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Physical Review A

Approximate scaling formula for collisional angular-momentum mixing of Rydberg atoms

A. P. Hickman

Published Jan 1, 1981• 50 citations
Publisher

Abstract

An approximate scaling formula has been determined that permits the rapid estimation of cross sections for angular-momentum-changing collisions of Rydberg atoms with a variety of targets, using information about low-energy-electron scattering from the target. The formula is obtained by fitting the results of coupled-channel and Born-approximation calculations to functions of reduced parameters. Application to $\mathrm{Na}(\mathrm{nd})$ + He, Ne, Ar, ${\mathrm{N}}_{2}$, C${\mathrm{H}}_{4}$, ${\mathrm{C}}_{3}$${\mathrm{H}}_{8}$; $\mathrm{Rb}(\mathrm{nf})$ + He, Ar, Xe; and $\mathrm{Xe}(\mathrm{nf})$ + C${\mathrm{O}}_{2}$, suggests that the accuracy is about a factor of 2.

DOI
10.1103/physreva.23.87

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Bulletin of the American Physical Society•May 1, 1993•0 citations
An approximate scaling formula has been determined that permits the rapid estimation of cross sections for angular-momentum-changing collisions of Rydberg atoms with a variety of targets, using information about low-energy-electron scattering from the target. The formula is obtained by fitting the results of coupled-channel and Born-approximation calculations to functions of reduced parameters. Application to Na(nd)\mathrm{Na}(\mathrm{nd})Na(nd) + He, Ne, Ar, N2{\mathrm{N}}_{2}N2​, CH4{\mathrm{H}}_{4}H4​, {\mathrm{C}}_{3}$${\mathrm{H}}_{8}; Rb(nf)\mathrm{Rb}(\mathrm{nf})Rb(nf) + He, Ar, Xe; and Xe(nf)\mathrm{Xe}(\mathrm{nf})Xe(nf) + CO2{\mathrm{O}}_{2}O2​, suggests that the accuracy is about a factor of 2.
Collisions of Rydberg atoms with other atoms may induce changes in the electronic orbital angular momentum of the Rydberg state. A theory is presented that expresses the cross section for this process in terms of the sss-wave amplitude for low-energy-electron scattering from the other atom. In its most accurate form, the theory requires a convolution of the electron-scattering amplitude and the initial momentum-space wave function of the Rydberg state. However, an approximate analytic solution is derived in which the lll-mixing cross section at a particular nnn is written as the electron-scattering cross section at the mean electronic kinetic energy of the Rydberg state, multiplied by a scaling function that depends only on nnn. The analytic solution clearly exhibits the asymptotic scaling behavior of the cross sections. Collisions of Na(nd)+He\mathrm{Na}(\mathrm{nd})+\mathrm{He}Na(nd)+He, Ne, and Ar are treated as specific examples.
A coupled-channel approach based on the Arthurs and Dalgarno formalism is presented to describe the scattering of a Rydberg atom and a rare-gas atom. The method permits the calculation of cross sections for changes in the electronic orbital angular momentum of the Rydberg atom. The theory explicitly relates the scattering behavior of the Rydberg state to the electron-rare-gas scattering length. Preliminary results for Na∗(nd){\mathrm{Na}}^{*}(\mathrm{nd})Na∗(nd)+He and Na∗(nf){\mathrm{Na}}^{*}(\mathrm{nf})Na∗(nf)+He are in good agreement with experiment.
The collisional angular-momentum mixing of $n=5\ensuremath{-}15$ Na ddd states with the l>2l>2l>2 states of the same nnn has been studied using He, Ne, and Ar as collision partners. At rare-gas pressures of \ensuremath{\sim}1 Torr, the $l\ensuremath{\ge}2$ states are thoroughly mixed and the mixture decays at the average radiative lifetime of all the $l\ensuremath{\ge}2$ states of the same nnn. Using \ensuremath{\sim}1 Torr of neon to collisionally mix the $l\ensuremath{\ge}2$ states, the average lifetime for $l\ensuremath{\ge}2$ was measured for each nnn and compared to the theoretical prediction for hydrogen, with which it is in excellent agreement. The cross section for lll mixing by each of the gases is found to increase sharply from n=5to10n=5 \mathrm{to} 10n=5to10 and decrease above n=10n=10n=10. The magnitudes of the lll-mixing cross sections are found to correlate with the low-energy scattering lengths of the collision partners.
For $20\ensuremath{\le}n\ensuremath{\le}45$, two types of quasielastic state-changing-collisional (QESCC) processes, i.e., (i) lll-changing and (ii) nnn-and lll-changing processes, have been theoretically investigated based on the free-electron model in which an excited Rydberg electron behaves as if it were "free" and slow with its interaction with a rare-gas atom playing a decisive role. It is shown that a parameter ${u}_{min}[=\frac{\ensuremath{\nu}{\ensuremath{\nu}}^{\ensuremath{'}}\ensuremath{\Delta}E{a}_{0}}{(\ensuremath{\hbar}V)}]$ is quite useful for characterizing both of these QESCC processes in a unified way where $\ensuremath{\nu}(\ensuremath{\simeq}{\ensuremath{\nu}}^{\ensuremath{'}})$ is an effective principal quantum number of the initial (final) state, $\ensuremath{\Delta}E$ is an energy defect, and VVV is a relative velocity. It is theoretically found that higher-angular-momentum states are dominantly populated in the final channel of these QESCC processes with $1<{u}_{min}\ensuremath{\lesssim}\ensuremath{\nu}$ such as in the nnn- and lll-changing collision of Rb∗∗(ns)+He{\mathrm{Rb}}^{**}(\mathrm{ns})+\mathrm{He}Rb∗∗(ns)+He. This is in contrast with the uniform distribution over the final angular-momentum states for the usual lll-changing processes, i.e., ${u}_{min}\ensuremath{\lesssim}1$. The calculated cross sections of these QESCC processes with $1<{u}_{min}\ensuremath{\lesssim}\ensuremath{\nu}$ are found to be in reasonable agreement with experimental findings available at present.
The analytical formulae for the cross-sections with arbitrary change {triangle}n=n{prime}-n and {triangle}1=1{prime}-1 has been obtained in the Born limit. No spin exchange {triangle}S=0: although the total cross-sections n->n are dominated by dipole transitions, the non-dipole transitions {triangle}1>1 can contribute up to 30-50%ER for large {triangle}n>>1. Intercombination transitions {triangle}S=1: the large transfer transitions {triangle}1>>1 are of major importance, as opposed to the previous case.