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arXiv:1309.7359 · Physical Review A

Production of very-high- n strontium Rydberg atoms

S. Ye, X. Zhang, T. C. Killian, F. B. Dunning, Moritz Hiller, S. Yoshida, Stefan Nagele, Joachim Burgdörfer

Published Oct 28, 2013• 41 citations
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Abstract

The production of very-high-$n$ ($n\ensuremath{\sim}300$--500) strontium Rydberg atoms is explored using a crossed-laser-atom-beam geometry. $n$${}^{1}{S}_{0}$ and $n$${}^{1}{D}_{2}$ states are created by two-photon excitation via the $5s5p$ ${}^{1}{P}_{1}$ intermediate state using radiation with wavelengths of $\ensuremath{\sim}$461 and $\ensuremath{\sim}$413 nm. Rydberg atom densities as high as $\ensuremath{\sim}3\ifmmode\times\else\texttimes\fi{}{10}^{5}$ cm${}^{\ensuremath{-}3}$ have been achieved, sufficient that Rydberg-Rydberg interactions can become important. The isotope shifts in the Rydberg series limits are determined by tuning the 461-nm light to preferentially excite the different strontium isotopes. Photoexcitation in the presence of an applied electric field is examined. The initially quadratic Stark shift of the $n$${}^{1}{P}_{1}$ and $n$${}^{1}{D}_{2}$ states becomes near-linear at higher fields and the possible use of $n{}^{1}{D}_{2}$ states to create strongly polarized, quasi-one-dimensional electronic states in strontium is discussed. The data are analyzed with the aid of a two-active-electron (TAE) approximation. The two-electron Hamiltonian, within which the Sr${}^{2+}$ core is represented by a semi-empirical potential, is numerically diagonalized allowing the calculation of the energies of high-$n$ Rydberg states and their photoexcitation probabilities.

