A quantum chemical study on gas phase decomposition pathways of triethylgallane (TEG, Ga(C2H5)3) and tert-butylphosphine (TBP, PH2(t-C4H9)) under MOVPE conditions
文献信息
Andreas Stegmüller, Phil Rosenow, Ralf Tonner
The gas phase decomposition reactions of precursor molecules relevant for metal–organic vapour phase epitaxy (MOVPE) of semiconductor thin films are investigated by computational methods on the density-functional level as well as on the ab initio (MP2, CCSD(T)) level. A comprehensive reaction catalogue of uni- and bimolecular reactions is presented for triethylgallium (TEG) as well as for tert-butylphosphine (TBP) containing thermodynamic data together with transition state energies. From these energies it can be concluded that TEG is decomposed in the gas phase under MOVPE conditions (T = 400–675 °C, p = 0.05 atm) to GaH3via a series of β-hydride elimination reactions. For elevated temperatures, further decomposition to GaH is thermodynamically accessible. In the case of TBP, the original precursor molecule will be most abundant since all reaction channels exhibit either large barriers or unfavorable thermodynamics. Dispersion-corrected density functional calculations (PBE-D3) provide an accurate description of the reactions investigated in comparison to high level CCSD(T) calculations serving as benchmark values.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.











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