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Physical Review A

Resonant Rydberg-atom — Rydbert-atom collisions

Thomas F. Gallagher, Kambiz Ali Safinya, F. Gounand, J. F. Delpech, Wolfgang Sandner, Ravinder Kachru

Published Apr 1, 1982• 50 citations
Publisher

Abstract

The experimental investigation of the resonant collision process $\mathrm{Na}ns+\mathrm{Na}\mathrm{ns}\ensuremath{\rightarrow}\mathrm{Na}np+\mathrm{Na}(n\ensuremath{-}1)p$ which occurs when the levels are tuned with an electric field so that the $\mathrm{ns}$ level lies midway between the two $p$ levels is described in detail. The observations are shown to be in good agreement with a long-range resonant dipole-dipole interaction.

DOI
10.1103/physreva.25.1905

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A careful numerical solution of the equations of the two-state theory of resonant collisions is presented. The particular process investigated is that of collisions of two sodium atoms in Rydberg states in the presence of a weak static electric field for which measurements have been carried out recently. Dipole-dipole interaction between the atoms is assumed as the interaction responsible for the transition. Comparison between calculations and experiments yields only moderately good agreement, this being ascribed mainly to simplifications adopted within the theoretical model.

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The experimental investigation of the resonant collision process Nans+Nans\ensuremath→Nanp+Na(n\ensuremath−1)p\mathrm{Na}ns+\mathrm{Na}\mathrm{ns}\ensuremath{\rightarrow}\mathrm{Na}np+\mathrm{Na}(n\ensuremath{-}1)pNans+Nans\ensuremath→Nanp+Na(n\ensuremath−1)p which occurs when the levels are tuned with an electric field so that the ns\mathrm{ns}ns level lies midway between the two ppp levels is described in detail. The observations are shown to be in good agreement with a long-range resonant dipole-dipole interaction.
We have observed the sharply resonant enhancement of the cross section of the collision process $ns+ns\ensuremath{\rightarrow}np+(n\ensuremath{-}1)p$ between two Nans\mathrm{Na}nsNans (16< n< 2716<~n<~2716< n< 27) atoms which occurs when the levels are shifted by an electric field so that the nsnsns level lies midway between the two ppp states. The widths of the collisional resonances scale as ${n}^{\ensuremath{-}2}$ and the magnitudes of the cross sections as n4{n}^{4}n4, with values of 0.5 GHz and 8\ifmmode\times\else\texttimes\fi{}108{10}^{8}108 A˚2{\mathrm{\AA{}}}^{2}A˚2 for the 20s20s20s state. These results are in good agreement with calculations based on the long-range dipole-dipole interaction between the two atoms.
A large enhancement in the resonant collisional energy-transfer process $\mathrm{Na}(\mathrm{ns})+\mathrm{Na}(\mathrm{ns})\ensuremath{\rightarrow}\mathrm{Na}[(n\ensuremath{-}1)p]+\mathrm{Na}(\mathrm{nl})$ or $\mathrm{Na}(\mathrm{ns})+\mathrm{Na}(\mathrm{ns})\ensuremath{\rightarrow}\mathrm{Na}(\mathrm{np})+\mathrm{Na}[(n\ensuremath{-}1)l]$ is observed when the initial ns\mathrm{ns}ns state lies midway between $(n\ensuremath{-}1)p$ and an nl\mathrm{nl}nl state or between np\mathrm{np}np and an $(n\ensuremath{-}1)l$ state. This resonance condition, achieved by the electric field tuning of the levels, leads to large cross sections \ensuremath{\sim} 109{10}^{9}109 A˚2{\mathrm{\AA{}}}^{2}A˚2 and narrow linewidths \ensuremath{\sim} 1 GHz. These cross sections and linewidths are comparable to the previously observed resonant process $\mathrm{Na}(\mathrm{ns})+\mathrm{Na}(\mathrm{ns})\ensuremath{\rightarrow}\mathrm{Na}[(n\ensuremath{-}1)p]+\mathrm{Na}(\mathrm{np})$. We have also observed a similar collisional energy transfer starting from a completely different initial state, i.e., $\mathrm{Na}(15d)+\mathrm{Na}(15d)\ensuremath{\rightarrow}\mathrm{Na}(16f)+\mathrm{Na}(15p)$. In this case the enhancement in the cross section (\ensuremath{\sim} 108{10}^{8}108 A˚2{\mathrm{\AA{}}}^{2}A˚2) is observed at a relatively low electric field \ensuremath{\sim} 17 V/cm.
