Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

arXiv:1705.01487 · Physical Review A

Electrically tuned Förster resonances in collisions of NH3 with Rydberg He atoms

Valentina Zhelyazkova, S. D. Hogan

Published Apr 21, 2017• 26 citations
arXivHTMLPDF

Abstract

The effects of weak electric fields on resonant energy transfer between ${\mathrm{NH}}_{3}$ in the $X$ ${^{1}A}_{1}$ ground electronic state and Rydberg He atoms in triplet states with principal quantum numbers $n=36$--41 have been studied in a crossed-beam apparatus. For these values of $n$, electric dipole transitions between the Rydberg states that evolve adiabatically to the $|ns\ensuremath{\rangle}$ and $|np\ensuremath{\rangle}$ states in zero electric field can be tuned into resonance with the ground-state inversion transitions in ${\mathrm{NH}}_{3}$ using electric fields, with energy transfer occurring via F\"orster resonance. In the experiments the Rydberg He atoms, traveling in pulsed supersonic beams, were prepared by resonant two-photon excitation from the metastable $1s2s\phantom{\rule{0.16em}{0ex}}{^{3}S}_{1}$ level and crossed an effusive beam of ${\mathrm{NH}}_{3}$ before being detected by state-selective pulsed-electric-field ionization. The resonant-energy-transfer process was identified by monitoring changes in the ionization signal from the $|ns\ensuremath{\rangle}$ and $|np\ensuremath{\rangle}$ Rydberg states for each value of $n$. The electric-field dependence of the experimental data is in good agreement with the results of calculations in which the resonant dipole-dipole coupling between the collision partners was accounted for.

DOI
10.1103/physreva.95.042710

Related papers

Rydberg-State-Resolved Resonant Energy Transfer in Cold Electric-Field-Controlled Intrabeam Collisions of NH3 with Rydberg He Atoms

K. Gawlas, S. D. Hogan

The resonant transfer of energy from the inversion sublevels in NH 3 to He atoms in triplet Rydberg states with principal quantum number n = 38 has been controlled using electric fields below 15 V/cm in intrabeam collisions at translational temperatures of ∼1 K. The experiments were performed in pulsed supersonic beams of NH 3 seeded in He at a ratio of 1:19. The He atoms were prepared in the metastable 1s2s 3 S 1 level in a pulsed electric discharge in the trailing part of the beams. The velocity slip between the heavy NH 3 and the lighter metastable He was exploited to perform collision studies at center-of-mass collision speeds of ∼70 m/s. Resonant energy transfer in the atom–molecule collisions was identified by Rydberg-state-selective electric-field ionization. The experimental data have been compared to a theoretical model of the resonant dipole–dipole interactions between the collision partners based on the impact parameter method.

arXiv:2001.08440•The Journal of Physical Chemistry Letters•Dec 10, 2019•20 citations

Electric-field-controlled resonant energy transfer between polar ground-state molecules and highly-excited Rydberg atoms

S. D. Hogan

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

Probing van der Waals interactions and detecting polar molecules by Förster-resonance energy transfer with Rydberg atoms at temperatures below 100 mK

Junwen Zou, S. D. Hogan

Electric-field-controlled F\"orster-resonance energy transfer (FRET) between Rydberg helium (He) atoms and ground-state ammonia (${\mathrm{NH}}_{3}$) molecules has been studied at translational temperatures below 100 mK. The experiments were performed in an intrabeam collision apparatus with pulsed supersonic beams of ${\mathrm{NH}}_{3}$ seeded in He. A range of F\"orster resonances, between triplet Rydberg states in He with principal quantum numbers of 38, 39, and 40, and the inversion intervals in ${\mathrm{NH}}_{3}$ were investigated. Resonance widths as low as $100\ifmmode\pm\else\textpm\fi{}20$ MHz were observed for Rydberg-Rydberg transitions with electric dipole transition moments of 3270 D. These widths result from binary collisions at a mean center-of-mass speed of $19.3\ifmmode\pm\else\textpm\fi{}2.6$ m/s. For transitions in which the initially prepared Rydberg states were strongly polarized, with large induced static electric dipole moments, van der Waals interactions between the collision partners increased the resonance widths to $\ensuremath{\sim}750$ MHz. From measurements of the rate of FRET for the narrowest resonances observed, a density of ${\mathrm{NH}}_{3}$ of $(9.4\ifmmode\pm\else\textpm\fi{}0.3)\ifmmode\times\else\texttimes\fi{}{10}^{9}\phantom{\rule{0.28em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$ in the upper ground-state inversion sublevel in the interaction region of the apparatus was determined nondestructively.

arXiv:2211.09880•Physical Review A•Oct 20, 2022•3 citations

Probing resonant energy transfer in collisions of ammonia with Rydberg helium atoms by microwave spectroscopy

