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Physical Review A

Study of Rydberg-atom l -changing collisions using selective field ionization

F. G. Kellert, THOMAS H. JEYS, G. B. McMillian, K. A. Smith, F. B. Dunning, R. F. Stebbings

Published Mar 1, 1981• 53 citations
Publisher

Abstract

The excited products of collisions between xenon atoms and $\mathrm{Na}(\mathrm{nd})$ atoms with $n=37$ and $n=42$ have been investigated by use of selective field ionization (SFI). It is observed that, at an ionizing-field slew rate of \ensuremath{\sim} ${10}^{9}$ V/cm sec, most of the collision products follow predominantly diabatic paths to ionization which occurs at field strengths consistent with those predicted by quantum mechanical tunneling calculations. Detailed analysis of the SFI data indicates that the collision products have a wide (possibly complete) range of values of $l$ and ${m}_{j}$, although it is not clear whether the observed distribution results from single or multiple collisions. No evidence of $n$-changing collisions was seen. Similar data for collisions involving $\mathrm{Xe}(\mathrm{nf})$ atoms are briefly discussed.

DOI
10.1103/physreva.23.1127

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Physical Review Letters•Feb 11, 1980•140 citations
The excited products of collisions between xenon atoms and Na(nd)\mathrm{Na}(\mathrm{nd})Na(nd) atoms with n=37n=37n=37 and n=42n=42n=42 have been investigated by use of selective field ionization (SFI). It is observed that, at an ionizing-field slew rate of \ensuremath{\sim} 109{10}^{9}109 V/cm sec, most of the collision products follow predominantly diabatic paths to ionization which occurs at field strengths consistent with those predicted by quantum mechanical tunneling calculations. Detailed analysis of the SFI data indicates that the collision products have a wide (possibly complete) range of values of lll and mj{m}_{j}mj​, although it is not clear whether the observed distribution results from single or multiple collisions. No evidence of nnn-changing collisions was seen. Similar data for collisions involving Xe(nf)\mathrm{Xe}(\mathrm{nf})Xe(nf) atoms are briefly discussed.
Thermal collisions between Xe(nf) Rydberg atoms and HF molecules have been investigated. The highly excited collision products were detected using selective field ionisation (SFI). Both n-changing and l-changing collisions were identified and the absolute rate constants for these processes, and for collisional ionisation, have been measured for n=26, 27. In addition, the first evidence of molecular rotational excitation through the transfer of energy of electronic excitation from a Rydberg atom is presented.
Selective field ionization (SFI) is frequently used to detect atoms in high Rydberg states and to analyze Rydberg population distributions. In order to realize the full potential of this technique, however, a detailed understanding of the behavior of Rydberg atoms during passage from low to ionizing fields is required. The factors influencing this passage are discussed quantitatively and are illustrated by means of detailed SFI data obtained for Na34d\mathrm{Na}34dNa34d atoms.
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.
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.
The collisional angular-momentum mixing of the Nand\mathrm{Na}\mathrm{nd}Nand Rydberg states into states of higher angular momentum with Xe as the collisional partner has been studied in zero field and in the presence of a small electric field. The collisional lll-mixing cross section in zero field has been measured for $9\ensuremath{\le}n\ensuremath{\le}23$ using a vapor-cell-fluorescence method and a crossed-beam technique with a selective-field-ionization (SFI) scheme as the state detector. Using the ∣ml∣|{m}_{l}|∣ml​∣ selectivity of the SFI, we have also investigated the final-∣ml∣|{m}_{l}|∣ml​∣-state distribution of the collisionally populated states of l>2l>2l>2. Our measurements suggest that the collisionally populated states have predominantly low ∣ml∣|{m}_{l}|∣ml​∣ values ($|{m}_{l}|\ensuremath{\le}2$). An application of a low electric field (\ensuremath{\sim} 50 V/cm) substantially reduces the collisional population of the low-∣ml∣|{m}_{l}|∣ml​∣ states, thus reducing the total cross section as well.