Atomic layer deposition of ln2O3: H from lnCp and H2O/O2: microstructure and isotope labelling studies

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Abstract

The atomic layer deposition (ALD) process of hydrogen-doped indium oxide (In2O3:H) using indium cyclopentadienyl (InCp) and both O2 and H2O as precursors is highly promising for the preparation of transparent conductive oxides. It yields a high growth per cycle (>0.1 nm), is viable at temperatures as low as 100 °C, and provides a record optoelectronic quality after postdeposition crystallization of the films ( ACS Appl. Mat. Interfaces, 2015, 7, 16723−16729, DOI: 10.1021/acsami.5b04420). Since both the dopant incorporation and the film microstructure play a key role in determining the optoelectronic properties, both the crystal growth and the incorporation of the hydrogen dopant during this ALD process are studied in this work. This has been done using transmission electron microscopy (TEM) and atom probe tomography (APT) in combination with deuterium isotope labeling. TEM studies show that an amorphous-to-crystalline phase transition occurs in the low-temperature regime (100–150 °C), which is accompanied by a strong decrease in carrier density and an increase in carrier mobility. At higher deposition temperatures (>200 °C), enhanced nucleation of crystals and the incorporation of carbon impurities lead to a reduced grain size and even an amorphous phase, respectively, resulting in a strong reduction in carrier mobility. APT studies on films grown with deuterated water show that the incorporated hydrogen mainly originates from the coreactant and not from the InCp precursor. In addition, it was established that the incorporation of hydrogen decreased from ∼4 atom % for amorphous growth to ∼2 atom % after the transition to crystalline film growth.
Original languageEnglish
Pages (from-to)592–601
Number of pages10
JournalACS Applied Materials & Interfaces
Volume9
Issue number1
Early online date5 Dec 2016
DOIs
Publication statusPublished - 2017

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Atomic layer deposition
Isotopes
Labeling
Hydrogen
Atoms
Microstructure
Indium
Carrier mobility
Crystallization
Optoelectronic devices
Tomography
Doping (additives)
Crystalline materials
Transmission electron microscopy
Deuterium
Film growth
Oxides
Temperature
Carrier concentration
Nucleation

Cite this

@article{9a0bf555b19447988da23437b7b6b757,
title = "Atomic layer deposition of ln2O3: H from lnCp and H2O/O2: microstructure and isotope labelling studies",
abstract = "The atomic layer deposition (ALD) process of hydrogen-doped indium oxide (In2O3:H) using indium cyclopentadienyl (InCp) and both O2 and H2O as precursors is highly promising for the preparation of transparent conductive oxides. It yields a high growth per cycle (>0.1 nm), is viable at temperatures as low as 100 °C, and provides a record optoelectronic quality after postdeposition crystallization of the films ( ACS Appl. Mat. Interfaces, 2015, 7, 16723−16729, DOI: 10.1021/acsami.5b04420). Since both the dopant incorporation and the film microstructure play a key role in determining the optoelectronic properties, both the crystal growth and the incorporation of the hydrogen dopant during this ALD process are studied in this work. This has been done using transmission electron microscopy (TEM) and atom probe tomography (APT) in combination with deuterium isotope labeling. TEM studies show that an amorphous-to-crystalline phase transition occurs in the low-temperature regime (100–150 °C), which is accompanied by a strong decrease in carrier density and an increase in carrier mobility. At higher deposition temperatures (>200 °C), enhanced nucleation of crystals and the incorporation of carbon impurities lead to a reduced grain size and even an amorphous phase, respectively, resulting in a strong reduction in carrier mobility. APT studies on films grown with deuterated water show that the incorporated hydrogen mainly originates from the coreactant and not from the InCp precursor. In addition, it was established that the incorporation of hydrogen decreased from ∼4 atom {\%} for amorphous growth to ∼2 atom {\%} after the transition to crystalline film growth.",
author = "Y. Wu and B. Macco and D. Vanhemel and S. K{\"o}lling and M.A. Verheijen and P.M. Koenraad and W.M.M. Kessels and F. Roozeboom",
year = "2017",
doi = "10.1021/acsami.6b13560",
language = "English",
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journal = "ACS Applied Materials & Interfaces",
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TY - JOUR

T1 - Atomic layer deposition of ln2O3: H from lnCp and H2O/O2

T2 - microstructure and isotope labelling studies

AU - Wu, Y.

