A comprehensive ab initio study of gallium and arsenic containing molecules

Theoretical calculations for the ground states of arsine (AsH$\sb3$), trimethylgallium (TMG) (Ga(CH$\sb3$)$\sb3$), the arsine$\cdot$TMG adduct, gallane (GaH$\sb3$), the gallane$\cdot$arsine adduct, small Ga$\sb{x}$As$\sb{y}$ clusters (x = y; x = 2-4), and small gallium hydrides are carried out at the self consistent field (SCF) Hartree-Fock level of theory, using analytic energy gradients for rapid geometry optimization. In addition, the SCF results are compared with theoretical predictions obtained at the coupled cluster level of theory including all single and double excitations, (CCSD). The precursors to the formation of GaAs, arsine and TMG, were determined to be of C$\sb{3v}$ and C$\sb3$ symmetries, respectively, while gallane was found to be D$\sb{3h}$ The equilibrium structures for Ga$\sb2$As$\sb2$, Ga$\sb3$As$\sb3$, and Ga$\sb4$As$\sb4$ are found to be of D$\sb{2h}$, C$\sb1$, and C$\sb{i}$ symmetry, respectively. The adduct binding energies and vibrational frequencies (SCF) are also obtained resulting in two stable bonded adduct species, arsine$\cdot$TMG of symmetry point group C$\sb3$ and arsine$\cdot$gallane of C$\sb{3v}$ symmetry. Finally, our theoretical predictions support a slightly exothermic gas-phase reaction yielding GaAs through a TMG$\cdot$AsH$\sb3$ adduct which is formed without an activation barrier.

Name thesis:degree_name

Master of Arts

Level thesis:degree_level

Masters

Discipline thesis:degree_discipline

Natural Sciences

Grantor

Rice University

Year dc:date.issued

1992

Author dc:creator

• Graves, Richard Marshall

Advisor dc:contributor.advisor

• Scuseria, Gustavo E.

• Physical chemistry

Statement dc:rights

• Copyright is held by the author, unless otherwise indicated. Permission to reuse, publish, or reproduce the work beyond the bounds of fair use or other exemptions to copyright law must be obtained from the copyright holder.

Language dc:language.iso

eng

Handle dc:identifier.uri

https://hdl.handle.net/1911/13606

OAI identifier oai:identifier

oai:repository.rice.edu:1911/13606