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arXiv:2504.06977 · Physical Review Letters

Probing Dipolar Interactions between Rydberg Atoms and Ultracold Polar Molecules

Lingbang Zhu, Jeshurun Luke, Roy Shaham, Yi-Xiang Liu, Kang-Kuen Ni

Published Sep 10, 2025• 3 citations
arXivHTMLPDF

Abstract

We probe resonant dipolar interactions between ultracold ^{40}K^{87}Rb molecules and Rydberg ^{87}Rb atoms in an optically trapped ensemble. Through state-selective ionization detection of the KRb molecules, we observe resonant energy transfer at 2.227 GHz from Rydberg atoms to molecules under a tunable external electric field. We measure a broadening up to 3.5 MHz, for the Rb Rydberg excitation spectrum, which matches a Monte Carlo simulation that describes a Rydberg atom and neighboring molecules evolving under a dipole-dipole interacting Hamiltonian. The demonstrated interspecies dipolar interaction is a key ingredient for hybrid Rydberg-polar molecule systems, where the advantages of each system can be leveraged and combined.

DOI
10.1103/48rk-sxfs

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Studying ultracold chemical reactions with quantum state resolution reveals details of the reaction processes, especially with single quantum state preparation of the reactants and state-selective detection of reaction products. In this thesis, we investigate two main processes: KRb + KRb → K2 + Rb2 reactions, and Rb and KRb atom-molecule collisions. In the KRb bimolecular reaction, we demonstrate the preservation of quantum coherence in bimolecular reactions for the first time, which is surprising in a reaction considered to be largely chaotic. Additionally, we proposed a coherent control scheme to manipulate product yields across different product channels. These results represent a critical step toward probing quantum coherence and entanglement in the chemical reaction. In atom-molecule collisions between Rb and KRb, we discovered an exceptionally long-lived intermediate complex, KRb2, which can be photo-excited by trapping light. The observed complex lifetime was orders of magnitude longer than theoretical predictions, underscoring the limitations of the current theory. We further explored the dependence of complex lifetimes on the initial quantum states and external electric and magnetic fields, providing additional experimental benchmarks to guide future theoretical work. Separately, we found that inelastic collisions between hyperfine-excited Rb atoms and KRb molecules can lead to rotation excitation of KRb post-collision. By probing the product state distribution, the result suggests that mechanical angular momentum is coupled to the spins. Such couplings are too weak in the current theory models to explain the result. Moreover, our result contradicts state-of-the-art coupled-channel calculations. These suggest that some subtle effects, such as molecular vibration and conical intersections, play a critical role in the reaction dynamics. The final piece of the thesis describes the observation of resonant interaction between a Rydberg atom and an ensemble of polar molecules. Such hybrid quantum systems have been proposed for a wide range of applications. Our work provides an experimental demonstration of resonant dipolar interactions between Rydberg atoms and ultracold polar molecules, paving the way for the realization of hybrid systems for quantum computation and simulation.

