Chemical analysis of the interface between hybrid organic−inorganic perovskite and atomic layer deposited Al2O3

D. Koushik, L. Hazendonk, V. Zardetto, V. Vandalon, M.A. Verheijen, W.M.M. Kessels, M. Creatore (Corresponding author)

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Ultrathin metal oxides prepared by atomic layer deposition (ALD) have gained utmost attention as moisture and thermal stress barrier layers in perovskite solar cells (PSCs). We have recently shown that 10 cycles of ALD Al2O3 deposited directly on top of the CH3NH3PbI3–xClx perovskite material, are effective in delivering a superior PSC performance with 18% efficiency (compared to 15% of the Al2O3-free cell) with a long-term humidity-stability of more than 60 days. Motivated by these results, the present contribution focuses on the chemical modification which the CH3NH3PbI3–xClx perovskite undergoes upon growth of ALD Al2O3. Specifically, we combine in situ Infrared (IR) spectroscopy studies during film growth, together with X-ray photoelectron spectroscopy (XPS) analysis of the ALD Al2O3/perovskite interface. The IR-active signature of the NH3+ stretching mode of the perovskite undergoes minimal changes upon exposure to ALD cycles, suggesting no diffusion of ALD precursor and co-reactant (Al(CH3)3 and H2O) into the bulk of the perovskite. However, by analyzing the difference between the IR spectra associated with the Al2O3 coated perovskite and the pristine perovskite, respectively, changes occurring at the surface of perovskite are monitored. The abstraction of either NH3 or CH3NH2 from the perovskite surface is observed as deduced by the development of negative N–H bands associated with its stretching and bending modes. The IR investigations are corroborated by XPS study, confirming the abstraction of CH3NH2 from the perovskite surface, whereas no oxidation of its inorganic framework is observed within the ALD window process investigated in this work. In parallel, the growth of ALD Al2O3 on perovskite is witnessed by the appearance of characteristic IR-active Al–O–Al phonon and (OH)–Al═O stretching modes. Based on the IR and XPS investigations, a plausible growth mechanism of ALD Al2O3 on top of perovskite is presented.
Originele taal-2Engels
Pagina's (van-tot)5526-5535
Aantal pagina's10
TijdschriftACS Applied Materials & Interfaces
Volume11
Nummer van het tijdschrift5
DOI's
StatusGepubliceerd - 6 feb 2019

Vingerafdruk

Perovskite
Atomic layer deposition
Chemical analysis
Infrared radiation
Stretching
X ray photoelectron spectroscopy
perovskite
Chemical modification
Film growth
Thermal stress
Oxides
Infrared spectroscopy
Atmospheric humidity
Moisture
Metals
Oxidation

Citeer dit

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title = "Chemical analysis of the interface between hybrid organic−inorganic perovskite and atomic layer deposited Al2O3",
abstract = "Ultrathin metal oxides prepared by atomic layer deposition (ALD) have gained utmost attention as moisture and thermal stress barrier layers in perovskite solar cells (PSCs). We have recently shown that 10 cycles of ALD Al2O3 deposited directly on top of the CH3NH3PbI3–xClx perovskite material, are effective in delivering a superior PSC performance with 18{\%} efficiency (compared to 15{\%} of the Al2O3-free cell) with a long-term humidity-stability of more than 60 days. Motivated by these results, the present contribution focuses on the chemical modification which the CH3NH3PbI3–xClx perovskite undergoes upon growth of ALD Al2O3. Specifically, we combine in situ Infrared (IR) spectroscopy studies during film growth, together with X-ray photoelectron spectroscopy (XPS) analysis of the ALD Al2O3/perovskite interface. The IR-active signature of the NH3+ stretching mode of the perovskite undergoes minimal changes upon exposure to ALD cycles, suggesting no diffusion of ALD precursor and co-reactant (Al(CH3)3 and H2O) into the bulk of the perovskite. However, by analyzing the difference between the IR spectra associated with the Al2O3 coated perovskite and the pristine perovskite, respectively, changes occurring at the surface of perovskite are monitored. The abstraction of either NH3 or CH3NH2 from the perovskite surface is observed as deduced by the development of negative N–H bands associated with its stretching and bending modes. The IR investigations are corroborated by XPS study, confirming the abstraction of CH3NH2 from the perovskite surface, whereas no oxidation of its inorganic framework is observed within the ALD window process investigated in this work. In parallel, the growth of ALD Al2O3 on perovskite is witnessed by the appearance of characteristic IR-active Al–O–Al phonon and (OH)–Al═O stretching modes. Based on the IR and XPS investigations, a plausible growth mechanism of ALD Al2O3 on top of perovskite is presented.",
keywords = "Al O, X-ray photoelectron spectroscopy, atomic layer deposition, infrared spectroscopy, perovskite, Al2O3",
author = "D. Koushik and L. Hazendonk and V. Zardetto and V. Vandalon and M.A. Verheijen and W.M.M. Kessels and M. Creatore",
year = "2019",
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journal = "ACS Applied Materials & Interfaces",
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Chemical analysis of the interface between hybrid organic−inorganic perovskite and atomic layer deposited Al2O3. / Koushik, D.; Hazendonk, L.; Zardetto, V.; Vandalon, V.; Verheijen, M.A.; Kessels, W.M.M.; Creatore, M. (Corresponding author).

