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We present a kinetic study of reactions of ground state atomic calcium, Ca[4 s  2 ( 1  S  0 )], with alkyl bromides at elevated temperature by time-resolved atomic resonance absorption spectroscopy.  Atomic calcium in its electronic ground state was generated by the broad band pulsed photodissociation of CaI 2  vapour in the presence of various reactants and excess helium buffer gas and monitored in absorption at λ = 422.673 nm {Ca[4 p ( 1  P  1 )] ← {Ca[4 s  2 ( 1  S  0 )]}. Atomic decay profiles were recorded digitally in the ‘single-shot mode’ in the time-domain using resonance radiation from a highly intense microwave-powered sealed atomic emission source and subject to computer analysis.  Absolute second-order rate data at elevated temperature are reported for reactions of ground state calcium atoms with the following Br-containing reactants at  T  = 873 K :  k  R /cm 3  molecule -1  s -1  CH 3 Br (4.4 ± 0.3) · 10 -12 , C 2 H 5 Br (1.4 ± 0.1) · 10 -12 , C 3 H 7 Br (1.2 ± 0.1) · 10 -12 , C 4 H 9 Br (8.5 ± 0.6) · 10 -13 , C 5 H 11 Br (9.4 ± 0.7) · 10 -13 , C 6 H 13 Br (5.9 ± 0.5) · 10 -13 , C 7 H 15 Br (6.6 ± 1.0) · 10 -13 , CH 2 Br 2  (3.1 ± 0.2) · 10 -12  and 1,2-C 2 H 4 Br 2  (1.0 ± 0.1 · 10 -12 ).  These data, representing a totally new body of absolute rate measurements for the calcium atom, exhibiting small steric effects, are compared with analogous rate data for reactions of atomic calcium with other halides determined hitherto by variants of time-resolved atomic resonance absorption spectroscopy following pulsed irradiation at elevated temperatures in the ‘single-shot mode’.

zeitschrift für physikalische chemie

Measurements of the Rates of Reactions of Ground State Atomic Calcium, Ca[4 s  2 ( 1  S  0 )], with Alkyl Bromides at Elevated Temperature by Time-Resolved Atomic Resonance Absorption Spectroscopy [Ca(4 1  P  1  - 4 1  S  0 ); λ = 422.7 nm]