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arXiv:0801.2386 · Physical Review A

Long-range potentials and ( n − 1 ) d + n s molecular resonances in an ultracold Rydberg gas

Jovica Stanojevic, Robin Côté, D. Tong, Edward E. Eyler, P. L. Gould

Published Nov 14, 2008• 39 citations
arXivHTMLPDF

Abstract

We have calculated long-range molecular potentials of the ${0}_{g}^{+}$, ${0}_{u}^{\ensuremath{-}}$, and ${1}_{u}$ symmetries between highly excited rubidium atoms. Strong $np+np$ potentials characterized by these symmetries are important in describing interaction-induced phenomena in the excitation spectra of high $np$ Rydberg states. Long-range molecular resonances are one such phenomenon and they were first reported in S. M. Farooqi et al., Phys. Rev. Lett. 91, 183002 (2003). One class of these resonances occurs at energies corresponding to excited atom pairs $(n\ensuremath{-}1)d+ns$. Such resonances are attributed to $\mathcal{l}$-mixing due to Rydberg-Rydberg interactions so that otherwise forbidden molecular transitions become allowed. We calculate molecular potentials in Hund's case (c), use them to find the resonance line shape, and compare to experimental results.

DOI
10.1103/physreva.78.052709

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We have calculated long-range molecular potentials of the 0g+{0}_{g}^{+}0g+​, 0u\ensuremath−{0}_{u}^{\ensuremath{-}}0u\ensuremath−​, and 1u{1}_{u}1u​ symmetries between highly excited rubidium atoms. Strong np+npnp+npnp+np potentials characterized by these symmetries are important in describing interaction-induced phenomena in the excitation spectra of high npnpnp Rydberg states. Long-range molecular resonances are one such phenomenon and they were first reported in S. M. Farooqi et al., Phys. Rev. Lett. 91, 183002 (2003). One class of these resonances occurs at energies corresponding to excited atom pairs (n\ensuremath−1)d+ns(n\ensuremath{-}1)d+ns(n\ensuremath−1)d+ns. Such resonances are attributed to l\mathcal{l}l-mixing due to Rydberg-Rydberg interactions so that otherwise forbidden molecular transitions become allowed. We calculate molecular potentials in Hund's case (c), use them to find the resonance line shape, and compare to experimental results.
We present evidence for molecular resonances in a cold dense gas of rubidium Rydberg atoms. Single UV photon excitation from the 5s ground state to np Rydberg states (n=50-90) reveals resonances at energies corresponding to excited atom pairs (n-1)d+ns. We attribute these normally forbidden transitions to avoided crossings between the long-range molecular potentials of two Rydberg atoms. These strong van der Waals interactions result in avoided crossings at extremely long range, e.g., approximately 58 000 times the Bohr radius (a(0)) for n=70.
New phenomena have been observed by exciting ultracold ground-state atoms to Rydberg states. Starting with a dense sample of Rb atoms in a magneto-optical trap, we excite them to high Rydberg states (n = 30 - 90) with a single UV excitation pulse. Long-range molecular resonances with interatomic distances exceeding 104 a0 have been discovered. We have also observed the Rydberg excitation blockade, crucial for the implementation of quantum phase gates using neutral atoms. The physics behind these observations is attributed to the strong long-range van der Waals interactions among the Rydberg atoms. In addition, we have seen dipole (E1) forbidden but quadrupole (E2) allowed 5s → nd transitions, allowing us to determine the E2 oscillator strengths to these high Rydberg states. Our narrow-band UV pulsed laser system, with ∼100 MHz bandwidth, also allows us to measure the ratios of j-dependent oscillator strengths to the p and d Rydberg states. ^
In this thesis I present several theoretical methods to explore the excitation dynamics of Ultracold Rydberg systems in various regimes. For some applications the details of interactions between Rydberg atoms have to be carefully examined, while for others, the many-body aspect of Rydberg excitation may be crucial. In both cases, the basic prerequisite is to know the interactions sufficiently well. I will review the basic concepts how to evaluate molecular potentials in various Hund's cases and approximations. Long-range Rydberg-Rydberg interactions between Rydberg atoms induce ℓ-mixing which in certain situations gives rise to molecular resonances. For these resonances, we calculate long-range potentials in Hund's case (c) by diagonalization of an interaction matrix. The excitation dynamics of the resonances is always modeled as pair excitation. At high principal quantum number n, the interactions between Rydberg atoms can blockade the excitation of many surrounding atoms in the range of few μm. The atoms within this range are strongly correlated so that many-body treatments are, in general, needed. To describe this blockading effect and other manifestations of the collective behavior of Rydberg excitation, such as the many-body Rabi oscillations, spatial correlations between atoms and the fluctuations of the number of excited atoms, I have used three different approaches. In the mean-field approach the interactions between different atoms is modeled by a distribution of mean-field shifts for which a distribution of probabilities is calculated, A good agreement between the theoretical model and experimental measurements is found. To study the correlations between atoms the many-body wavefunction is numerically computed. The possibility of observing the many-body Rabi oscillations of Rydberg excitation and other aspects of many-body dynamics is analyzed. Although strong interactions cannot be treated perturbatively other expansions may be feasible. I will show that the expansion in powers of the single atom Rabi frequency can be evaluated in the interaction and Heisenberg picture. The expansion is expected to behave well for arbitrary strong interactions. ^
