. The numerical calculations are also used for the prediction of selective field ionization spectra and the results are used to identify Förster resonances in the Stark spectrum of the 45D5/2 state. Complementary to the spatially resolved measurements in high electric fields, the Rydberg blockade effect is also observed via the excitation number statistics at Förster resonances.