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Journal of Physics B Atomic Molecular and Optical Physics

Detecting electric-field-tuned atom–atom level mixing in a cold85Rb Rydberg gas by two-unequal-frequency photons

Jianing Han

Published Nov 19, 2010• 7 citations
Publisher

Abstract

We use two-unequal-frequency microwave photons as sensitive probes to study the n s n s to the n p( n + m − 1)p Rydberg pair state transition in a cold 85 Rb gas, where n and m are integers. The principal quantum number n dependence of the energy differences between n s( n + 1)s and n p 3/2 n p 3/2 as well as n s( n + 2)s and n p 1/2 ( n + 1)p 1/2 has been measured and the results are consistent with the calculated values. Additionally, we demonstrate that the pair state Stark shift is the sum of the Stark shifts of both isolated Rydberg atoms. Finally, we tune the dipole–dipole mixing probability by applying an electric field to tune the energy difference between the dipole–dipole coupled states, n s( n + 2)s and n p 1/2 ( n + 1)p 1/2 . The results reported here are essential steps towards electric-field-controlled chemical reactions [1], quantum gates, molecular autoionization and few-body correlations.

DOI
10.1088/0953-4075/43/23/235205

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Journal of Physics B Atomic Molecular and Optical Physics•Aug 9, 2023•2 citations
We use two-unequal-frequency microwave photons as sensitive probes to study the n s n s to the n p( n + m − 1)p Rydberg pair state transition in a cold 85 Rb gas, where n and m are integers. The principal quantum number n dependence of the energy differences between n s( n + 1)s and n p 3/2 n p 3/2 as well as n s( n + 2)s and n p 1/2 ( n + 1)p 1/2 has been measured and the results are consistent with the calculated values. Additionally, we demonstrate that the pair state Stark shift is the sum of the Stark shifts of both isolated Rydberg atoms. Finally, we tune the dipole–dipole mixing probability by applying an electric field to tune the energy difference between the dipole–dipole coupled states, n s( n + 2)s and n p 1/2 ( n + 1)p 1/2 . The results reported here are essential steps towards electric-field-controlled chemical reactions [1], quantum gates, molecular autoionization and few-body correlations.
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).
Systems of cold, interacting Rydberg atoms are of interest because they exhibit a wide range of collective quantum phenomena. This thesis describes experimental and theoretical work related to these systems with an emphasis on two phenomena: Rydberg excitation blockades and quantum-state-changing collisions. I begin by presenting a detailed calculation of the interaction energies of two Rydberg atoms for a variety of orientations, quantum states, and applied electric fields. The calculated energies are used to interpret the experimental results that follow. I then describe measurements showing that the widths of the distributions of Rydberg excitation number are related to the effectiveness of a Rydberg excitation blockade. These distributions are investigated as a function of principal quantum number, n, and applied electric field. In the presence of a Forster resonant field, sub-Poissonian distributions are measured. I next present a spectroscopic measurement of the energy level shift of a system of atoms which collectively shares two Rydberg excitations. The qualitative nature of the shift depends sensitively on the type of interactions between the atoms (van der Waals or dipole-dipole) and may be changed by changing the quantum state or applied electric field. This measurement provides the first spectroscopic proof that Rydberg excitation blockades are operative. Finally, I describe measurements of the probability for quantum state-changing and Penning-ionizing collisions to provide evidence for intrinsic, electric field-free-interaction resonances and complex many-body interactions in systems of cold Rydberg atoms.
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.
Long-range interactions between cold Rydberg atoms, which are used in many important applications, can be enhanced using F\"orster resonances between collective many-body states controlled by an external electric field. Here we report on the first experimental observation of highly resolved radio-frequency-assisted F\"orster resonances in a few cold Rb Rydberg atoms. We also observed radio-frequency-induced F\"orster resonances which cannot be tuned by a dc electric field. They imply an efficient transition from van der Waals to resonant dipole-dipole interaction due to Floquet sidebands of Rydberg levels appearing in the rf field. This method can be applied to enhance the interactions of almost arbitrary Rydberg atoms with large principal quantum numbers.
We have observed a density-dependent frequency shift of more than 4 MHz in a cold 85{}^{85}85Rb Rydberg gas trapped in a magneto-optical trap. A one-dimensional linearly aligned four-body model is proposed to explain the experimental data, and the calculation matches the experimental data. The calculation also shows that if the energy detuning between the two coupled states, the nsnsns(n+1)snsnsns(n+1)snsnsns(n+1)s and nsnsnpnpnsnsnpnpnsnsnpnp states in this case, is small, the lowest level of the nsnsnpnpnsnsnpnpnsnsnpnp manifold has the maximum mixing probability, causing a frequency shift instead of line broadening. The results reported may be used for few-body blockade, Rydberg single-atom imaging, studying few-body to many-body transitions and interactions, and few-body ionization as well as quantum metrology.