Modern information technologies have
tremendous demands on flexible
electronic devices such as thin-film transistors (TFTs). As the flexible
TFT technology continues to advance, the properties of the gate dielectric
become a bottleneck for the flexible TFTs to achieve fast switching
speed, low operation voltage, and downscaling. The gate dielectric
layer should be sufficiently thin, insulating, and flexible, and therefore,
hybrid organic–inorganic dielectrics are of great promise for
this purpose. In this work, we develop a scalable vapor-phase MLD/ALD
technique, which combines molecular layer deposition (MLD) and atomic
layer deposition (ALD), to grow a new hybrid polymer–oxide
dielectric thin-film material of polyimide (PI) and Al2O3, and demonstrate that the afforded hybrid polyimide–Al2O3 (HPA) films are well suited as the bendable
gate dielectrics for flexible electronic applications. We also perform
mechanism investigation on the growth of PI and Al2O3 during the MLD/ALD HPA process and find that the growth of
PI is strongly affected by the Al2O3 surface
and therefore exhibits a two-stage behavior. We further evaluate the
electrical and bending performances of the afforded HPA dielectrics
and apply the HPA films as the gate dielectrics for flexible carbon-nanotube
TFTs. The fabricated TFTs can well withstand 1000-time repetitive
bending without an increase in the TFT gate leakage current, which
shows the high promise of the HPA dielectrics for flexible electronic
applications. Considering that the MLD/ALD fabrication approach is
advantageous for high process reproducibility and large-scale compatibility,
we envision that the MLD/ALD-prepared HPA dielectrics will have great
applications in future complex flexible electronic circuits.
Herein, we report the design and scalable synthesis of three new Co(III) complexes, which have an unusual hydrocarbon η1‐alkyl‐η3‐allyl‐η5‐cyclopentadienyl ligation structure, from the reactions of readily available cobalt(II) compound CoCl2(PPh3)2 and biomass material β‐pinene via C−C bond activation. These Co(III) complexes are air‐stable, fairly volatile, and thermally stable, so they are excellent candidates as the metal precursors for the vapor deposition of cobalt‐containing thin films. As a demonstration, we show that the Co(III) complex of [(3’‐5’‐η,1‐σ)‐methylene(2,2,4‐trimethyl‐4‐cyclohexene‐1,3‐diyl)](η5‐methylcyclopentadienyl)Co (i. e. (seco‐pinene)(MeCp)Co) is well suited for the atomic layer deposition (ALD) of Co3O4 and CoS2 thin films, and the deposited Co3O4 and CoS2 films are able to conformally cover trench structures with a fairly high aspect ratio of 10 : 1.
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