Initial growth study of atomic-layer deposition of Al2O3 by vibrational sum-frequency generation

Vincent Vandalon (Corresponding author), Erwin Kessels (Corresponding author)

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The initial growth during the atomic-layer deposition (ALD) of Al2O3 using trimethylaluminum (TMA) and water was studied on two starting surfaces: SiO2 and −H-terminated Si(111) [H/Si(111)]. In situ spectroscopy ellipsometry (SE) showed virtually immediate growth of Al2O3 on both surfaces, although for H/Si(111) a reduced growth-per-cycle was observed in the initial 20 cycles. The underlying surface chemistry during the initial cycles of ALD was monitored with in situ broadband sum-frequency generation (BB-SFG) spectroscopy. For the SiO2 surface, the −CH3 surface groups were followed revealing that only the first TMA half-cycle deviates from the steady-growth regime. The reaction cross section of the initial TMA half-cycle (σTMA = 2.0 ± 0.2 × 10–18 cm2) was a factor of 3 lower than the cross section of the TMA half-cycle during the steady-growth regime of ALD (σTMA = 6.5 ± 0.6 × 10–18 cm2). All H2O half-cycles, including the first, showed steady-growth behavior with a corresponding reaction cross section (σH2O = 4.0 ± 0.4 × 10–20 cm2). Therefore, only the first ALD cycle was affected by initial growth effects on the SiO2 starting surface, in line with the SE data. For the H/Si(111) surface, the Si–H groups were monitored with BB-SFG spectroscopy, revealing a reaction cross section of σTMA = 3.1 ± 0.3 × 10–18 cm2 for the first TMA half-cycle on H/Si(111); a factor two lower than that during the steady regime of Al2O3. These results demonstrate that the chemistry during the initial growth regime of Al2O3 ALD on SiO2 and H/Si(111) shows subtle but measurable differences compared to the steady-growth regime.
Originele taal-2Engels
Pagina's (van-tot)10374-10382
Aantal pagina's9
TijdschriftLangmuir
Volume35
Nummer van het tijdschrift32
DOI's
StatusGepubliceerd - 13 aug 2019

Vingerafdruk

Atomic layer deposition
Vibrational spectra
atomic layer epitaxy
cycles
Spectroscopy
cross sections
Ellipsometry
spectroscopy
ellipsometry
chemistry
broadband
Surface chemistry
Water

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title = "Initial growth study of atomic-layer deposition of Al2O3 by vibrational sum-frequency generation",
abstract = "The initial growth during the atomic-layer deposition (ALD) of Al2O3 using trimethylaluminum (TMA) and water was studied on two starting surfaces: SiO2 and −H-terminated Si(111) [H/Si(111)]. In situ spectroscopy ellipsometry (SE) showed virtually immediate growth of Al2O3 on both surfaces, although for H/Si(111) a reduced growth-per-cycle was observed in the initial 20 cycles. The underlying surface chemistry during the initial cycles of ALD was monitored with in situ broadband sum-frequency generation (BB-SFG) spectroscopy. For the SiO2 surface, the −CH3 surface groups were followed revealing that only the first TMA half-cycle deviates from the steady-growth regime. The reaction cross section of the initial TMA half-cycle (σTMA = 2.0 ± 0.2 × 10–18 cm2) was a factor of 3 lower than the cross section of the TMA half-cycle during the steady-growth regime of ALD (σTMA = 6.5 ± 0.6 × 10–18 cm2). All H2O half-cycles, including the first, showed steady-growth behavior with a corresponding reaction cross section (σH2O = 4.0 ± 0.4 × 10–20 cm2). Therefore, only the first ALD cycle was affected by initial growth effects on the SiO2 starting surface, in line with the SE data. For the H/Si(111) surface, the Si–H groups were monitored with BB-SFG spectroscopy, revealing a reaction cross section of σTMA = 3.1 ± 0.3 × 10–18 cm2 for the first TMA half-cycle on H/Si(111); a factor two lower than that during the steady regime of Al2O3. These results demonstrate that the chemistry during the initial growth regime of Al2O3 ALD on SiO2 and H/Si(111) shows subtle but measurable differences compared to the steady-growth regime.",
author = "Vincent Vandalon and Erwin Kessels",
year = "2019",
month = "8",
day = "13",
doi = "10.1021/acs.langmuir.9b01600",
language = "English",
volume = "35",
pages = "10374--10382",
journal = "Langmuir",
issn = "0743-7463",
publisher = "American Chemical Society",
number = "32",

}

Initial growth study of atomic-layer deposition of Al2O3 by vibrational sum-frequency generation. / Vandalon, Vincent (Corresponding author); Kessels, Erwin (Corresponding author).

