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Le Journal de Physique Colloques

RADIATIVE COLLISIONS IN A STRONG FIELD REGIME

P. Pillet, Ravinder Kachru, Nam Huu Tran, W. W. Smith, Thomas F. Gallagher

Published Jan 1, 1985• 1 citation
Publisher

Abstract

The process of resonant collisional energy transfer between Rydberg atoms provides an ideal starting point for systematic studies of radiatively assisted collisions. In fact using modest, readily available microwave sources it is straightforward to enter the strong field regime for such processes.
DOI
10.1051/jphyscol:1985108

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Physics Reports•Jan 1, 1992•21 citations
The observation of radiative collisions in the strong-field regime is reported, specifically the multiphoton-microwave-assisted resonant collisional energy-transfer process $\mathrm{Na}(\mathrm{ns})+\mathrm{Na}(\mathrm{ns})\ensuremath{\rightarrow}\mathrm{Na}(\mathrm{np})+\mathrm{Na}((n\ensuremath{-}1)p)+mh\ensuremath{\nu}$, where mmm is as high as 4. By use of a "dressed-atom" approach in a low-frequency (or adiabatic) approximation, a theoretical interpretation valid for the strong-field regime is given which is in good agreement with the present experimental results.
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 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 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.
A radiative collision is a resonant energy transfer collision in which two atoms absorb or emit photons during the collision. Alternatively, a radiative collision is the emission or absorption of a photon from a transient molecule, and, as shown by Gallagher and Holstein, radiative collisions can also be described in terms of line broadening. In a line broadening experiment there are typically many atoms and weak radiation fields, and in a radiative collision experiment there are few atoms and intense radiation fields. The only real difference is whether there are many atoms or many photons. Due to the short collision times, ∼10 −12 s, simply observing radiative collisions between low lying states requires high optical powers, and entering the regime where the optical field is no longer a minor perturbation seems unlikely. Due to their long collision times and large dipole moments, Rydberg atoms provide the ideal system in which to study radiative collisions in a quantitative fashion. As we shall see, it is straightforward to enter the strong field regime in which the radiation field, a microwave or rf field to be precise, is no longer a minor perturbation. Ironically, while the experiments are radiative collision experiments, with few atoms and many photons, the description of the strong field regime is given in terms of dressed molecular states, which is more similar to a line broadening description.