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Photoionization mass spectrometric studies of AsH/sub n/ (n = 1--3)

Journal Article · · J. Chem. Phys.; (United States)
OSTI ID:6726683

The photoion yield curves of the free radicals AsH and AsH/sub 2/, prepared by the reaction of H atoms with AsH/sub 3/, have been measured. The adiabatic ionization potential of AsH (forming AsH/sup +/, X /sup 2/Pi/sub 1//sub ///sub 2/) is 9.641 +- 0.008 eV. Autoionizing Rydberg states are observed and analyzed to converge to an a /sup 4//Sigma//sup -/ state lying 1.94 eV higher in energy. The adiabatic ionization potential of AsH/sub 2/ (forming AsH/sup +//sub 2/, X /sup 1/A/sub 1/) is 9.443 +- 0.007 eV. The /sup 3/B/sub 1/ state of AsH/sup +//sub 2/ is conservatively estimated from the spectrum to lie 0.60--1.46 eV higher in energy, with the lower figure expected to be close to the true value. In addition, the ion yield curves of AsH/sup +//sub 3/, AsH/sup +//sub 2/, and AsH/sup +/ from photoionization of AsH/sub 3/ have been measured. From these measurements, the adiabatic ionization potential of AsH/sub 3/ is 9.82 +- 0.01 eV, the appearance potential of AsH/sup +//sub 2/ (+H) is 12.69 +- 0.01 eV, and that of AsH/sup +/(+H/sub 2/) is 11.295 +- 0.05 eV. The latter two measurements, when combined with the corresponding ionization potentials, yield D/sub 0/(H/sub 2/As--H) = 74.9 +- 0.2 kcal/mol and D/sub 0/(HAs--H) = 66.5 +- 0.2 kcal/mol. The value of D/sub 0/(As--H), as deduced from these measurements, depends upon an accurate heat of atomization of AsH/sub 3/, which in turn requires an accurate value for /Delta//sup circle-open//sub f//sub =/ (As,g). An analysis of alternative values is presented, from which D/sub 0/(As--H) = 64.6 +- 0.7 kcal/mol (2.80 +- 0.03 eV) is obtained.

Research Organization:
Chemistry Division, Argonne National Laboratory, Argonne, Illinois 60439
OSTI ID:
6726683
Journal Information:
J. Chem. Phys.; (United States), Journal Name: J. Chem. Phys.; (United States) Vol. 89:12; ISSN JCPSA
Country of Publication:
United States
Language:
English