In: Langmuir, Vol. 35, Nr. 32, 13.08.2019, blz. 10374-10382.

Onderzoeksoutput: Bijdrage aan tijdschriftTijdschriftartikelAcademicpeer review

TY - JOUR

T1 - Initial growth study of atomic-layer deposition of Al2O3 by vibrational sum-frequency generation

AU - Vandalon, Vincent

AU - Kessels, Erwin

PY - 2019/8/13

Y1 - 2019/8/13

N2 - The initial growth during the atomic-layer deposition (ALD) of Al2O3 using trimethylaluminum (TMA) and water was studied on two starting surfaces: SiO2 and −H-terminated Si(111) [H/Si(111)]. In situ spectroscopy ellipsometry (SE) showed virtually immediate growth of Al2O3 on both surfaces, although for H/Si(111) a reduced growth-per-cycle was observed in the initial 20 cycles. The underlying surface chemistry during the initial cycles of ALD was monitored with in situ broadband sum-frequency generation (BB-SFG) spectroscopy. For the SiO2 surface, the −CH3 surface groups were followed revealing that only the first TMA half-cycle deviates from the steady-growth regime. The reaction cross section of the initial TMA half-cycle (σTMA = 2.0 ± 0.2 × 10–18 cm2) was a factor of 3 lower than the cross section of the TMA half-cycle during the steady-growth regime of ALD (σTMA = 6.5 ± 0.6 × 10–18 cm2). All H2O half-cycles, including the first, showed steady-growth behavior with a corresponding reaction cross section (σH2O = 4.0 ± 0.4 × 10–20 cm2). Therefore, only the first ALD cycle was affected by initial growth effects on the SiO2 starting surface, in line with the SE data. For the H/Si(111) surface, the Si–H groups were monitored with BB-SFG spectroscopy, revealing a reaction cross section of σTMA = 3.1 ± 0.3 × 10–18 cm2 for the first TMA half-cycle on H/Si(111); a factor two lower than that during the steady regime of Al2O3. These results demonstrate that the chemistry during the initial growth regime of Al2O3 ALD on SiO2 and H/Si(111) shows subtle but measurable differences compared to the steady-growth regime.

AB - The initial growth during the atomic-layer deposition (ALD) of Al2O3 using trimethylaluminum (TMA) and water was studied on two starting surfaces: SiO2 and −H-terminated Si(111) [H/Si(111)]. In situ spectroscopy ellipsometry (SE) showed virtually immediate growth of Al2O3 on both surfaces, although for H/Si(111) a reduced growth-per-cycle was observed in the initial 20 cycles. The underlying surface chemistry during the initial cycles of ALD was monitored with in situ broadband sum-frequency generation (BB-SFG) spectroscopy. For the SiO2 surface, the −CH3 surface groups were followed revealing that only the first TMA half-cycle deviates from the steady-growth regime. The reaction cross section of the initial TMA half-cycle (σTMA = 2.0 ± 0.2 × 10–18 cm2) was a factor of 3 lower than the cross section of the TMA half-cycle during the steady-growth regime of ALD (σTMA = 6.5 ± 0.6 × 10–18 cm2). All H2O half-cycles, including the first, showed steady-growth behavior with a corresponding reaction cross section (σH2O = 4.0 ± 0.4 × 10–20 cm2). Therefore, only the first ALD cycle was affected by initial growth effects on the SiO2 starting surface, in line with the SE data. For the H/Si(111) surface, the Si–H groups were monitored with BB-SFG spectroscopy, revealing a reaction cross section of σTMA = 3.1 ± 0.3 × 10–18 cm2 for the first TMA half-cycle on H/Si(111); a factor two lower than that during the steady regime of Al2O3. These results demonstrate that the chemistry during the initial growth regime of Al2O3 ALD on SiO2 and H/Si(111) shows subtle but measurable differences compared to the steady-growth regime.

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