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Absolute rate data are reported for reactions of ground state atomic caesium, Cs(6  2 S 1/2 ), with a wide range of alkyl chlorides and bromides at elevated temperatures following the broad band pulsed generation of the heavy alkali atom from CsI vapour in the presence of the halogenated reactants and excess helium buffer gas. Cs(6  2 S 1/2 ) was monitored by laser-induced fluorescence (LIF) in the time-domain using the shorter wavelength component of the Rydberg doublet transition at λ = 455.5 nm [Cs(7  3 P 3/2  – 6  2 S 1/2 )]. The LIF signals were captured in digital form and subject to computerised analysis. The following second-order rate constants are reported for reaction at essentially single elevated temperatures:  k R  /cm 3  molecule −1  s −1  CH 3 Cl (6.7 ± 0.1) × 10 −12  (860 K); C 3 H 7 Cl (8.7 ± 0.1) × 10 −12  (855 K); C 4 H 9 Cl (1.1 ± 0.1) × 10 −11  (855); C 5 H 11 Cl (8.2 ± 0.1) × 10 −12  (855 K); C 6 H 13 Cl (3.9 ± 0.1) × 10 −12  (855 K); C 7 H 15 Cl (4.5 ± 0.1) × 10 −12  (856 K); C 3 H 7 Br (1.7 ± 0.1) × 10 −11  (855 K); C 4 H 9 Br (1.2 ± 0.1) × 10 −11  (856 K); C 5 H 11 Br (1.5 ± 0.1) × 10 −11  (855 K); C 6 H 13 Br (5.9 ± 0.1) × 10 −12  (856 K); C 7 H 15 Br (5.9 ± 0.1) × 10 −12  (856 K). With the exception of CH 3 Cl, these represent a new body of absolute rate data for atomic caesium reported by any method. All the reactions reported here are exothermic though values of the appropriate thermochemistry cannot be accurately assigned in many cases as, whilst these may be sensibly estimated, the bond dissociation energies are not fully established. The rate data for the reaction of this alkali atom, characterised by a low ionisation potential, are mostly compared with absolute rate data for the lighter but heavy atomic rubidium, Rb(5  2 S 1/2 ), which has also a low ionisation potential. The diffusional behaviour of Cs(6  1 S 1/2 ) in He and Kr are also reported in this study.

zeitschrift für physikalische chemie

Absolute Rate Data for Halogen Atom-Abstraction Reactions of Ground State Atomic Caesium, Cs(6  2 S 1/2 ) Determined by Time-Resolved Laser-induced Fluorescence [Cs(7  2 P 3/2  – 6  2 S 1/2 ); λ = 455.5 nm] Following Pulsed Irradiation