Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 9, Issue 1, Pages 592-601Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.6b13560
Keywords
transparent conductive oxide; indium oxide; atomic layer deposition; hydrogen isotope doping; morphology; atom probe tomography; transmission electron microscopy
Funding
- Dutch Technology Foundation STW through the Flash Perspectief Programma
- Holst Centre/IMEC-NL, The Netherlands
- Solliance, a solar energy R&D initiative of ECN, TNO, Holst Centre, Eindhoven University of Technology, Imec and Forschungszentrum Julich
- Netherlands Organisation for Scientific Research (NWO, VICI program)
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The atomic layer deposition (ALD) process of hydrogen-doped indium oxide (In2O3:H) using indium cyclopentadienyl (InCp) and both O-2 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 degrees 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 degrees C), which is accompanied by a strong decrease in carrier density and an increase in carrier mobility. At higher deposition temperatures (>200 degrees 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 similar to 4 atom % for amorphous growth to similar to 2 atom % after the transition to crystalline film growth.
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