Transparent thin fi lm transistors (TFTs) have stimulated great scientifi c and technological interest due to potential applications in "invisible" electronics, such as transparent touch panels and see-through displays. [1][2][3][4][5][6] Since the fi rst demonstration of transparent TFTs using a crystalline ZnO semiconductor, [ 7 ] extensive efforts have sought to enhance performance by increasing the fi eld-effect mobility ( μ FE ) and/or lowering the operating voltage. [8][9][10][11][12] Principal foci have included the semiconductor and gate dielectric, two essential TFT materials. Among the diverse transparent semiconductors, amorphous transparent oxide semiconductors (a-TOSs) offer distinctive attractions vis-à-vis organics and crystalline TOSs, including good mobility, excellent environmental stability, low-temperature processability, optical transparency, smooth surfaces, and compositional uniformity. [ 4 , 13-15 ] For example, amorphous Zn-In-Sn-O (a-ZITO) fi lms afford moderate TFT performance at operating voltages ≥ 10 V when paired with a SiO 2 gate dielectric. [16][17][18][19][20] An effective approach to enhancing TFT performance is to introduce a self-assembled nanodielectric (SAND; Figure 1 a ) composed of a saturated hydrocarbon layer, a π -polarizable stilbazolium layer, and a chlorosiloxane-derived SiO x "capping" layer. These gate dielectrics can be deposited near room temperature by straightforward wet chemistry, and have large capacitances, low leakage, high breakdown fi elds, and suppress trapped charge between the dielectric and semiconductor for many classes of organic and inorganic semiconductors. [21][22][23] Nevertheless, while SANDs exhibit good chemical and thermal stability, [24][25][26] recent work suggests that direct exposure to high-energy ions and plasmas present in pulsed laser deposition (PLD) semiconductor growth processes, seriously degrades SAND dielectric properties and TFT performance. [ 27 ] It would therefore be highly desirable to devise approaches to enhancing SAND robustness. We report here that a simple vapor-derived hexachlorodisiloxane (HCDS, Cl 3 SiOSiCl 3 ) coating ("v-SiO x ") greatly enhances SAND durability with respect to PLD laser plumes. This "reinforced" SAND (R-SAND) enables the growth of high-quality, optically transparent a-ZITO TOS channels and TFTs operating at voltages of ≤1.0 V with mobilities as high as 140 cm 2 /V · s.After SAND fi lms were fabricated via solution processing, [ 21 ] a ∼ 5 nm thick v-SiO x layer was grown by HCDS vapor deposition, followed by ambient exposure for crosslinking. [ 28 ] Figure 1b shows capacitance vs. frequency (at 2.0 V) data for SAND, R-SAND, and v-SiO x fi lms measured as n + -Si/dielectric/Au devices. Compared to SAND, which exhibits a high capacitance ( C i ) of ∼ 220 nF/cm 2 at 2.0 V/10 KHz, C i for R-SAND is ∼ 180 nF/cm 2 measured under the same conditions. The slightly smaller R-SAND C i is not unexpected considering the series-connected nature of the top v-SiO x layer, which by itself exhibits C i ∼ 750 n...