We have observed resonant-energy-transfer collisions between K Rydberg atoms. We have tuned the ns1/2{\mathrm{ns}}_{1/2}ns1/2​+(n-2)dj{\mathrm{d}}_{\mathrm{j}}dj​\ensuremath{\rightarrow}${\mathrm{np}}_{\mathrm{j}\ensuremath{'}}$+(n-1)${\mathrm{p}}_{\mathrm{j}\mathrm{\ensuremath{''}}}$ collisional process into resonance with a static electric field. The measured resonance field positions from n=24 to 29 agree well with the calculated positions. We show that the dipole-dipole selection rule, \ensuremath{\Delta}mj{\mathrm{m}}_{\mathrm{j}}mj​=0,\ifmmode\pm\else\textpm\fi{}1, is valid for these resonances but that \ensuremath{\Delta}J=0,\ifmmode\pm\else\textpm\fi{}1 is not, due to the presence of the electric field. In addition, the polarization of the lasers used to excite the Rydberg states can suppress many of the resonances.
We describe the experimental observation of the resonant collisional energy transfer Na(ns)+Na(ns)+qh\ensuremath{\nu}\ensuremath{\rightarrow}Na(np)+Na[(n-1)p]+(q○)h\ensuremath{\nu} which occurs when the Na atoms in a strong microwave field are tuned in energy with a static field so that the energy resonance Ens{E}_{\mathrm{ns}}Ens​+Ens{E}_{\mathrm{ns}}Ens​=Enp{E}_{\mathrm{np}}Enp​+${E}_{n\mathrm{\ensuremath{-}}1}$,p\ifmmode\pm\else\textpm\fi{}mh\ensuremath{\nu} occurs. We describe our experimental observations and provide a detailed description of a nonperturbative theory which we have developed to explain our observations. The theory is essentially developed in terms of the resonant dipole-dipole collisions between ``microwave dressed'' atoms. Using an extension of the approach we used previously to describe resonant dipole-dipole collisions in the absence of microwaves, we are able to take into account all the coherences in the problem in a completely straightforward way.
Resonant collisional energy transfer can be studied in uprecedented detail using Rydberg atoms. Using the dependence of the energy level spacing on principal quantum number it is possible to examine resonant energy transfer in collisions with molecules. Finer control of the level spacing is possible by varying the level spacings with an electric field. Using this approach it is possible to observe sharply resonant collisions between Rydberg atoms. They are resonant dipole-dipole collisions which have cross sections orders of magnitude larger than the geometric cross sections of the colliding Rydberg atoms. These collisions are interesting in themselves; for example, they exhibit intracollisional interference, and it is possible to know when individual collisions begin and end. Perhaps the most interesting aspect of these collisions is that, because of the large dipole moments of the Rydberg atoms, they are easily controlled by microwave and radio frequency fields.
A careful numerical solution of the equations of the two-state theory of resonant collisions is presented. The particular process investigated is that of collisions of two sodium atoms in Rydberg states in the presence of a weak static electric field for which measurements have been carried out recently. Dipole-dipole interaction between the atoms is assumed as the interaction responsible for the transition. Comparison between calculations and experiments yields only moderately good agreement, this being ascribed mainly to simplifications adopted within the theoretical model.