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arXiv:2205.04327 · The Journal of Physical Chemistry Letters

Rydberg Atom-Enabled Spectroscopy of Polar Molecules via Förster Resonance Energy Transfer

Sabrina Patsch, Martin Zeppenfeld, Christiane P. Koch

Published Nov 11, 2022• 10 citations
arXivHTMLPDF

Abstract

Non-radiative energy transfer between a Rydberg atom and a polar molecule can be controlled by a static electric field. Here, we show how to exploit this control for state-resolved, non-destructive detection and spectroscopy of the molecules, where the lineshape reflects the type of molecular transition. Using the example of ammonia, we identify the conditions for collision-mediated spectroscopy in terms of the required electric field strengths, relative velocities, and molecular densities. Rydberg atom-enabled spectroscopy is feasible with current experimental technology, providing a versatile detection method as a basic building block for applications of polar molecules in quantum technologies and chemical reaction studies.

DOI
10.1021/acs.jpclett.2c02521

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Non-radiative energy transfer between a Rydberg atom and a polar molecule can be controlled by a static electric field. Here, we show how to exploit this control for state-resolved, non-destructive detection and spectroscopy of the molecules, where the lineshape reflects the type of molecular transition. Using the example of ammonia, we identify the conditions for collision-mediated spectroscopy in terms of the required electric field strengths, relative velocities, and molecular densities. Rydberg atom-enabled spectroscopy is feasible with current experimental technology, providing a versatile detection method as a basic building block for applications of polar molecules in quantum technologies and chemical reaction studies.
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 perform a comprehensive investigation of Förster resonant energy transfer in a room-temperature thermal mixture of ammonia molecules and rubidium Rydberg atoms. Fully state-resolved measurement of the Rydberg-atom populations is achieved by combining millimeter-wave state transfer with state-selective field ionization. This allows aspects of the energy transfer process such as state dependence, ammonia pressure dependence, and dependence on the energy resonance condition to be investigated in detail. Our results pave the way for future quantum experiments combining polar molecules and Rydberg atoms.
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.
A highly sensitive, general, and preferably nondestructive technique to detect polar molecules would greatly advance a number of fields, in particular quantum science with cold and ultracold molecules. Here, we propose using resonant energy transfer between molecules and Rydberg atoms to detect molecules. Based on an energy transfer cross-section of > 10 −6 cm 2 for sufficiently low collision energies, a near unit efficiency non-destructive detection of basically any polar molecule species in a well-defined internal state should be possible.
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.
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.