Tseng M.-HSu D.-YChen G.-LFENG-YU TSAI2022-03-222022-03-22202119448244https://www.scopus.com/inward/record.uri?eid=2-s2.0-85108386293&doi=10.1021%2facsami.1c03895&partnerID=40&md5=41213bf17eb01d8ae29fc7344f3a8f37https://scholars.lib.ntu.edu.tw/handle/123456789/598369Stretchable barrier films capable of maintaining high levels of moisture- and gas-barrier performance under significant mechanical strains are a critical component for wearable/flexible electronics and other devices, but realization of stretchable moisture-barrier films has not been possible due to the inevitable issues of strain-induced rupturing compounded with moisture-induced swelling of a stretched barrier film. This study demonstrates nanolaminated polymer/metal oxide stretchable moisture-barrier films fabricated by a novel molecular layer deposition (MLD) process of polyamide-2,3 (PA-2,3) integrated with atomic layer deposition (ALD) metal oxide processes and an in situ surface-functionalization technique. The PA-2,3 surface upon in situ functionalization with H2O2 vapor offers adequate surface chemisorption sites for rapid nucleation of ALD oxides, minimizing defects at the PA-2,3/oxide interfaces in the nanolaminates. The integrated ALD/MLD process enables facile deposition and precise structural control of many-layered oxide/PA-2,3 nanolaminates, where the large number of PA-2,3 nanolayers provide high tolerance against mechanical stretching and flexing thanks to their defect-decoupling and stress-buffering functions, while the large number of oxide nanolayers shield against swelling by moisture. Specifically, a nanolaminate with 72 pairs of alternating 2 nm (5 cycles) PA-2,3 and 0.5 nm HfO2 (five cycles) maintains its water vapor transmission rate (WVTR) at the 10-6 g/m2 day level upon 10% tensile stretching and 2 mm-radius bending, a significant breakthrough for the wearable/flexible electronics technologies. ? 2021 American Chemical Society.atomic layer depositionmolecular layer depositionnanolaminatesstretchable gas barriersthin-film encapsulationAtomic layer depositionHafnium oxidesHydrogen peroxideMetalsMoistureOxide filmsPolymer filmsStrainStructural dynamicsWearable technologyElectronics technologyFunctionalizationsMechanical stretchingMolecular layer depositions (MLD)Structural controlSurface chemisorptionSurface FunctionalizationWater vapor transmission rateGas permeable membranes[SDGs]SDG6journal article10.1021/acsami.1c03895340974022-s2.0-85108386293