Preparation and Characterization of Trimethylamine-Alane Thin Films on Oxidized Silicon

Fiona M. Elms; Robert N. Lamb; Paul J. Pigram; Michael G. Gardiner; Barry J. Wood; Colin L. Raston

doi:10.1021/cm00043a030

Preparation and Characterization of Trimethylamine-Alane Thin Films on Oxidized Silicon

Fiona M. Elms, Robert N. Lamb, Paul J. Pigram, Michael G. Gardiner, Barry J. Wood, Colin L. Raston

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Abstract

The surface adsorption characteristics of trimethylamine-alane, H₃AlNMe₃, on a SiO₂ substrate have been investigated using X-ray photoelectron spectroscopy and static secondary ion mass spectrometry. Molecular adsorption prevails at exposures of ~15 langmuirs with the aluminum centers becoming five-coordinate via binding to surface oxygen centers. High XPS X-ray flux (>240 W) results in migration of NMe₃ to silicon centers, ascertained by comparison with the adsorption of NMe₃ gas. At exposures greater than ~30 langmuirs an aluminum-rich species is formed, with the ratio of Al:N close to 2:1. Similar results are obtained for dosing of bis- (trimethylamine)-alane, H₃Al(NMe₃)₂. Ab initio molecular orbital calculations (HF/D95*) on H₃AlNH₃ and H₂O, and H₃AlOH₂, as model systems for the interaction of H₃AlNMe₃ with surface oxygen centers, gave formation of H₃AlNH₃(OH₂) as energetically favored by 4.53 kcal mol⁻¹ and its fragmentation to H₃AlOH₂ and NH₃ requiring 13.16 kcal mol⁻¹; association of H₃AlOH₂ and H₃AlNH₃ to H₂(NH₃)Al(µ-H)₂Al(OH₂)H₂, as a model for the aluminum-rich species, is also favored by 3.39 and 3.24 kcal mol⁻¹ for two isomers with different orientations of the H atoms on sp³ oxygen.

Original language	English
Pages (from-to)	1059-1066
Number of pages	8
Journal	Chemistry of Materials
Volume	6
Issue number	7
DOIs	https://doi.org/10.1021/cm00043a030
Publication status	Published - 1 Jul 1994
Externally published	Yes

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@article{a37c39acedc24fc58025456e512c5419,

title = "Preparation and Characterization of Trimethylamine-Alane Thin Films on Oxidized Silicon",

abstract = "The surface adsorption characteristics of trimethylamine-alane, H3AlNMe3, on a SiO2 substrate have been investigated using X-ray photoelectron spectroscopy and static secondary ion mass spectrometry. Molecular adsorption prevails at exposures of ~15 langmuirs with the aluminum centers becoming five-coordinate via binding to surface oxygen centers. High XPS X-ray flux (>240 W) results in migration of NMe3 to silicon centers, ascertained by comparison with the adsorption of NMe3 gas. At exposures greater than ~30 langmuirs an aluminum-rich species is formed, with the ratio of Al:N close to 2:1. Similar results are obtained for dosing of bis- (trimethylamine)-alane, H3Al(NMe3)2. Ab initio molecular orbital calculations (HF/D95*) on H3AlNH3 and H2O, and H3AlOH2, as model systems for the interaction of H3AlNMe3 with surface oxygen centers, gave formation of H3AlNH3(OH2) as energetically favored by 4.53 kcal mol−1 and its fragmentation to H3AlOH2 and NH3 requiring 13.16 kcal mol−1; association of H3AlOH2 and H3AlNH3 to H2(NH3)Al(µ-H)2Al(OH2)H2, as a model for the aluminum-rich species, is also favored by 3.39 and 3.24 kcal mol−1 for two isomers with different orientations of the H atoms on sp3 oxygen.",

author = "Elms, {Fiona M.} and Lamb, {Robert N.} and Pigram, {Paul J.} and Gardiner, {Michael G.} and Wood, {Barry J.} and Raston, {Colin L.}",

year = "1994",

month = jul,

day = "1",

doi = "10.1021/cm00043a030",

language = "English",

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pages = "1059--1066",

journal = "Chemistry of Materials",

issn = "0897-4756",

publisher = "American Chemical Society",

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T1 - Preparation and Characterization of Trimethylamine-Alane Thin Films on Oxidized Silicon

AU - Elms, Fiona M.

AU - Lamb, Robert N.

AU - Pigram, Paul J.

AU - Gardiner, Michael G.

AU - Wood, Barry J.

AU - Raston, Colin L.

PY - 1994/7/1

Y1 - 1994/7/1

N2 - The surface adsorption characteristics of trimethylamine-alane, H3AlNMe3, on a SiO2 substrate have been investigated using X-ray photoelectron spectroscopy and static secondary ion mass spectrometry. Molecular adsorption prevails at exposures of ~15 langmuirs with the aluminum centers becoming five-coordinate via binding to surface oxygen centers. High XPS X-ray flux (>240 W) results in migration of NMe3 to silicon centers, ascertained by comparison with the adsorption of NMe3 gas. At exposures greater than ~30 langmuirs an aluminum-rich species is formed, with the ratio of Al:N close to 2:1. Similar results are obtained for dosing of bis- (trimethylamine)-alane, H3Al(NMe3)2. Ab initio molecular orbital calculations (HF/D95*) on H3AlNH3 and H2O, and H3AlOH2, as model systems for the interaction of H3AlNMe3 with surface oxygen centers, gave formation of H3AlNH3(OH2) as energetically favored by 4.53 kcal mol−1 and its fragmentation to H3AlOH2 and NH3 requiring 13.16 kcal mol−1; association of H3AlOH2 and H3AlNH3 to H2(NH3)Al(µ-H)2Al(OH2)H2, as a model for the aluminum-rich species, is also favored by 3.39 and 3.24 kcal mol−1 for two isomers with different orientations of the H atoms on sp3 oxygen.

AB - The surface adsorption characteristics of trimethylamine-alane, H3AlNMe3, on a SiO2 substrate have been investigated using X-ray photoelectron spectroscopy and static secondary ion mass spectrometry. Molecular adsorption prevails at exposures of ~15 langmuirs with the aluminum centers becoming five-coordinate via binding to surface oxygen centers. High XPS X-ray flux (>240 W) results in migration of NMe3 to silicon centers, ascertained by comparison with the adsorption of NMe3 gas. At exposures greater than ~30 langmuirs an aluminum-rich species is formed, with the ratio of Al:N close to 2:1. Similar results are obtained for dosing of bis- (trimethylamine)-alane, H3Al(NMe3)2. Ab initio molecular orbital calculations (HF/D95*) on H3AlNH3 and H2O, and H3AlOH2, as model systems for the interaction of H3AlNMe3 with surface oxygen centers, gave formation of H3AlNH3(OH2) as energetically favored by 4.53 kcal mol−1 and its fragmentation to H3AlOH2 and NH3 requiring 13.16 kcal mol−1; association of H3AlOH2 and H3AlNH3 to H2(NH3)Al(µ-H)2Al(OH2)H2, as a model for the aluminum-rich species, is also favored by 3.39 and 3.24 kcal mol−1 for two isomers with different orientations of the H atoms on sp3 oxygen.

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DO - 10.1021/cm00043a030

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SN - 0897-4756

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SP - 1059

EP - 1066

JO - Chemistry of Materials

JF - Chemistry of Materials

IS - 7

ER -

Preparation and Characterization of Trimethylamine-Alane Thin Films on Oxidized Silicon

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