Valentina Zhelyazkova, S. D. Hogan

We present the results of experiments demonstrating the spectroscopic detection of Förster resonance energy transfer from NH3 in the X1A1 ground electronic state to helium atoms in 1sns 3S1 Rydberg levels, where n = 37 and n = 40. For these values of n, the 1sns 3S1 → 1snp 3PJ transitions in helium lie close to resonance with the ground-state inversion transitions in NH3 and can be tuned through resonance using electric fields of less than 10 V/cm. In the experiments, energy transfer was detected by direct state-selective electric field ionization of the 3S1 and 3PJ Rydberg levels and by monitoring the population of the 3DJ levels following pulsed microwave transfer from the 3PJ levels. Detection by microwave spectroscopic methods represents a highly state selective, low-background approach to probing the collisional energy transfer process and the environment in which the atom-molecule interactions occur. The experimentally observed electric-field dependence of the resonant energy transfer process, probed both by direct electric field ionization and by microwave transfer, agrees well with the results of calculations performed using a simple theoretical model of the energy transfer process. For measurements performed in zero electric field with atoms prepared in the 1s40s 3S1 level, the transition from a regime in which a single energy transfer channel can be isolated for detection to one in which multiple collision channels begin to play a role has been identified as the NH3 density was increased.

arXiv:1801.01390•The Journal of Chemical Physics•Dec 26, 2017•11 citations

Electric Field Tuned Dipolar Interaction Between Rydberg Atoms

Yuechun Jiao, Jingxu Bai, Rong Song +3 more

We demonstrated a tuned dipole interaction between Rydberg atoms by employing a controllable electric field in a cold cesium ensemble. The | n P 3/2 ⟩ ( n = 38–40) Rydberg pairs are prepared with a three-photon scheme and detected via the state-selective field ionization technique. A weak DC electric field is used to tune the Rydberg pair interaction from the van der Waals interaction regime to the dipole–dipole interaction regime. The Förster resonant interaction and an adiabatic resonance energy transfer between the n P and n S Rydberg states are attained by precisely tuning the electric field. Rydberg excitation blockade with and without the electric field is investigated by changing the excitation pulse duration, which demonstrates that the dipole interaction–induced blockade effect is stronger than the van der Waals interaction–induced blockade effect. The precise control of the Rydberg interaction is of great significance to the coherent interaction in many-body systems and non-radiative collision processes.

Frontiers in Physics•Apr 27, 2022•8 citations

Resonant collisions of K Rydberg atoms

Michael J. Renn, Wayne A. Anderson, James Veale +1 more

We have studied the collisional energy transfer process K (ns) +K (n-2) d {yields} K (np) +K (n-1) p which is tuned into resonance with an applied static electric field. The initial Rydberg states are excited stepwise with two dye laser pulses. The resonant energy transfer is detected by selectively field ionizing the final K(np) state as the static field is swept over many laser shots. Due to fine structure splitting of the d and p levels 45 resonances are energetically allowed at n{sub s}=25. The actual number of resonances that are observed depends on the polarization of the laser light, the dipole-dipole selection rules, and the n state excited. Above n{sub s}=29 all resonances are energically forbidden. We have measured the position of the resonances in electric field from n{sub s}=25 to n{sub s}=29 and found them to be in good agreement with calculated positions.

