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Physical Review A

Cold Cs Rydberg-gas interactions

Arne Schwettmann, Jeff Crawford, K. Richard Overstreet, James P. Shaffer

Published Aug 25, 2006• 92 citations
Publisher

Abstract

We present calculations of potential curves for very high-$n$ $(89D)$ 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, $n$-changing collisions, and observable ultracold long-range Rydberg molecules.

DOI
10.1103/physreva.74.020701

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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∼30−−70MHz\ensuremath{\sim}30--70\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}\ensuremath∼30−−70MHz, 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.
We have observed the evolution of cold Rydberg gases and ultracold plasmas in an environment that allows for the control of interactions of the blackbody radiation temperature from 4K to 300K. The work in this thesis describes the influence of initial densities, populations, excitation state, evolution time and thermal background temperature on the evolution of cold Rydberg gases as well as directly excited ultracold plasmas. With some initial ionization, cold-Rydberg-atom gases easily develop a positive space charge that traps electrons for times on the order of tens of mus. This acts as a catalyst for electron-Rydberg atom collisions, increasing the collision probabilities by orders of magnitude and profoundly altering the final state of the Rydberg gas. Using state-selective field ionization, we have provided direct proof that these collisions cause changes in l-states, and we have seen the first experimental evidence that they also lead to inelastic n-changing collisions, as predicted by theory. We have also found evidence for Rydberg-Rydberg collisions, enabled by the attractive electric-dipole forces between atoms in high-l states and possibly by van-der-Waal's interactions at very high-n . Thermal interactions are seen to influence the formation of a plasma from a cold Rydberg gas. Plasmas form more easily in the presence of a 300K radiation field than at 4K, due to the contribution of thermal ionization to the plasma formation. The background temperature also appears to affect the electron temperature in both the directly excited plasma and the plasma spontaneously formed from a cold Rydberg gas. In Rydberg atom gases that have undergone partial ionization, electron temperatures were estimated using the dependence of n-changing collisions on the electron temperature.
The interaction between a Rydberg electron and a neutral atom situated inside its extended orbit is described via contact interactions for each atom-electron scattering channel. In ultracold environments, these interactions lead to long-range molecules with binding energies typically ranging from 10 to $1\ifmmode\times\else\texttimes\fi{}{10}^{4}$ MHz. These energies are comparable to the relativistic and hyperfine structure of the separate atomic components. Studies of molecular formation aiming to reproduce observations with spectroscopic accuracy must therefore include the hyperfine splitting of the neutral atom and the spin-orbit splittings of both the Rydberg atom and the electron-atom interaction. Adiabatic potential energy curves and permanent electric dipole moments are presented for Rb2{\mathrm{Rb}}_{2}Rb2​ and Cs2{\mathrm{Cs}}_{2}Cs2​. The influence of spin degrees of freedom on the potential energy curves and multipole moments probed in recent experimental work is elucidated, and the observed dipole moments of butterfly molecules are explained by the generalized 3PJ^{3}P_{J}3PJ​ pseudopotential derived here.
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.
Ultra-cold long-range Rydberg-ground molecule consisting of a Rydberg atom and one or more ground-state atoms is formed by low-energy scattering between the Rydberg electron and ground-state atoms located inside the Rydberg electron’s wave function. The low-energy scattering interaction, initially investigated by Fermi and Omont, has been predicted to lead to molecular binding in a novel type of Rydberg molecules, including the trilobite and butterfly molecules. Their unconventional binding mechanism, which is unlike covalent, or ionic, or van der Waals bonds, results in loosely bound molecules with bond lengths on the order of thousands of Bohr radius. This kind of molecule with large size and huge permanent electric dipole moment is a good candidate for realizing the certain strongly correlated many-body gases and for quantum information processing, as well as for dipolar quantum gases and spin systems with long-range interactions. Consequently, these molecules have received considerable attention in recent years. In this paper, we review the recent theoretical and experimental investigations of ultra-cold long-range Rydberg-ground molecules, including the scattering interaction between the Rydberg electron and ground-state atom and the resulting adiabatic potential curves, experimental observations of photo-associated Rydberg-ground molecules spectra, as well as the measurements of permanent electric dipole moment. Ultra-cold long-range Rydberg-ground molecules are prepared by photoassociation in a high-density cold atom sample. Therefore, the Rydberg electron can bind several ground-state atoms to form a polyatomic Rydberg-ground molecule. The permanent molecular electric-dipole moments are revealed by spectral line broadening in the electric fields. The latest research pointed out that the permanent electric dipole moments of the Cs nDJ -type Rydberg-ground molecules are negative, which is different from the previous reports (the electric dipole moments are positive). The negative sign reflects a deficiency of Rydberg-electron density near the ground-state perturber, which is caused by electronic configuration mixing.
Collisions involving Rydberg atoms reveal detailed information on the state of a background medium and can be used as diagnostic probes of temperature and density distributions in a neutral or ionized gas. Spectroscopy of Rydberg atoms in highly excited states reveals the interaction of the Rydberg electron with core electrons, including relativistic effects, and can be used for precise determination of fundamental constants. The advent of ultracold trapping and cooling methods in the last three decades has ushered in a new paradigm in Rydberg physics control and manipulation. The concept of the Rydberg blockade, for instance, al- lows for precise control of long-range dipolar interaction between atoms, creation of correlated many-body wave functions, and realization of macroscopic quantum entanglement and quan- tum logic operations. The formation of a new class of Rydberg molecules arising from ground and Rydberg atom collisions can be used to manipulate electron-atom scattering phase shifts, form and manipulate molecules with enormous permanent electric dipole moments, study Ry- dberg chemistry at the ultracold, and realize macroscopic quantum polaronic systems. In this thesis, I will investigate charge transfer from covalent ground-Rydberg collisions to form heavy ion pair states. In another related study, I explore the formation of spin-mixed ultralong range Rydberg molecules, by accounting for spin-dependent relativistic fine and hyperfine interac- tion. Such studies help to not only explain experimental observations, but also point to how molecular reactions can be controlled using small electric or magnetic fields.
Cold Rydberg atoms are known to display dipole-dipole interaction-allowed resonances, also called F\"orster resonances, which lead to an efficient energy transfer when the proper electric field is used. This electric field also enables resonances, which do not respect the dipole-dipole selection rules under zero field. A few of these quasiforbidden resonances have been observed but they are often overlooked. Here we show that in cold 133Cs^{133}\mathrm{Cs}133Cs atoms there is a large number of these resonances that display a significant transfer efficiency due to their strong interactions, even at low electric field. We also develop a graphical method enabling us to find all possible resonances simultaneously. The resulting dramatic increase in the total number of addressable resonant energy transfers at different electric fields could have implications in the search for few-body interactions or macromolecules built from Rydberg atoms.