Amorphous In–Ga–Zn Oxide Semiconducting
Thin Films with High Mobility from Electrochemically Generated Aqueous
Nanocluster Inks
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Abstract
Solution processing
is a scalable means of depositing large-area electronics for applications
in displays, sensors, smart windows, and photovoltaics. However, solution
routes typically yield films with electronic quality inferior to traditional
vacuum deposition, as the solution precursors contain excess organic
ligands, counterions, and/or solvent that leads to porosity in the
final film. We show that electrolysis of aq. mixed metal nitrate salt
solutions drives the formation of indium gallium zinc oxide (IGZO)
precursor solutions, without purification, that consist of ∼1
nm radii metal–hydroxo clusters, minimal nitrate counterions,
and no organic ligands. Films deposited from cluster precursors over
a wide range of composition are smooth (roughness of 0.24 nm), homogeneous,
dense (80% of crystalline phase), and crack-free. The transistor performance
of IGZO films deposited from electrochemically synthesized clusters
is compared to those from the starting nitrate salt solution, sol–gel
precursors, and, as a control, vacuum-sputter-deposited films. The
average channel mobility (μ<sub><i>AVE</i></sub>)
of air-annealed cluster films (In:Ga:Zn = 69:12:19) at 400 °C
was ∼9 cm<sup>2</sup> V<sup>–1</sup> s<sup>–1</sup>, whereas those of control nitrate salt and sol–gel precursor
films were ∼5 and ∼2 cm<sup>2</sup> V<sup>–1</sup> s<sup>–1</sup>, respectively. By incorporating an ultrathin
indium–tin–zinc oxide interface layer prior to IGZO
film deposition and air-annealing at 550 °C, a μ<sub><i>AVE</i></sub> of ∼30 cm<sup>2</sup> V<sup>–1</sup> s<sup>–1</sup> was achieved, exceeding that of sputtered
IGZO control films. These data show that electrochemically derived
cluster precursors yield films that are structurally and electrically
superior to those deposited from metal nitrate salt and related organic
sol–gel precursor solutions and approach the quality of sputtered
films