Thermal decomposition of trimethylindium and indium trisguanidinate precursors for InN growth: An ab initio and kinetic modeling study
2023 (English)In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 158, no 17, article id 174313Article in journal (Refereed) Published
Abstract [en]
Indium nitride (InN) is an interesting material for future electronic and photonic-related applications, as it combines high electron mobility and low-energy band gap for photoabsorption or emission-driven processes. In this context, atomic layer deposition techniques have been previously employed for InN growth at low temperatures (typically <350 °C), reportedly yielding crystals with high quality and purity. In general, this technique is assumed to not involve any gas phase reactions as a result from the time-resolved insertion of volatile molecular sources into the gas chamber. Nonetheless, such temperatures could still favor the precursor decomposition in the gas phase during the In half-cycle, therefore altering the molecular species that undergoes physisorption and, ultimately, driving the reaction mechanism to pursue other pathways. Thence, we herein evaluate the thermal decomposition of relevant In precursors in the gas phase, namely, trimethylindium (TMI) and tris(N,N′-diisopropyl-2-dimethylamido-guanidinato) indium (III) (ITG), by means of thermodynamic and kinetic modeling. According to the results, at T = 593 K, TMI should exhibit partial decomposition of ∼8% after 400 s to first generate methylindium and ethane (C2H6), a percentage that increases to ∼34% after 1 h of exposure inside the gas chamber. Therefore, this precursor should be present in an intact form to undergo physisorption during the In half-cycle of the deposition (<10 s). On the other hand, the ITG decomposition starts already at the temperatures used in the bubbler, in which it slowly decomposes as it is evaporated during the deposition process. At T = 300 °C, the decomposition is a fast process that reaches 90% completeness after 1 s and where equilibrium, at which almost no ITG remains, is achieved before 10 s. In this case, the decomposition pathway is likely to occur via elimination of the carbodiimide ligand. Ultimately, these results should contribute for a better understanding of the reaction mechanism involved in the InN growth from these precursors.
Place, publisher, year, edition, pages
AIP Publishing , 2023. Vol. 158, no 17, article id 174313
Keywords [en]
Atomic Layer Deposition (ALD), Density Functional Theory (DFT), Indium nitride, trimethylindium, indiumtrisguanidinate
National Category
Theoretical Chemistry
Identifiers
URN: urn:nbn:se:liu:diva-194227DOI: 10.1063/5.0148070ISI: 001010643300002PubMedID: 37144715Scopus ID: 2-s2.0-85157988578OAI: oai:DiVA.org:liu-194227DiVA, id: diva2:1760246
Funder
Swedish Research Council
Note
Funding: Swedish Foundation for Strategic Research (SSF) through the project "Time-Resolved Low temperature CVD; Swedish Research Council (VR); [SSF-RMA 15-0018]
2023-05-292023-05-292026-02-16