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Physical Review A•Nov 28, 2011•26 citations
We probe resonant dipolar interactions between ultracold ^{40}K^{87}Rb molecules and Rydberg ^{87}Rb atoms in an optically trapped ensemble. Through state-selective ionization detection of the KRb molecules, we observe resonant energy transfer at 2.227 GHz from Rydberg atoms to molecules under a tunable external electric field. We measure a broadening up to 3.5 MHz, for the Rb Rydberg excitation spectrum, which matches a Monte Carlo simulation that describes a Rydberg atom and neighboring molecules evolving under a dipole-dipole interacting Hamiltonian. The demonstrated interspecies dipolar interaction is a key ingredient for hybrid Rydberg-polar molecule systems, where the advantages of each system can be leveraged and combined.
Studying ultracold chemical reactions with quantum state resolution reveals details of the reaction processes, especially with single quantum state preparation of the reactants and state-selective detection of reaction products. In this thesis, we investigate two main processes: KRb + KRb → K2 + Rb2 reactions, and Rb and KRb atom-molecule collisions. In the KRb bimolecular reaction, we demonstrate the preservation of quantum coherence in bimolecular reactions for the first time, which is surprising in a reaction considered to be largely chaotic. Additionally, we proposed a coherent control scheme to manipulate product yields across different product channels. These results represent a critical step toward probing quantum coherence and entanglement in the chemical reaction. In atom-molecule collisions between Rb and KRb, we discovered an exceptionally long-lived intermediate complex, KRb2, which can be photo-excited by trapping light. The observed complex lifetime was orders of magnitude longer than theoretical predictions, underscoring the limitations of the current theory. We further explored the dependence of complex lifetimes on the initial quantum states and external electric and magnetic fields, providing additional experimental benchmarks to guide future theoretical work. Separately, we found that inelastic collisions between hyperfine-excited Rb atoms and KRb molecules can lead to rotation excitation of KRb post-collision. By probing the product state distribution, the result suggests that mechanical angular momentum is coupled to the spins. Such couplings are too weak in the current theory models to explain the result. Moreover, our result contradicts state-of-the-art coupled-channel calculations. These suggest that some subtle effects, such as molecular vibration and conical intersections, play a critical role in the reaction dynamics. The final piece of the thesis describes the observation of resonant interaction between a Rydberg atom and an ensemble of polar molecules. Such hybrid quantum systems have been proposed for a wide range of applications. Our work provides an experimental demonstration of resonant dipolar interactions between Rydberg atoms and ultracold polar molecules, paving the way for the realization of hybrid systems for quantum computation and simulation.
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 demonstrate Rydberg blockade due to the charge-dipole interaction between a single Rb atom and a single RbCs molecule confined in optical tweezers. The molecule is formed by magnetoassociation of a Rb+Cs atom pair and subsequently transferred to the rovibrational ground state with an efficiency of 91(1)%. Species-specific tweezers are used to control the separation between the atom and molecule. The charge-dipole interaction causes blockade of the transition to the Rb(52s) Rydberg state, when the atom-molecule separation is set to 310(40) nm. The observed excitation dynamics are in good agreement with simulations using calculated interaction potentials. Our results open up the prospect of a hybrid platform where quantum information is transferred between individually trapped molecules using Rydberg atoms.
The dipole-dipole interaction strongly couples ultracold highly excited atoms, known as Rydberg atoms, and is the dominant mechanism for energy exchange among such atoms on microsecond time scales. I present the results of experiments that investigate this interaction using rubidium atoms excited to Rydberg states with an all-diode laser system. In the first of these, high resolution dipole-dipole interaction spectra for different magnetic sublevels of the 32d5/2 state are collected and analyzed. In the second experiment, ultracold rubidium atoms are implusively excited to coherent superpositions of three closely spaced |mj|sublevels of the 32d5/2 state in a weak electric field. The magnitude of the field sets the energy level spacing between these states, and hence the frequency of the phase dependent oscillations resulting from interference in resonant energy exchange processes. In the third experiment, the dipole-dipole interaction induced resonant energy exchange between columns of ultracold rubidium Rydberg atoms is imaged using a new technique involving selective field ionization with a spatially sensitive ion detector.
The energy level spectrum of a many-body system containing two shared, collective Rydberg excitations is measured using cold atoms in an optical dipole trap. Two pairs of independently tunable laser pulses are employed to spectroscopically probe the spectrum in a double-resonance excitation scheme. Depending on the magnitude of an applied electric field, the Rydberg-atom interactions can vary from resonant dipole-dipole to attractive or repulsive van der Waals, leading to characteristic signatures in the measured spectra. Our results agree with theoretical estimates of the magnitude and sign of the interactions.
Ultracold Rydberg atoms in a static electric field can exchange energy via the dipole-dipole interaction. The Stark effect shifts the energy levels of the atoms which tunes the energy exchange into resonance at specific values of the electric field (F\"orster resonances). We excite rubidium atoms to Rydberg states by focusing either a 480 nm beam from a tunable dye laser or a pair of diode lasers into a magneto-optical trap. The trap lies at the center of a configuration of electrodes. We scan the electric field by controlling the voltage on the electrodes while measuring the fraction of atoms that interact. Dipole-dipole interaction spectra are presented for initially excited rubidium ndndnd states for n=31n=31n=31 to 46 and for four different pairs of initially excited rubidium nsnsns states. We also present the dipole-dipole interaction spectra for individual rubidium 32ddd (j,mj)(j,\phantom{\rule{0.16em}{0ex}}{m}_{j})(j,mj​) fine structure levels that have been selectively excited. The data are compared to calculated spectra.