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arXiv:0901.1825

Observation of Cs Rydberg atom macrodimers

K. Richard Overstreet, Arne Schwettmann, Tallant, Jonathan, Donald W. Booth, James P. Shaffer

Published Jan 13, 2009• 3 citations
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Abstract

We report the observation of cold Cs Rydberg atom molecules bound at internuclear separations of R~3-9 um. The bound states result from avoided crossings between Rydberg atom pair interaction potentials in an applied electric field. The molecular states can be modified by changing the applied electric field. The molecules are observed by mapping the radial separation of the two Rydberg atoms as a function of time delay between excitation and detection using the Coulomb repulsion of the ions after pulsed field ionization. Measurements were performed for 63D+65D, 64D+66D, 65D+67D, and 66D+68D pairs. The experiment is in good agreement with calculations of the pair interactions for these states.

DOI
10.48550/arxiv.0901.1825

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•Jan 1, 2008•2 citations
We report the observation of cold Cs Rydberg atom molecules bound at internuclear separations of R~3-9 um. The bound states result from avoided crossings between Rydberg atom pair interaction potentials in an applied electric field. The molecular states can be modified by changing the applied electric field. The molecules are observed by mapping the radial separation of the two Rydberg atoms as a function of time delay between excitation and detection using the Coulomb repulsion of the ions after pulsed field ionization. Measurements were performed for 63D+65D, 64D+66D, 65D+67D, and 66D+68D pairs. The experiment is in good agreement with calculations of the pair interactions for these states.
Long-range metastable molecules consisting of two cesium atoms in high Rydberg states have been observed in an ultracold gas. A sequential three-photon two-color photoassociation scheme is employed to form these molecules in states, which correlate to np(n+1)s dissociation asymptotes. Spectral signatures of bound molecular states are clearly resolved at the positions of avoided crossings between long-range van der Waals potential curves. The experimental results are in agreement with simulations based on a detailed model of the long-range multipole-multipole interactions of Rydberg-atom pair states. We show that a full model is required to accurately predict the occurrence of bound Rydberg macrodimers. The macrodimers are distinguished from repulsive molecular states by their behavior with respect to spontaneous ionization and possible decay channels are discussed.
Long-range macrodimers formed by DDD-state cesium Rydberg atoms are studied in experiments and calculations. Cesium [62DJ]2{[62{D}_{J}]}_{2}[62DJ​]2​ Rydberg-atom macrodimers, bonded via long-range multipole interaction, are prepared by two-color photoassociation in a cesium atom trap. The first color (pulse A) resonantly excites seed Rydberg atoms, while the second (pulse B, detuned by the molecular binding energy) resonantly excites the Rydberg-atom macrodimers below the [62DJ]2{[62{D}_{J}]}_{2}[62DJ​]2​ asymptotes. The molecules are measured by extraction of autoionization products and Rydberg-atom electric-field ionization, and ion detection. Molecular spectra are compared with calculations of adiabatic molecular potentials. From the dependence of the molecular signal on the detection delay time, the lifetime of the molecules is estimated to be $3--6\phantom{\rule{0.28em}{0ex}}\ensuremath{\mu}\mathrm{s}$.
We present calculations of potential curves for very high-nnn (89D)(89D)(89D) Cs Rydberg-atom pairs, including a background electric field. From these potentials, we show that energy transfer occurs at rates of $\ensuremath{\sim}30--70\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, background electric fields play an important role and dipole-dipole- and quadrupole-quadrupole-induced avoided curve crossings should lead to conversion of electronic to kinetic energy, nnn-changing collisions, and observable ultracold long-range Rydberg molecules.
The Stark effect of ultra-cold Cs Rydberg atom is investigated in a magneto-optical trap, and the avoided crossing between nS state and (n-4) manifold is observed. The ion spectrum near the avoided crossing is obtained by using state-selective field pulse ionization technique. By changing the intensity of the applied electric field, we find that the relative intensities of two Stark states near the avoided crossing exchange obviously. Furthermore, state transfer from nS Rydberg state to high-l state due to the avoided crossing is also obtained.
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.
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.