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The Journal of Chemical Physics

Associative ionization in collisions of K(n d) Rydberg atoms with molecules

A. Kalamarides, C. W. Walter, Byron George Zollars, K. A. Smith, F. B. Dunning

Published Oct 1, 1987• 3 citations
Publisher

Abstract

Measurements of associative ionization in collisions of K(nd) Rydberg atoms with a variety of molecular targets are reported, demonstrating that the Rydberg electron can serve as a catalyst to promote reactions involving the Rydberg core ion.
DOI
10.1063/1.452880

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In the present work very-high-n Rydberg-atoms (nsim100−nsim400)(n \\sim 100 - n \\sim 400)(nsim100−nsim400) are used to probe electron-molecule collisions at ultra-low electron energies. Based on the essentially-free-electron model, for sufficiently high n, Rydberg atom-molecule collisions can be described in terms of a binary interaction between the target molecule and the essentially-free Rydberg electron. Since the average kinetic energy of the Rydberg electron is ultra-low rm(sim85mueV−sim1.4meV),\\rm({\\sim}85\\mu eV - {\\sim}1.4meV),rm(sim85mueV−sim1.4meV), analysis of the very-high-n Rydberg-atom collision data can provide information on electron-molecule scattering at electron energies corresponding to electron temperatures of only $\\sim111\\sp\\circ$K, which are far below those accessible using any alternate approach.\nRate constants for destruction of very-high-n Rydberg atoms in collisions with various target molecules have been measured. This study focuses on Rydberg electron transfer to an electron-attaching molecule which results in negative ion formation via the reactions rmK(itnp/)+XYtoKsp++(XY)sp−∗ortoKsp++Xsp−+Yeqno(1)\\rm K({\\it np\\/}) + XY \\to K\\sp+ + (XY)\\sp{-*}\\ or\\ \\to K\\sp+ + X\\sp- + Y\\eqno(1)rmK(itnp/)+XYtoKsp++(XY)sp−∗ortoKsp++Xsp−+Yeqno(1)and on rotational energy transfer from polar molecules which leads to Rydberg atom ionization rmK(itnp/)+XY(itJ/)toKsp++itesp−+XY(itJ/−1)eqno(2)\\rm K({\\it np\\/}) + XY({\\it J\\/}) \\to K\\sp+ + {\\it e}\\sp- + XY({\\it J\\/}-1)\\eqno(2)rmK(itnp/)+XY(itJ/)toKsp++itesp−+XY(itJ/−1)eqno(2)\nThe n dependence of the rate constants for Rydberg-atom destruction depends on the reactions involved. In reaction (1) the rate constant is independent of n whereas in reaction (2) it increases nearly linearly with n. When both reactions are possible, the measured n dependence can be explained in terms of contributions from each process.\nThe essentially-free-electron model suggests that the n dependence of the rate constants for Rydberg-atom destruction reflects the energy dependence of the cross sections of the corresponding free electron-molecule collision processes which are $$\\eqalignno{&e\\sp- + \\rm XY \\to (XY)\\sp{-*}\\ or\\ \\to X\\sp- + Y&(1\\sp\\prime)\\cr &e\\sp- + \\rm XY({\\it J\\/}) \\to {\\it e}\\sp- + XY({\\it J\\/}-1)&(2\\sp\\prime)\\cr}$$Analysis of the data therefore provides the behavior of cross sections for these processes at ultra-low electron energies.