AU - Macco, B.

AU - Vanhemel, D.

AU - Kölling, S.

AU - Verheijen, M.A.

AU - Koenraad, P.M.

AU - Kessels, W.M.M.

AU - Roozeboom, F.

PY - 2017

Y1 - 2017

N2 - The atomic layer deposition (ALD) process of hydrogen-doped indium oxide (In2O3:H) using indium cyclopentadienyl (InCp) and both O2 and H2O as precursors is highly promising for the preparation of transparent conductive oxides. It yields a high growth per cycle (>0.1 nm), is viable at temperatures as low as 100 °C, and provides a record optoelectronic quality after postdeposition crystallization of the films ( ACS Appl. Mat. Interfaces, 2015, 7, 16723−16729, DOI: 10.1021/acsami.5b04420). Since both the dopant incorporation and the film microstructure play a key role in determining the optoelectronic properties, both the crystal growth and the incorporation of the hydrogen dopant during this ALD process are studied in this work. This has been done using transmission electron microscopy (TEM) and atom probe tomography (APT) in combination with deuterium isotope labeling. TEM studies show that an amorphous-to-crystalline phase transition occurs in the low-temperature regime (100–150 °C), which is accompanied by a strong decrease in carrier density and an increase in carrier mobility. At higher deposition temperatures (>200 °C), enhanced nucleation of crystals and the incorporation of carbon impurities lead to a reduced grain size and even an amorphous phase, respectively, resulting in a strong reduction in carrier mobility. APT studies on films grown with deuterated water show that the incorporated hydrogen mainly originates from the coreactant and not from the InCp precursor. In addition, it was established that the incorporation of hydrogen decreased from ∼4 atom % for amorphous growth to ∼2 atom % after the transition to crystalline film growth.

AB - The atomic layer deposition (ALD) process of hydrogen-doped indium oxide (In2O3:H) using indium cyclopentadienyl (InCp) and both O2 and H2O as precursors is highly promising for the preparation of transparent conductive oxides. It yields a high growth per cycle (>0.1 nm), is viable at temperatures as low as 100 °C, and provides a record optoelectronic quality after postdeposition crystallization of the films ( ACS Appl. Mat. Interfaces, 2015, 7, 16723−16729, DOI: 10.1021/acsami.5b04420). Since both the dopant incorporation and the film microstructure play a key role in determining the optoelectronic properties, both the crystal growth and the incorporation of the hydrogen dopant during this ALD process are studied in this work. This has been done using transmission electron microscopy (TEM) and atom probe tomography (APT) in combination with deuterium isotope labeling. TEM studies show that an amorphous-to-crystalline phase transition occurs in the low-temperature regime (100–150 °C), which is accompanied by a strong decrease in carrier density and an increase in carrier mobility. At higher deposition temperatures (>200 °C), enhanced nucleation of crystals and the incorporation of carbon impurities lead to a reduced grain size and even an amorphous phase, respectively, resulting in a strong reduction in carrier mobility. APT studies on films grown with deuterated water show that the incorporated hydrogen mainly originates from the coreactant and not from the InCp precursor. In addition, it was established that the incorporation of hydrogen decreased from ∼4 atom % for amorphous growth to ∼2 atom % after the transition to crystalline film growth.

U2 - 10.1021/acsami.6b13560

DO - 10.1021/acsami.6b13560

M3 - Article

C2 - 27977925

VL - 9

SP - 592

EP - 601

JO - ACS Applied Materials & Interfaces

JF - ACS Applied Materials & Interfaces

SN - 1944-8244

IS - 1

ER -