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SPIE Nanophotonics

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

S. D. Hogan

Published May 24, 2022• 0 citations
Publisher

Abstract

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).

DOI
10.1117/12.2630919

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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).
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.
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.
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.
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.
Resonant energy transfer (RET) between the equal parity 1s65s ^{3}S_{1} and 1s66s ^{3}S_{1} Rydberg levels in helium has been observed in low-temperature (∼80 mK) collisions with ammonia molecules that undergo inversion transitions in their X ^{1}A_{1} ground electronic state. This hybrid Rydberg-atom-polar-molecule resonant energy transfer represents a monopole-dipole energy exchange reaction that necessarily requires spatial overlap of the Rydberg-electron and molecular wave functions. Calculations that account explicitly for the charge-dipole interaction between the Rydberg electron and the molecule provide a quantitative explanation of the observations. Total parity is conserved in the reaction through the mixing of collisional angular momentum in the atom-molecule complex. This work opens opportunities to expand the toolbox for quantum science with charge-dipole-mediated energy exchange in hybrid atom-polar-molecule platforms.
Dipole-dipole interactions between helium atoms in Rydberg-Stark states with principal quantum number n=53n=53n=53 and approximately linear Stark energy shifts, resulting from induced electric dipole moments of approximately 7900 D, have been investigated experimentally. The experiments were performed in pulsed supersonic metastable helium beams, with particle number densities of up to $\ensuremath{\sim}{10}^{9}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$. In the presence of amplitude-modulated, radio-frequency electric fields, changes in the spectral intensity distributions associated with the transitions to these states that are attributed to dipole-dipole interactions within the ensembles of excited atoms have been observed. The experimental results are in excellent agreement with calculations of the Rydberg energy level structure carried out using Floquet methods, and excitations shared by up to four atoms. The use of these Rydberg-Stark states as sensors for nonresonant broadband radio-frequency electrical noise is also discussed.