The work presented in this dissertation represents a comprehensive study on long-range interactions between alkali Rydberg atoms. As a consequence of their size, Rydberg atoms possess very large dipole moments, making them highly sensitive to external fields and to other Rydberg atoms. The strong dipole-dipole interaction between two Rydberg atoms results in a mixing of their angular momentum characters, which is the cornerstone of the work presented here. We describe the ℓ-mixing between various local molecular asymptotes through a residual Coulomb potential, assuming no electron cloud overlap. We then directly diagonalize an interaction Hamiltonian consisting of these Rydberg-Rydberg interactions and spin-orbit (fine structure) coupling in the Hund's case (c). In this manner, we calculate potential energy curves for various molecular symmetries and find that some of these curves exhibit deep potential wells, capable of supporting very extended bound molecular states ( macrodimers). We analyze the specific structure of the ℓ-mixing for these potential wells and derive convenient n-scaling relations for both their equilibrium separations Re and well depths De. We also explore various properties of the macrodimers, including their response to small electric fields and stability with respect to predissociation. We note throughout the dissertation that the detection of such extended dimers could help progress studies in a variety of areas such as exotic, ultracold chemistry and quantum information and computing. To facilitate detection, we propose a scheme to form and study the macrodimers via photoassociation (PA). We present calculated PA lineshapes from two different electronic ground states based on a harmonic trapping model. We find that both PA signals vary significantly with the laser detunings, indicating that different ℓ-characters could be probed at different equilibrium lengths. Finally, we extend the two-body formalism to the case of three interacting Rydberg atoms and present preliminary results for triply excited 58p rubidium atoms along a common axis. We provide a few examples of surface plots corresponding to different local asymptotes, each with a unique three-dimensional "landscape" and discuss the relevance of the physical features. The highlight of our analysis is the appearance of a potential well, which indicates the formation of a linear trimer. ^
When an excited atomic electron interacts with a neutral perturbing atom or molecule that possesses a shape resonance, it generates a characteristic class of Born-Oppenheimer potential curves that rise with internuclear distance. We document this effect, and predict the existence of a diverse class of stable, strongly bound atom-atom and atom-molecule states that result from this phenomenon. For the specific case in which Rb is the perturbing atom, we show that such states should be observable in the spectroscopy of an ultracold gas or condensate.
Pulsed laser excitation of a dense ultracold Cs vapor has been used to study the pairwise interactions between Cs atoms excited to np3/2n{p}_{3/2}np3/2​ Rydberg states of principal quantum numbers in the range n=22−−36n=22--36n=22−−36. Molecular resonances were observed that correspond to excitation of Rydberg-atom-pair states correlated not only to the np3/2+np3/2n{p}_{3/2}+n{p}_{3/2}np3/2​+np3/2​ dissociation asymptotes, but also to $n{s}_{1/2}+(n+1){s}_{1/2}, n{s}_{1/2}+{n}^{\ensuremath{'}}{f}_{j}$, and $(n\ensuremath{-}4){f}_{j}+(n\ensuremath{-}3){f}_{j}\phantom{\rule{4pt}{0ex}}(j=5/2,7/2)$ dissociation asymptotes. These pair resonances are interpreted as arising from dipole-dipole and higher-order long-range-interaction terms between the Rydberg atoms on the basis of (i) their spectral positions, (ii) their response to static and pulsed electric fields, and (iii) millimeter-wave spectra between pair states correlated to different pair-dissociation asymptotes. The Rydberg-atom-pair states were found to spontaneously decay by Penning ionization and the dynamics of the ionization process were investigated during the first 15 $\ensuremath{\mu}\mathrm{s}$ following initial photoexcitation. To interpret the experimental observations, a potential model was derived that is based on the numerical determination of the eigenvalues and eigenfunctions of the long-range interaction Hamiltonian. With this potential model, which does not include adjustable parameters, all experimental observations could be accounted for, and the results demonstrate that long-range-interaction models provide a global and accurate description of interactions in ultracold Rydberg gases and that they correctly account for, and enable the analysis of, phenomena as diverse as the formation of Rydberg macrodimers, Penning ionization in dense Rydberg gases, and Rydberg-excitation-blockade effects.