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Journal of Physics B Atomic Molecular and Optical Physics

Dipole–quadrupole Förster resonance in cesium Rydberg gas

W. Maineult, Bruno Pelle, Riccardo Faoro, E. Arimondo, P. Pillet, Patrick Cheinet

Published Oct 10, 2016• 15 citations
Publisher

Abstract

Abstract The resonant energy transfer between two close particles, also known as Förster resonance in atomic or biological systems, is usually associated with dipole–dipole interaction. In Rydberg atoms, it is a widely used tool to enhance the interactions between particles. Here, we observe a resonant energy transfer between Rydberg atoms that cannot be attributed to a dipole–dipole interaction, owing to selection rules, and comes instead from an efficient dipole–quadrupole process. We compare the measured probability transfer with a theoretical model including quadrupolar terms and find very good agreement with our measurement. Further studies of those multipolar resonances should probe their dependences on various parameters (quantum numbers, relative orientation of the atoms), and may find some applications in quantum procedures where dipole–dipole resonance cannot be used, for instance where the states of interest have a difference in angular momentum of two.

DOI
10.1088/0953-4075/49/21/214001

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The large electric dipole moments associated with transitions between Rydberg states of atoms or molecules, make them ideal model systems with which to study Förster resonance energy transfer in collisions with other Rydberg atoms or molecules, or with polar ground-state molecules [1,2]. The sensitivity of high Rydberg states to electric fields allows these energy transfer processes to be tuned thorough resonance by exploiting the Stark effect. In this talk, I will describe recent experiments in which we have observed the resonant transfer of energy from the ground-state inversion sublevels in ammonia, to helium atoms in triplet Rydberg states with principal quantum numbers between 38 and 43. The experiments were performed at translational temperatures below 1 K in seeded, pulsed supersonic beams [3]. Electric fields up to ~10 V/cm were used to tune transitions between selected Rydberg states into resonance with the transitions between the inversion sublevels. Resonant energy transfer was identified by Rydberg-state-selective electric-field ionisation. The experimental data exhibit quantum-state-dependent resonance widths that range from 200 to 700 MHz and, in general, reduce as the value of the principal quantum number is increased. Comparison with the results of numerical calculations of the Rydberg energy-level structure and transition moments, shows a dependence of the measured widths on the electric dipole transition moments of the Rydberg-Rydberg transitions. These results are of particular interest, e.g., for applications in coherent control and quantum sensing [4-6], and in the study of low-temperature ion-molecule reactions performed within the orbit of a Rydberg electron [7]. [1] T. F. Gallagher, Phys. Rep. 210, 319 (1992) [2] F. B. Dunning, S. Buathong, Int. Rev. Phys. Chem. 37, 287 (2018) [3] K. Gawlas and S. D. Hogan, J. Phys. Chem. Lett. 11, 83 (2020) [4] M. Zeppenfeld, Euro. Phys. Lett. 118, 13002 (2017). [5] E. Kuznetsova, S. T. Rittenhouse, H. R. Sadeghpour, and S. F. Yelin, Phys. Rev. A 94, 032325 (2016). [6] E. Kuznetsova, S. T. Rittenhouse, H. R. Sadeghpour, and S. F. Yelin, Phys. Chem. Chem. Phys. 13, 17115 (2011). [7] K. Höveler, J. Deiglmayr, J. A. Agner, H. Schmutz and F. Merkt, Phys. Chem. Chem. Phys. 23, 2676 (2021).