In: ACS Applied Materials & Interfaces, Vol. 11, Nr. 5, 06.02.2019, blz. 5526-5535.

Onderzoeksoutput: Bijdrage aan tijdschriftTijdschriftartikelAcademicpeer review

TY - JOUR

T1 - Chemical analysis of the interface between hybrid organic−inorganic perovskite and atomic layer deposited Al2O3

AU - Koushik, D.

AU - Hazendonk, L.

AU - Zardetto, V.

AU - Vandalon, V.

AU - Verheijen, M.A.

AU - Kessels, W.M.M.

AU - Creatore, M.

PY - 2019/2/6

Y1 - 2019/2/6

N2 - Ultrathin metal oxides prepared by atomic layer deposition (ALD) have gained utmost attention as moisture and thermal stress barrier layers in perovskite solar cells (PSCs). We have recently shown that 10 cycles of ALD Al2O3 deposited directly on top of the CH3NH3PbI3–xClx perovskite material, are effective in delivering a superior PSC performance with 18% efficiency (compared to 15% of the Al2O3-free cell) with a long-term humidity-stability of more than 60 days. Motivated by these results, the present contribution focuses on the chemical modification which the CH3NH3PbI3–xClx perovskite undergoes upon growth of ALD Al2O3. Specifically, we combine in situ Infrared (IR) spectroscopy studies during film growth, together with X-ray photoelectron spectroscopy (XPS) analysis of the ALD Al2O3/perovskite interface. The IR-active signature of the NH3+ stretching mode of the perovskite undergoes minimal changes upon exposure to ALD cycles, suggesting no diffusion of ALD precursor and co-reactant (Al(CH3)3 and H2O) into the bulk of the perovskite. However, by analyzing the difference between the IR spectra associated with the Al2O3 coated perovskite and the pristine perovskite, respectively, changes occurring at the surface of perovskite are monitored. The abstraction of either NH3 or CH3NH2 from the perovskite surface is observed as deduced by the development of negative N–H bands associated with its stretching and bending modes. The IR investigations are corroborated by XPS study, confirming the abstraction of CH3NH2 from the perovskite surface, whereas no oxidation of its inorganic framework is observed within the ALD window process investigated in this work. In parallel, the growth of ALD Al2O3 on perovskite is witnessed by the appearance of characteristic IR-active Al–O–Al phonon and (OH)–Al═O stretching modes. Based on the IR and XPS investigations, a plausible growth mechanism of ALD Al2O3 on top of perovskite is presented.

AB - Ultrathin metal oxides prepared by atomic layer deposition (ALD) have gained utmost attention as moisture and thermal stress barrier layers in perovskite solar cells (PSCs). We have recently shown that 10 cycles of ALD Al2O3 deposited directly on top of the CH3NH3PbI3–xClx perovskite material, are effective in delivering a superior PSC performance with 18% efficiency (compared to 15% of the Al2O3-free cell) with a long-term humidity-stability of more than 60 days. Motivated by these results, the present contribution focuses on the chemical modification which the CH3NH3PbI3–xClx perovskite undergoes upon growth of ALD Al2O3. Specifically, we combine in situ Infrared (IR) spectroscopy studies during film growth, together with X-ray photoelectron spectroscopy (XPS) analysis of the ALD Al2O3/perovskite interface. The IR-active signature of the NH3+ stretching mode of the perovskite undergoes minimal changes upon exposure to ALD cycles, suggesting no diffusion of ALD precursor and co-reactant (Al(CH3)3 and H2O) into the bulk of the perovskite. However, by analyzing the difference between the IR spectra associated with the Al2O3 coated perovskite and the pristine perovskite, respectively, changes occurring at the surface of perovskite are monitored. The abstraction of either NH3 or CH3NH2 from the perovskite surface is observed as deduced by the development of negative N–H bands associated with its stretching and bending modes. The IR investigations are corroborated by XPS study, confirming the abstraction of CH3NH2 from the perovskite surface, whereas no oxidation of its inorganic framework is observed within the ALD window process investigated in this work. In parallel, the growth of ALD Al2O3 on perovskite is witnessed by the appearance of characteristic IR-active Al–O–Al phonon and (OH)–Al═O stretching modes. Based on the IR and XPS investigations, a plausible growth mechanism of ALD Al2O3 on top of perovskite is presented.

KW - Al O

KW - X-ray photoelectron spectroscopy

KW - atomic layer deposition

KW - infrared spectroscopy

KW - perovskite

KW - Al2O3

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U2 - 10.1021/acsami.8b18307

DO - 10.1021/acsami.8b18307

M3 - Article

C2 - 30624886

VL - 11

SP - 5526

EP - 5535

JO - ACS Applied Materials & Interfaces

JF - ACS Applied Materials & Interfaces

SN - 1944-8244

IS - 5

ER -