Bulletin of the American Physical Society•May 1, 1993•0 citations
The effects of weak electric fields on resonant energy transfer between NH3{\mathrm{NH}}_{3}NH3​ in the XXX 1A1{^{1}A}_{1}1A1​ ground electronic state and Rydberg He atoms in triplet states with principal quantum numbers n=36n=36n=36--41 have been studied in a crossed-beam apparatus. For these values of nnn, electric dipole transitions between the Rydberg states that evolve adiabatically to the ∣ns\ensuremath⟩|ns\ensuremath{\rangle}∣ns\ensuremath⟩ and ∣np\ensuremath⟩|np\ensuremath{\rangle}∣np\ensuremath⟩ states in zero electric field can be tuned into resonance with the ground-state inversion transitions in NH3{\mathrm{NH}}_{3}NH3​ using electric fields, with energy transfer occurring via F"orster resonance. In the experiments the Rydberg He atoms, traveling in pulsed supersonic beams, were prepared by resonant two-photon excitation from the metastable 1s2s3S11s2s\phantom{\rule{0.16em}{0ex}}{^{3}S}_{1}1s2s3S1​ level and crossed an effusive beam of NH3{\mathrm{NH}}_{3}NH3​ before being detected by state-selective pulsed-electric-field ionization. The resonant-energy-transfer process was identified by monitoring changes in the ionization signal from the ∣ns\ensuremath⟩|ns\ensuremath{\rangle}∣ns\ensuremath⟩ and ∣np\ensuremath⟩|np\ensuremath{\rangle}∣np\ensuremath⟩ Rydberg states for each value of nnn. The electric-field dependence of the experimental data is in good agreement with the results of calculations in which the resonant dipole-dipole coupling between the collision partners was accounted for.
The resonant transfer of energy from the inversion sublevels in NH 3 to He atoms in triplet Rydberg states with principal quantum number n = 38 has been controlled using electric fields below 15 V/cm in intrabeam collisions at translational temperatures of ∼1 K. The experiments were performed in pulsed supersonic beams of NH 3 seeded in He at a ratio of 1:19. The He atoms were prepared in the metastable 1s2s 3 S 1 level in a pulsed electric discharge in the trailing part of the beams. The velocity slip between the heavy NH 3 and the lighter metastable He was exploited to perform collision studies at center-of-mass collision speeds of ∼70 m/s. Resonant energy transfer in the atom–molecule collisions was identified by Rydberg-state-selective electric-field ionization. The experimental data have been compared to a theoretical model of the resonant dipole–dipole interactions between the collision partners based on the impact parameter method.
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).
Electric-field-controlled F\"orster-resonance energy transfer (FRET) between Rydberg helium (He) atoms and ground-state ammonia (NH3{\mathrm{NH}}_{3}NH3​) molecules has been studied at translational temperatures below 100 mK. The experiments were performed in an intrabeam collision apparatus with pulsed supersonic beams of NH3{\mathrm{NH}}_{3}NH3​ seeded in He. A range of F\"orster resonances, between triplet Rydberg states in He with principal quantum numbers of 38, 39, and 40, and the inversion intervals in NH3{\mathrm{NH}}_{3}NH3​ were investigated. Resonance widths as low as $100\ifmmode\pm\else\textpm\fi{}20$ MHz were observed for Rydberg-Rydberg transitions with electric dipole transition moments of 3270 D. These widths result from binary collisions at a mean center-of-mass speed of $19.3\ifmmode\pm\else\textpm\fi{}2.6$ m/s. For transitions in which the initially prepared Rydberg states were strongly polarized, with large induced static electric dipole moments, van der Waals interactions between the collision partners increased the resonance widths to $\ensuremath{\sim}750$ MHz. From measurements of the rate of FRET for the narrowest resonances observed, a density of NH3{\mathrm{NH}}_{3}NH3​ of $(9.4\ifmmode\pm\else\textpm\fi{}0.3)\ifmmode\times\else\texttimes\fi{}{10}^{9}\phantom{\rule{0.28em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$ in the upper ground-state inversion sublevel in the interaction region of the apparatus was determined nondestructively.
We present the results of experiments demonstrating the spectroscopic detection of Förster resonance energy transfer from NH3 in the X1A1 ground electronic state to helium atoms in 1sns 3S1 Rydberg levels, where n = 37 and n = 40. For these values of n, the 1sns 3S1 → 1snp 3PJ transitions in helium lie close to resonance with the ground-state inversion transitions in NH3 and can be tuned through resonance using electric fields of less than 10 V/cm. In the experiments, energy transfer was detected by direct state-selective electric field ionization of the 3S1 and 3PJ Rydberg levels and by monitoring the population of the 3DJ levels following pulsed microwave transfer from the 3PJ levels. Detection by microwave spectroscopic methods represents a highly state selective, low-background approach to probing the collisional energy transfer process and the environment in which the atom-molecule interactions occur. The experimentally observed electric-field dependence of the resonant energy transfer process, probed both by direct electric field ionization and by microwave transfer, agrees well with the results of calculations performed using a simple theoretical model of the energy transfer process. For measurements performed in zero electric field with atoms prepared in the 1s40s 3S1 level, the transition from a regime in which a single energy transfer channel can be isolated for detection to one in which multiple collision channels begin to play a role has been identified as the NH3 density was increased.
We demonstrated a tuned dipole interaction between Rydberg atoms by employing a controllable electric field in a cold cesium ensemble. The | n P 3/2 ⟩ ( n = 38–40) Rydberg pairs are prepared with a three-photon scheme and detected via the state-selective field ionization technique. A weak DC electric field is used to tune the Rydberg pair interaction from the van der Waals interaction regime to the dipole–dipole interaction regime. The Förster resonant interaction and an adiabatic resonance energy transfer between the n P and n S Rydberg states are attained by precisely tuning the electric field. Rydberg excitation blockade with and without the electric field is investigated by changing the excitation pulse duration, which demonstrates that the dipole interaction–induced blockade effect is stronger than the van der Waals interaction–induced blockade effect. The precise control of the Rydberg interaction is of great significance to the coherent interaction in many-body systems and non-radiative collision processes.
We have studied the collisional energy transfer process K (ns) +K (n-2) d {yields} K (np) +K (n-1) p which is tuned into resonance with an applied static electric field. The initial Rydberg states are excited stepwise with two dye laser pulses. The resonant energy transfer is detected by selectively field ionizing the final K(np) state as the static field is swept over many laser shots. Due to fine structure splitting of the d and p levels 45 resonances are energetically allowed at n{sub s}=25. The actual number of resonances that are observed depends on the polarization of the laser light, the dipole-dipole selection rules, and the n state excited. Above n{sub s}=29 all resonances are energically forbidden. We have measured the position of the resonances in electric field from n{sub s}=25 to n{sub s}=29 and found them to be in good agreement with calculated positions.