SPIE Nanophotonics•May 24, 2022•0 citations
Abstract The resonant energy transfer between two close particles, also known as Förster resonance in atomic or biological systems, is usually associated with dipole–dipole interaction. In Rydberg atoms, it is a widely used tool to enhance the interactions between particles. Here, we observe a resonant energy transfer between Rydberg atoms that cannot be attributed to a dipole–dipole interaction, owing to selection rules, and comes instead from an efficient dipole–quadrupole process. We compare the measured probability transfer with a theoretical model including quadrupolar terms and find very good agreement with our measurement. Further studies of those multipolar resonances should probe their dependences on various parameters (quantum numbers, relative orientation of the atoms), and may find some applications in quantum procedures where dipole–dipole resonance cannot be used, for instance where the states of interest have a difference in angular momentum of two.
Abstract Förster resonances provide a highly flexible tool to tune both the strength and the angular shape of interactions between two Rydberg atoms. We give a detailed explanation about how Förster resonances can be found by searching through a large range of possible quantum number combinations. We apply our search method to SS , SD and DD pair states of 87 Rb with principal quantum numbers from 30 to 100, taking into account the fine structure splitting of the Rydberg states. We find various strong resonances between atoms with a large difference in principal quantum numbers. We quantify the strength of these resonances by introducing a figure of merit C ˜ 3 which is independent of the magnetic quantum numbers and geometry to classify the resonances by interaction strength. We further predict to what extent excitation exchange is possible on different resonances and point out limitations of the coherent hopping process. Finally, we discuss the angular dependence of the dipole–dipole interaction and its tunability near resonances.
Cold Rydberg atoms are known to display dipole-dipole interaction-allowed resonances, also called F\"orster resonances, which lead to an efficient energy transfer when the proper electric field is used. This electric field also enables resonances, which do not respect the dipole-dipole selection rules under zero field. A few of these quasiforbidden resonances have been observed but they are often overlooked. Here we show that in cold 133Cs^{133}\mathrm{Cs}133Cs atoms there is a large number of these resonances that display a significant transfer efficiency due to their strong interactions, even at low electric field. We also develop a graphical method enabling us to find all possible resonances simultaneously. The resulting dramatic increase in the total number of addressable resonant energy transfers at different electric fields could have implications in the search for few-body interactions or macromolecules built from Rydberg atoms.
High resolution laser excitation of np Rydberg states of cesium atoms shows a dipole blockade at Förster resonances corresponding to the resonant dipole-dipole energy transfer of the np + np → ns + (n + 1)s reaction. The dipole-dipole interaction can be tuned on and off by the Stark effect, and such a process observed for relatively low n (25 − 41) is promising for quantum gate devices. Both Penning ionization and saturation in the laser excitation can limit the range of observation of the dipole blockade
Cold Rydberg atoms subject to long-range dipole-dipole interactions represent a particularly interesting system for exploring few-body interactions and probing the transition from 2-body physics to the many-body regime. In this work we report the direct observation of a resonant 4-body Rydberg interaction. We exploit the occurrence of an accidental quasicoincidence of a 2-body and a 4-body resonant Stark-tuned Förster process in cesium to observe a resonant energy transfer requiring the simultaneous interaction of at least four neighboring atoms. These results are relevant for the implementation of quantum gates with Rydberg atoms and for further studies of many-body physics.
High resolution laser excitation of np Rydberg states of cesium atoms shows a dipole blockade at Förster resonances corresponding to the resonant dipole-dipole energy transfer of the np+np --> ns+(n+1)s reaction. The dipole-dipole interaction can be tuned on and off by the Stark effect, and such a process, observed for relatively low n(25-41), is promising for quantum gate devices. Both Penning ionization and saturation in the laser excitation can limit the range of observation of the dipole blockade.
The large electric dipole moments associated with transitions between Rydberg states of atoms or molecules, make them ideal model systems with which to study Förster resonance energy transfer in collisions with other Rydberg atoms or molecules, or with polar ground-state molecules [1,2]. The sensitivity of high Rydberg states to electric fields allows these energy transfer processes to be tuned thorough resonance by exploiting the Stark effect. In this talk, I will describe recent experiments in which we have observed the resonant transfer of energy from the ground-state inversion sublevels in ammonia, to helium atoms in triplet Rydberg states with principal quantum numbers between 38 and 43. The experiments were performed at translational temperatures below 1 K in seeded, pulsed supersonic beams [3]. Electric fields up to ~10 V/cm were used to tune transitions between selected Rydberg states into resonance with the transitions between the inversion sublevels. Resonant energy transfer was identified by Rydberg-state-selective electric-field ionisation. The experimental data exhibit quantum-state-dependent resonance widths that range from 200 to 700 MHz and, in general, reduce as the value of the principal quantum number is increased. Comparison with the results of numerical calculations of the Rydberg energy-level structure and transition moments, shows a dependence of the measured widths on the electric dipole transition moments of the Rydberg-Rydberg transitions. These results are of particular interest, e.g., for applications in coherent control and quantum sensing [4-6], and in the study of low-temperature ion-molecule reactions performed within the orbit of a Rydberg electron [7]. [1] T. F. Gallagher, Phys. Rep. 210, 319 (1992) [2] F. B. Dunning, S. Buathong, Int. Rev. Phys. Chem. 37, 287 (2018) [3] K. Gawlas and S. D. Hogan, J. Phys. Chem. Lett. 11, 83 (2020) [4] M. Zeppenfeld, Euro. Phys. Lett. 118, 13002 (2017). [5] E. Kuznetsova, S. T. Rittenhouse, H. R. Sadeghpour, and S. F. Yelin, Phys. Rev. A 94, 032325 (2016). [6] E. Kuznetsova, S. T. Rittenhouse, H. R. Sadeghpour, and S. F. Yelin, Phys. Chem. Chem. Phys. 13, 17115 (2011). [7] K. Höveler, J. Deiglmayr, J. A. Agner, H. Schmutz and F. Merkt, Phys. Chem. Chem. Phys. 23, 2676 (2021).