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arXiv:1206.4852 · Physical Review A

Enlarged molecules from excited atoms in nanochannels

M. Boström, Iver Brevik, Bo E. Sernelius, Maofeng Dou, Clas Persson, Barry William Ninham

Published Jul 3, 2012• 4 citations
arXivHTMLPDF

Abstract

The resonance interaction that takes place in planar nanochannels between pairs of excited-state atoms is explored. We consider interactions in channels of silica, zinc oxide, and gold. The nanosized channels induce a dramatically different interaction from that in free space. Illustrative calculations for two lithium and cesium atoms demonstrate that there is a short-range repulsion followed by long-range attraction. The binding energy is strongest near the surfaces. The size of the enlarged molecule is biggest at the center of the cavity and increases with channel width. Since the interaction is generic, we predict that enlarged molecules are formed in porous structures, and that the molecule size depends on the size of the nanochannels.

DOI
10.1103/physreva.86.014701

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This chapter deals with atom-wall interaction occurring in the "long-range" regime (typical distances: 1-1000 nm), when the electromagnetic fluctuations of an isolated atom are modified by the vicinity with a surface. Various regimes of interaction are discussed in an Introductory part, from Cavity Quantum ElectroDynamics modifications of the spontaneous emission, to Casimir effect, with emphasis on the atom-surface van der Waals interaction, characterized as a near-field interaction governed by a z-3 dependence. The major part of the Chapter focuses on the experimental measurements of this van der Waals interaction, reviewing various recent techniques, and insists upon optical techniques, and notably selective reflection spectroscopy which is particularly well-suited when excited atoms are considered. A review of various experiments illustrates the specific effects associated with a resonant coupling between the atomic excitation and surface modes, from van der Waals repulsion to surface-induced resonant transfer, and with anisotropy effects, including metastability transfer induced by a quadrupole contribution in the interaction. The effects of a thermal excitation of the surface -with a possible remote energy transfer to an atom-, and of interaction with nanobodies -which are intrinsically non planar- are notably discussed among the prospects.
We present a two-channel model to describe the quantum state of two atoms with finite-range interaction near a Feshbach resonance. This model provides a simple picture to analytically derive the wave function and the binding energy of the molecular bound state. The results agree excellently with the measurements and multichannel calculations. For small binding energies, the system enters a threshold regime in which the Feshbach molecules are identical to long range atom pairs in single channel. According to their threshold behavior, we find Feshbach resonances can be classified into two types.
We study the molecular behavior of two atoms interacting near a Feshbach resonance in the presence of a 1D periodic potential. The critical value of the scattering length needed to produce a molecule and the binding energy at resonance are calculated as a function of the intensity of the periodic potential. Because of the non-separability of the center of mass and relative motion, the binding energy depends on the quasimomentum of the molecule. This has dramatic consequences on the molecular tunneling properties, which become strongly dependent on the scattering length.
We consider the feasibility of observing a trap-induced resonance [Stock et al., Phys. Rev. Lett. 91, 183201 (2003)] for the case of two 133Cs^{133}\mathrm{Cs}133Cs atoms, trapped in separated wells of a polarization-gradient optical lattice, and interacting through a multichannel scattering process. Due to the anomalously large scattering length of cesium dimers, a strong coupling can occur between vibrational states of the trap and a weakly bound molecular state that is made resonant by the ac Stark shift of the lattice. We calculate the energy spectrum of the two-atom system as a function of the distance between two potential wells by connecting the solutions of the Schr\"odinger equation for the short-range molecular potential to that of the long-range trap in a self-consistent manner. The short-range potential is treated through a multichannel pseudopotential, parametrized by the KKK matrix, calculated numerically for atoms in free space in a close-coupling approximation. This captures both the bound molecular spectrum as well as the energy-dependent scattering for all partial waves. We establish realistic operating conditions under which the trap-induced resonance could be observed and show that this strong and coherent interaction could be used as a basis for high-fidelity two-qubit quantum logic operations.
Long-range Rydberg molecules (LRMs) form when a highly excited Rydberg electron scatters from ground-state atoms inside its orbit, creating oscillatory, long-range potentials. We present a combined theoretical and experimental study of caesium dimers correlated to 402P3/2 Rydberg states, with an emphasis on decay via autoionisation (associative ionisation). Our model includes a relativistic treatment of electron-atom scattering with spin-orbit coupling, the perturber's hyperfine structure, and coupling of vibrational levels to a continuum of short-range decay channels. Calculated potential-energy curves predict two families of wells: outer wells near the classical outer turning point supporting long-lived states, and inner wells at shorter range whose lifetimes are limited by tunneling and subsequent vibronic decay. Using photoassociation in an ultracold Cs gas and an analysis of pulsed-field-ionisation signals which are highly selective for the detection of molecules, we assign resonances by binding energy and measure lifetimes. The measured lifetimes of inner-well states increase systematically with increasing detuning and agree with calculated lifetimes; detection of Cs2+ product ions supports autoionisation as a dominant channel. We show that the lifetimes are strongly reduced by spin-orbit interactions in the transient Cs-collision complex, which lift the near-degeneracy in Omega observed for states in the outer well and control the inner-well binding. The identified states also provide promising pathways to create ultracold molecules in ion-pair states.