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arXiv:1708.02768 · Physical Review A

Cs 62 D J Rydberg-atom macrodimers formed by long-range multipole interaction

Xiaoxuan Han, Suying Bai, Yuechun Jiao, Liping Hao, Yongmei Xue, Jianming Zhao, Suotang Jia, Georg A. Raithel

Published Mar 9, 2018• 25 citations
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Abstract

Long-range macrodimers formed by $D$-state cesium Rydberg atoms are studied in experiments and calculations. Cesium ${[62{D}_{J}]}_{2}$ 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 ${[62{D}_{J}]}_{2}$ 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 $3--6\phantom{\rule{0.28em}{0ex}}\ensuremath{\mu}\mathrm{s}$.

DOI
10.1103/physreva.97.031403

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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\ensuremathμs3--6\phantom{\rule{0.28em}{0ex}}\ensuremath{\mu}\mathrm{s}3−−6\ensuremathμs.
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.
Abstract Electrostatic multipole interactions generate long-range Rydberg–Rydberg macrodimers. We calculate the adiabatic potentials of cesium nD J 2 Rydberg macrodimers for principal quantum numbers n ranging from 56 to 62, for J = 3/2 and 5/2, and for the allowed values of the conserved sum of the atomic angular-momentum components along the internuclear axis, M . For most combinations ( n , M , J ) exactly one binding potential exists, which should give rise to Rydberg macrodimer states. We study the dependence of the adiabatic potentials on the size of the two-body basis sets used in the calculation, and on the maximal order, q max , of the multipole terms included in the calculation. We determine the binding energies and lengths of the binding adiabatic potentials, investigate their scaling behaviors as a function of the effective principal quantum number, and discuss vibrational-state wave functions. We consider the applicability of the calculated potentials and excitation rates to an experimental scheme for preparing nD J 2 Rydberg-atom macrodimers using two-color double-resonant photoassociation.
The long-range multipole interactions between ultra-cold Rydberg atoms form adiabatic potentials, one of which shows a binding potential that can be used to bind Rydberg-Rydberg molecules. Rydberg-atom molecule, known as macrodimer due to its larger size (~μm), has the properties of the abundant vibrational energy levels and large electric dipole moment and so on. Compared with Rydberg atom, the Rydberg molecule, including Rydberg-ground molecule and Rydberg-Rydberg molecule, is susceptible to manipulate by an external field and possesses potential applications in the weak-signal detection, the quantum gas correlation measurement and the vacuum fluctuation and so on. In this paper, we investigate a (60D5/2)2 Rydberg macrodimer theoretically and experimentally. In the calculation, we take into account the multipole interaction of a Rydberg-atom pair, including dipole-dipole, dipole-quadrupole, dipole-octupole and quadrupole-quadrupole interaction and so on. The adiabatic potential of 60D5/2 Rydberg-atom pair is obtained by diagonalizing the interaction Hamiltonian on a grid of internuclear separations, R. The potential depth and binding length of the Rydberg molecular potential well are obtained. In experiment, we prepare the ultra-cold Cs (60D5/2)2 Rydberg molecules by a two-color photoassociation method in a cesium ultracold atom trap. The first-color (pulse-A) resonantly excites a seed Rydberg atom A, and the second color (pulse-B) is detuned and resonantly excites the second Rydberg atom B near to the atom A. Both pulse-A and pulse-B are two-photon excitations (852 nm + 510 nm), between which their 852-nm lasers have the same frequency, whereas the 510-nm laser frequency of the pulse-A is set to be resonant with the atomic transition and the frequency of the pulse-B is detuned by using a double-passed acousto-optic modulator. When the pulse-B is detuned to the molecular binding energy, atom-A and-B are bonded, forming an ultra-cold Cs (60D5/2)2 Rydberg molecule. The two-color photoassociation spectra of Rydberg-Rydberg molecules are detected by the field ionization of Rydberg atoms and molecules with a ramped electric field. Molecular spectra are compared with calculated adiabatic molecular potentials, which yields the binding energy and equilibrium internuclear distance. The two-color photoassociation method used in this work has a doubly resonant character that results in the enhanced excitation rate.
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. ^
We study long range interactions between two Rydberg atoms and predict the existence of ultralong range Rydberg dimers with equilibrium distances of many thousands of Bohr radii. We calculate the dispersion coefficients C5, C6, and C8 for two rubidium atoms in the same excited level np and find that they scale like n(8), n(11), and n(15), respectively. We show that for certain molecular symmetries these coefficients lead to long range potential wells that can support molecular bound levels. Such macrodimers would be very sensitive to their environment and could probe weak interactions. We suggest experiments to detect these macrodimers.