title: Atomic Layer Deposition of In2O3:H from InCp and H2O/O2: Microstructure and Isotope Labeling Studies.
abstract: The atomic layer deposition (ALD) process of hydrogen-doped indium oxide (In2O3:H) using indium cyclopentadienyl (InCp) and both O2and 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.
authors.affiliation: Eindhoven University of Technology , PO Box 513, 5600 MB Eindhoven, The Netherlands.|Holst Centre , PO Box 8550, 5605 KN Eindhoven, The Netherlands.
authors.forename: Yizhi
authors.initials: Y
authors.lastname: Wu
authors.affiliation: Eindhoven University of Technology , PO Box 513, 5600 MB Eindhoven, The Netherlands.
authors.forename: Bart
authors.identifier: http://orcid.org/0000-0003-1197-441X
authors.initials: B
authors.lastname: Macco
authors.affiliation: Eindhoven University of Technology , PO Box 513, 5600 MB Eindhoven, The Netherlands.
authors.forename: Dries
authors.initials: D
authors.lastname: Vanhemel
authors.affiliation: Eindhoven University of Technology , PO Box 513, 5600 MB Eindhoven, The Netherlands.
authors.forename: Sebastian
authors.initials: S
authors.lastname: Kölling
authors.affiliation: Eindhoven University of Technology , PO Box 513, 5600 MB Eindhoven, The Netherlands.
authors.forename: Marcel A
authors.initials: MA
authors.lastname: Verheijen
authors.affiliation: Eindhoven University of Technology , PO Box 513, 5600 MB Eindhoven, The Netherlands.
authors.forename: Paul M
authors.initials: PM
authors.lastname: Koenraad
authors.affiliation: Eindhoven University of Technology , PO Box 513, 5600 MB Eindhoven, The Netherlands.
authors.forename: Wilhelmus M M
authors.initials: WM
authors.lastname: Kessels
authors.affiliation: Eindhoven University of Technology , PO Box 513, 5600 MB Eindhoven, The Netherlands.|Holst Centre , PO Box 8550, 5605 KN Eindhoven, The Netherlands.
authors.forename: Fred
authors.initials: F
authors.lastname: Roozeboom
keywords: atom probe tomography; atomic layer deposition; hydrogen isotope doping; indium oxide; morphology; transmission electron microscopy; transparent conductive oxide