Abstract
Using crossed atomic, molecular cluster, and cw laser beams in conjunction with mass spectrometric ion detection, we have obtained for the first time results for electron transfer fromstate-selected Rydberg atoms to molecular clusters. We report negative ion mass spectra for (CO2) − (4≦k≦25) and (O2) − (1≦k≦13) cluster ions, resulting from collisions of Ar** (nd) Rydberg atoms (12≦n≦40) with (CO2) m and (O2) m clusters at relative velocities around 830 m/s, and, for comparison, positive ion mass spectra due to Ne(3s 3 P 2, 0) Penning ionization. For both CO 2 − and O2-clusters, the negative and the positive ion mass spectra are very different. For (CO2) Emphasis>/− cluster ions, the mass spectra show distinct variations with principal quantum number of the Rydberg atom, corresponding to differentn-dependences of the effective rate constant for selected cluster ions, as measured relative to the knownn-dependence for SF 6 − formation in collisions with SF6. For (O2) − cluster ions, on the other hand, the mass spectra are almost independent ofn with ion intensities, which clearly reflect their thermochemical stabilities (O 4 − as dominant species).
Published Version
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