DOI
10.1103/physreva.88.043430

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arXiv:1505.07152•May 26, 2015•1 citation
The production of very-high-nnn (n\ensuremath∼300n\ensuremath{\sim}300n\ensuremath∼300--500) strontium Rydberg atoms is explored using a crossed-laser-atom-beam geometry. n$${}^{1}{S}_{0} and n$${}^{1}{D}_{2} states are created by two-photon excitation via the 5s5p5s5p5s5p 1P1{}^{1}{P}_{1}1P1​ intermediate state using radiation with wavelengths of \ensuremath∼\ensuremath{\sim}\ensuremath∼461 and \ensuremath∼\ensuremath{\sim}\ensuremath∼413 nm. Rydberg atom densities as high as \ensuremath∼3\ifmmode×\else\texttimes\fi105\ensuremath{\sim}3\ifmmode\times\else\texttimes\fi{}{10}^{5}\ensuremath∼3\ifmmode×\else\texttimes\fi105 cm\ensuremath−3{}^{\ensuremath{-}3}\ensuremath−3 have been achieved, sufficient that Rydberg-Rydberg interactions can become important. The isotope shifts in the Rydberg series limits are determined by tuning the 461-nm light to preferentially excite the different strontium isotopes. Photoexcitation in the presence of an applied electric field is examined. The initially quadratic Stark shift of the n$${}^{1}{P}_{1} and n$${}^{1}{D}_{2} states becomes near-linear at higher fields and the possible use of n1D2n{}^{1}{D}_{2}n1D2​ states to create strongly polarized, quasi-one-dimensional electronic states in strontium is discussed. The data are analyzed with the aid of a two-active-electron (TAE) approximation. The two-electron Hamiltonian, within which the Sr2+{}^{2+}2+ core is represented by a semi-empirical potential, is numerically diagonalized allowing the calculation of the energies of high-nnn Rydberg states and their photoexcitation probabilities.
The efficient production of very-high-nnn, $n\ensuremath{\sim}300$, quasi-one-dimensional (quasi-1D) strontium Rydberg atoms through three-photon excitation of extreme Stark states in the presence of a weak dc field is demonstrated using a crossed laser-atom beam geometry. Strongly polarized quasi-1D states with large permanent dipole moments $\ensuremath{\sim}1.2{n}^{2}$ a.u. can be created in the beam at densities ($\ensuremath{\sim}{10}^{6}$ cm${}^{\ensuremath{-}3}$) where dipole blockade effects should become important. A further advantage of three-photon excitation is that the product FFF states are sensitive to the presence of external fields, allowing stray fields to be reduced to very small values. The experimental data are analyzed using quantum calculations based on a two-active-electron model together with classical trajectory Monte Carlo simulations. These allow determination of the atomic dipole moments and confirm that stray fields can be reduced to $\ensuremath{\le}25\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}$V cm${}^{\ensuremath{-}1}$.
The production of high-nnn, $n\ensuremath{\sim}300$, quasi-one-dimensional (quasi-1D) strontium Rydberg atoms through two-photon excitation of selected extreme Stark states in the presence of a weak dc field is examined using a crossed laser-atom beam geometry. The dipolar polarization of the electron wave function in the product states is probed using two independent techniques. The experimental data are analyzed with a classical trajectory Monte Carlo simulation employing initial ensembles that are obtained with the aid of quantum calculations based on a two-active-electron model. Comparisons between theory and experiment highlight different characteristics of the product quasi-1D states, in particular, their large permanent dipole moments, $\ensuremath{\sim}1.0to1.21.0 to 1.21.0to1.2{n}^{2}e{a}_{0}$, where eee is the electronic charge and a0{a}_{0}a0​ is the Bohr radius. Such states can be engineered using pulsed electric fields to create a wide variety of target states.
Dipole-dipole interactions, the strongest, longest-range interactions possible between two neutral atoms, cannot be better manifested anywhere else than in a Rydberg atomic system. Rydberg atoms, having high principal quantum numbers n>>1 and dipole moments that scale as n^2, provide a powerful tool to examine dipole-dipole interactions. Therefore, we have studied the production and production rates of strontium Rydberg atoms created using two-photon excitation and have explored their properties in two distinct experiments. In the first experiment, very-high-n (n~300) Rydberg atoms are produced in a tightly collimated atomic beam allowing spectroscopic studies of their energy levels and their Stark effects. Simulations using a two-active-electron model, developed by our theoretical collaborators, allow detailed analysis of the results and are in remarkable agreement with the experimental results. The high density of Rydberg atoms achieved ~ 5*10^5 cm^(-3), in this experiment will allow studies of strongly interacting Rydberg-Rydberg systems. The second experiment, in which a cold strontium Rydberg gas is excited in a magneto-optic trap, features an imaging technique offering both spatial and temporal resolution. We use this technique to observe and study the evolution of an ultra-cold strontium Rydberg gas which reveals the importance of Rydberg-Rydberg interactions in the early stages of this evolution. Strongly interacting Rydberg gas provides an opportunity to realize a very strongly-correlated ultra-cold plasma.
We investigate the effect of series perturbation on the second-order dipole-dipole interactions between strontium atoms in the 5sns(1S0)5sns({^1}S_0)5sns(1S0​) and 5snp(1P1)5snp({^1}P_1)5snp(1P1​) Rydberg states as a means of engineering long-range interactions between atoms. The series perturbation in these atoms enables modifying the strength and the sign of the interaction by varying the principal quantum number nnn of the Rydberg electron. We utilize experimentally available data to estimate the importance of perturber states, and find that van der Waals interaction between two strontium atoms in the 5snp(1P1)5snp({^1}P_1)5snp(1P1​) states shows strong peaks outside the anticipated hydrogenic n11n^{11}n11 scaling. We identify this to be the result of the perturbation of 5snd(1D2)5snd({^1}D_2)5snd(1D2​) intermediate states by the 4d2(1D2)4d^2({^1}D_2)4d2(1D2​) and 4dn′s(1D2)4dn's({^1}D_2)4dn′s(1D2​) states in the n<20n<20n<20 range. This demonstrates that divalent atoms offer a unique advantage for generating substantially stronger or weaker inter-atomic interactions than those that can be achieved using alkali metal atoms. This is due to the highly perturbed spectra of divalent atoms and other multivalent atoms that can persist up to high nnn. Such irregularities can be especially useful in engineering asymmetric Ry blockade requiring the simultaneous presence of both ``weak'' and ``strong'' interactions.