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AsH3 ultraviolet photochemistry.

L A Smith-Freeman1, W P Schroeder, C Wittig

  • 1Department of Chemistry, University of Southern California, Los Angeles, California 90089, USA.

The Journal of Physical Chemistry. A
|February 5, 2009
PubMed
Summary
This summary is machine-generated.

High-n Rydberg time-of-flight spectroscopy revealed that 193.3 nm photolysis of arsine (AsH3) leads to significant internal excitation and rotation in the resulting AsH2 fragments. This study offers insights into group-V hydride photochemistry.

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Area of Science:

  • Chemical Physics
  • Molecular Spectroscopy
  • Photochemistry

Background:

  • Understanding the photolysis of group-V hydrides is crucial for elucidating their chemical reactivity and energy disposal pathways.
  • Arsine (AsH3) presents a unique case, bridging nonrelativistic and relativistic electronic effects.

Purpose of the Study:

  • To investigate the 193.3 nm photolysis of arsine (AsH3) using high-n Rydberg time-of-flight spectroscopy.
  • To determine the translational energy distribution and internal excitation of fragments produced from AsH3 photodissociation.
  • To explore the role of secondary photodissociation of AsH2 fragments.

Main Methods:

  • High-n Rydberg time-of-flight spectroscopy was employed to probe the dissociation dynamics.
  • Analysis of center-of-mass translational energy distributions (P(E(c.m.))) provided insights into energy partitioning.
  • Examination of spectral features revealed internal excitation and rotational dynamics of AsH2.

Main Results:

  • The primary photolysis channel, AsH3 + hν → AsH2 + H, results in AsH2 internal excitation accounting for ~64% of the available energy.
  • Evidence for secondary photodissociation of AsH2 was observed.
  • AsH2 fragments were found to possess significant a-axis rotation and bending excitation.

Conclusions:

  • The observed energy disposal in AsH3 photolysis supports proposed reaction mechanisms, especially when compared to lighter group-V hydrides.
  • The electronic structure of AsH3 necessitates advanced theoretical calculations due to its intermediate relativistic character.
  • This study contributes to a deeper understanding of molecular photodissociation dynamics and chemical bonding in p-block element hydrides.