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Physical Review A

Influence of an applied electric field on state changing in xenon-Rydberg-atom—xenon collisions

Morgan P. Slusher, C. Higgs, K. A. Smith, F. B. Dunning, R. F. Stebbings

Published Sep 1, 1982• 15 citations
Publisher

Abstract

The influence of an applied electric field on state changing in collisions between laser-excited $\mathrm{Xe}(\mathrm{nf})$ atoms and xenon target gas is described. The presence of the field results in marked changes in both the rate constant for collisional state changing and the final-state distribution. The changes can be generally understood in terms of energy-transfer arguments based on the "essentially-free" electron model, although the degree of spatial overlap between the wave functions associated with the initial and final states may also be important.

DOI
10.1103/physreva.26.1350

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We have observed resonant-energy-transfer collisions between K Rydberg atoms. We have tuned the ${\mathrm{ns}}_{1/2}$+(n-2)${\mathrm{d}}_{\mathrm{j}}$\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}${\mathrm{m}}_{\mathrm{j}}$=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.

Physical Review A•Feb 1, 1994•7 citations
The influence of an applied electric field on state changing in collisions between laser-excited Xe(nf)\mathrm{Xe}(\mathrm{nf})Xe(nf) atoms and xenon target gas is described. The presence of the field results in marked changes in both the rate constant for collisional state changing and the final-state distribution. The changes can be generally understood in terms of energy-transfer arguments based on the "essentially-free" electron model, although the degree of spatial overlap between the wave functions associated with the initial and final states may also be important.
Studies of Rydberg atom collision processes, especially those with small reaction rate constants, are frequently complicated by spurious background signals associated with photoionization by thermal blackbody radiation and with ionization resulting from collisions with background gas. Here we demonstrate that the magnitude and relative importance of the signals that result from these processes are strongly influenced by the presence of an applied electric field. Possible causes of this dependence are discussed.
The theory of collisions of Rydberg atoms with rare-gas atoms is generalized to include the effects of an applied static electric field. Two effects occur. First, the field causes the states to split, and the increased energy separations lead to a decrease in the inelastic cross sections. Second, there is a change in the form of the wave functions, because the various Stark states in the field have electron charge distributions that may be localized in very different regions of space. The present work focuses on this second effect. With the description of the initial and final Stark states of the Rydberg atom by the proper electronic wave functions obtained in parabolic coordinates, cross sections are obtained for a variety of specific transitions of Rydberg atoms (n=10,15,and20n=10, 15, \mathrm{and} 20n=10,15,and20) caused by collisions. The calculations are strictly valid for hydrogen, but exhibit general features that are expected to apply to other Rydberg atoms as well. The results show a dramatic effect on the cross section for particular transitions depending on the degree of overlap of the initial and final charge distributions. In addition, it is observed that transitions are favored that involve small changes in the azimuthal quantum number mmm. The origin of this tendency is discussed.
Thermal collisions between laser excited Xe(nf) Rydberg atoms and a variety of neutral atomic and molecular targets have been investigated. In Xe(nf)-HF collisions, n-changing, 4-changing and collisional ionization were observed. For n = 26 and 27, absolute collisional cross sections for these processes have been determined using time-resolved selective field ionization. In addition, the first evidence of molecular rotational excitation through the transfer of energy of electronic excitation from a Rydberg atom is presented. In Xe(nf) - Xe, Kr, Ar, CO2, CO and N2 collisions the dominant mechanism was observed to be 4-changing: no evidence of n-changing or collisional ionization was apparent. Absolute collisional cross sections have been determined for a range of n between 24 and 37. Comparison of these cross sections with those obtained using a theoretical model in which effects due to the Rydberg core are ignored appears to lead to satisfactory results only for Xe, Kr and CO2, whereas when core effects are included satisfactory agreement between experiment and theory is found in all cases.
In thermal collisions between Xe(nf) Rydberg atoms and NH(,3) collisional depopulation of the nf state occurs through at least three distinct mechanisms: n-changing collisions, l-changing collisions, and ionizing collisions. Using selective field ionization, the total collisional depopulation rate constants k(,d) are measured for laser-excited Xe(nf) atoms in the n range of 22 to 39. The magnitudes of k(,d) are large, corresponding to reaction cross sections comparable to the geometric size of the Xe(nf) atom at n = 22. In the n range of 25 to 40, Xe('+) ion production provides an absolute measure of the rate constants for collisional ionization. Approximate rate constants for n-and l-changing collisions are also presented for the 31f state. In these experiments, one finds that the state-changing collision rate constants are fairly independent of n and are determined largely by the l-changing collisions. The collisional ionization rate constants measured are smaller than the state-changing rate constants and increase with increasing n, ranging between 0.2 and 4.6 x 10('-7) cm('3)/sec for n between 25 and 40. The present results are compared to those of recent theoretical calculations.
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.
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.