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Bulletin of the American Physical Society

Resonant collisions of K Rydberg atoms

Michael J. Renn, Wayne A. Anderson, James Veale, Thomas F. Gallagher

Published May 1, 1993• 0 citations
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Abstract

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.

Related papers

Resonant collisions of K Rydberg atoms

Michael J. Renn, W. R. Anderson, Thomas F. Gallagher

We have observed resonant-energy-transfer collisions between K Rydberg atoms. We have tuned the ${\mathrm{ns}}_{1/2}$+(n-2)${\mathrm{d}}_{\mathrm{j}}$\ensuremath{\rightarrow}${\mathrm{np}}_{\mathrm{j}\ensuremath{'}}$+(n-1)${\mathrm{p}}_{\mathrm{j}\mathrm{\ensuremath{''}}}$ collisional process into resonance with a static electric field. The measured resonance field positions from n=24 to 29 agree well with the calculated positions. We show that the dipole-dipole selection rule, \ensuremath{\Delta}${\mathrm{m}}_{\mathrm{j}}$=0,\ifmmode\pm\else\textpm\fi{}1, is valid for these resonances but that \ensuremath{\Delta}J=0,\ifmmode\pm\else\textpm\fi{}1 is not, due to the presence of the electric field. In addition, the polarization of the lasers used to excite the Rydberg states can suppress many of the resonances.

Physical Review A•Feb 1, 1994•7 citations

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

Valentina Zhelyazkova, S. D. Hogan

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.

arXiv:1705.01487•Physical Review A•Apr 21, 2017•26 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

Resonant collisions of Na Rydberg atoms in electric and magnetic fields

M. J. Renn, Q. S. Sun, Thomas F. Gallagher

We have observed 10-MHz-wide energy-transfer resonances between colliding Na Rydberg atoms. The narrow linewidth allows us to apply a modest 5--40-G static magnetic field in addition to a static tuning electric field and resolve new resonances arising from magnetic-field-induced splitting of the Stark energy levels. When B is parallel to E, the nine resolved resonances observed with only an E field are further split into 144 possible resonances. However, only the 21 resonances corresponding to collisions in which the spins are unchanged are observable. When B is perpendicular to E, the spectrum of collisional resonances is similar to that of the vertical field case, except that the final spin states cannot be determined. With both parallel and perpendicular fields present, linear and quadratic terms of the B field interaction create more complicated spectra than with either case alone. The experimental spectra agree quantitatively with the spectra calculated using a simple Zeeman model of the energy levels.

Physical Review A•Nov 1, 1994•2 citations

Radiative Rydberg-atom–Rydberg-atom collisions in the strong-field regime

P. Pillet, Ravinder Kachru, Nam Huu Tran +2 more

We describe the experimental observation of the resonant collisional energy transfer Na(ns)+Na(ns)+qh\ensuremath{\nu}\ensuremath{\rightarrow}Na(np)+Na[(n-1)p]+(q○)h\ensuremath{\nu} which occurs when the Na atoms in a strong microwave field are tuned in energy with a static field so that the energy resonance ${E}_{\mathrm{ns}}$+${E}_{\mathrm{ns}}$=${E}_{\mathrm{np}}$+${E}_{n\mathrm{\ensuremath{-}}1}$,p\ifmmode\pm\else\textpm\fi{}mh\ensuremath{\nu} occurs. We describe our experimental observations and provide a detailed description of a nonperturbative theory which we have developed to explain our observations. The theory is essentially developed in terms of the resonant dipole-dipole collisions between ``microwave dressed'' atoms. Using an extension of the approach we used previously to describe resonant dipole-dipole collisions in the absence of microwaves, we are able to take into account all the coherences in the problem in a completely straightforward way.

Physical Review A•Aug 1, 1987•37 citations

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
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.
We have observed resonant-energy-transfer collisions between K Rydberg atoms. We have tuned the ns1/2{\mathrm{ns}}_{1/2}ns1/2​+(n-2)dj{\mathrm{d}}_{\mathrm{j}}dj​\ensuremath{\rightarrow}${\mathrm{np}}_{\mathrm{j}\ensuremath{'}}$+(n-1)${\mathrm{p}}_{\mathrm{j}\mathrm{\ensuremath{''}}}$ collisional process into resonance with a static electric field. The measured resonance field positions from n=24 to 29 agree well with the calculated positions. We show that the dipole-dipole selection rule, \ensuremath{\Delta}mj{\mathrm{m}}_{\mathrm{j}}mj​=0,\ifmmode\pm\else\textpm\fi{}1, is valid for these resonances but that \ensuremath{\Delta}J=0,\ifmmode\pm\else\textpm\fi{}1 is not, due to the presence of the electric field. In addition, the polarization of the lasers used to excite the Rydberg states can suppress many of the resonances.
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 $|ns\ensuremath{\rangle}$ and $|np\ensuremath{\rangle}$ 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 $|ns\ensuremath{\rangle}$ and $|np\ensuremath{\rangle}$ 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 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).
We have observed 10-MHz-wide energy-transfer resonances between colliding Na Rydberg atoms. The narrow linewidth allows us to apply a modest 5--40-G static magnetic field in addition to a static tuning electric field and resolve new resonances arising from magnetic-field-induced splitting of the Stark energy levels. When B is parallel to E, the nine resolved resonances observed with only an E field are further split into 144 possible resonances. However, only the 21 resonances corresponding to collisions in which the spins are unchanged are observable. When B is perpendicular to E, the spectrum of collisional resonances is similar to that of the vertical field case, except that the final spin states cannot be determined. With both parallel and perpendicular fields present, linear and quadratic terms of the B field interaction create more complicated spectra than with either case alone. The experimental spectra agree quantitatively with the spectra calculated using a simple Zeeman model of the energy levels.
We describe the experimental observation of the resonant collisional energy transfer Na(ns)+Na(ns)+qh\ensuremath{\nu}\ensuremath{\rightarrow}Na(np)+Na[(n-1)p]+(q○)h\ensuremath{\nu} which occurs when the Na atoms in a strong microwave field are tuned in energy with a static field so that the energy resonance Ens{E}_{\mathrm{ns}}Ens​+Ens{E}_{\mathrm{ns}}Ens​=Enp{E}_{\mathrm{np}}Enp​+${E}_{n\mathrm{\ensuremath{-}}1}$,p\ifmmode\pm\else\textpm\fi{}mh\ensuremath{\nu} occurs. We describe our experimental observations and provide a detailed description of a nonperturbative theory which we have developed to explain our observations. The theory is essentially developed in terms of the resonant dipole-dipole collisions between ``microwave dressed'' atoms. Using an extension of the approach we used previously to describe resonant dipole-dipole collisions in the absence of microwaves, we are able to take into account all the coherences in the problem in a completely straightforward way.
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.