Reversible and Irreversible Reactions of Trimethylaluminum with Common Organic Functional Groups as a Model for Molecular Layer Deposition and Vapor Phase Infiltration

Yang, Fan; Brede, Jens; Ablat, Hayrensa; Abadía, Mikel; Zhang, Lianbing; Rogero, Celia; Elliott, Simon D.; Knez, Mato

doi:10.1002/admi.201700237

Cited by 42 publications

(53 citation statements)

References 72 publications

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“…Additionally, EDS line scan shown in Figure S2 for a nanolaminate sample shows no or little Zn within the sub-surface growth. Subsurface diffusion of ALD precursors into polymers and other soft substrates is a relatively well known phenomenon [48,49,50,51,52]. For instance Sun et al reported very similar looking sub-surface growth deposited on polyamide-6, and discovered that thinner subsurface growth had higher fracture strain [51].…”

Section: Resultsmentioning

confidence: 99%

Fracture Mechanics and Oxygen Gas Barrier Properties of Al2O3/ZnO Nanolaminates on PET Deposited by Atomic Layer Deposition

et al. 2019

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Rapid progress in the performance of organic devices has increased the demand for advances in the technology of thin-film permeation barriers and understanding the failure mechanisms of these material systems. Herein, we report the extensive study of mechanical and gas barrier properties of Al2O3/ZnO nanolaminate films prepared on organic substrates by atomic layer deposition (ALD). Nanolaminates of Al2O3/ZnO and single compound films of around 250 nm thickness were deposited on polyethylene terephthalate (PET) foils by ALD at 90 °C using trimethylaluminium (TMA) and diethylzinc (DEZ) as precursors and H2O as the co-reactant. STEM analysis of the nanolaminate structure revealed that steady-state film growth on PET is achieved after about 60 ALD cycles. Uniaxial tensile strain experiments revealed superior fracture and adhesive properties of single ZnO films versus the single Al2O3 film, as well as versus their nanolaminates. The superior mechanical performance of ZnO was linked to the absence of a roughly 500 to 900 nm thick sub-surface growth observed for single Al2O3 films as well as for the nanolaminates starting with an Al2O3 initial layer on PET. In contrast, the gas permeability of the nanolaminate coatings on PET was measured to be 9.4 × 10−3 O2 cm3 m−2 day−1. This is an order of magnitude less than their constituting single oxides, which opens prospects for their applications as gas barrier layers for organic electronics and food and drug packaging industries. Direct interdependency between the gas barrier and the mechanical properties was not established enabling independent tailoring of these properties for mechanically rigid and impermeable thin film coatings.

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Section: Resultsmentioning

confidence: 99%

Fracture Mechanics and Oxygen Gas Barrier Properties of Al2O3/ZnO Nanolaminates on PET Deposited by Atomic Layer Deposition

et al. 2019

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“…Previous work on another metalcone film, alucone, suggests that the observed conversion process in alucone is driven by the reaction of water or oxygen with the carbon or metal atoms in the film, splitting the CO or metal–oxygen bonds, respectively . This reaction with oxygen or water is exothermic or slightly endothermic at ambient conditions for alucone films and can produce a mixture of formaldehyde, glycols, and acid products .…”

Section: Resultsmentioning

confidence: 77%

Structurally Stable Manganese Alkoxide Films Grown by Hybrid Molecular Layer Deposition for Electrochemical Applications

Bergsman

Baker

Closser

et al. 2019

Adv Funct Materials

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Hybrid molecular layer deposition (MLD) has significant potential for the creation of ultrathin electrochemically active materials, due to its ability to combine organic and inorganic species to modulate film properties. However, only a limited number of hybrid MLD processes are demonstrated with electrochemically relevant elements, such as manganese. Here, a "manganicone" manganese hybrid MLD chemistry is developed using the precursors bis(ethylcyclopentadienyl)manganese and ethylene glycol. The resulting manganese alkoxide coordination networks are shown to have many interesting properties, including the ability to seamlessly fill high aspect ratio vias and the chemical conversion into manganese carboxylate in air over several hours at room temperature. Linear, self-saturating growth is reported. Importantly, hybrid manganicone films annealed to 480 °C in air demonstrate a greater stability to restructuring during electrochemical testing than their inorganic counterparts grown by atomic layer deposition, without reducing the activity of the reactive sites on the manganese surface. Thus, hybrid manganese films grown by MLD have significant promise for use as catalysts for the oxygen evolution reaction and as electrodes in thin film batteries.

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“…Yang et al concluded in their study of phenyls, substituted with −OH, −NH 2 , or −NO 2 groups, that whenever −OH groups were present TMA would react irreversibly with it. 52 MH consists of three hydroxyl groups per repeating unit, or 22 per molecule (see Figure 1 ). It is therefore reasonable to assume that the main initial process for alumina infiltration of MH involves the reaction between TMA and these hydroxyl groups.…”

Section: Resultsmentioning

confidence: 99%

Poly(styrene)-block-Maltoheptaose Films for Sub-10 nm Pattern Transfer: Implications for Transistor Fabrication

Löfstrand

Jam

Mothander

et al. 2021

ACS Appl. Nano Mater.

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Sequential infiltration synthesis (SIS) into poly(styrene)- block -maltoheptaose (PS- b -MH) block copolymer using vapors of trimethyl aluminum and water was used to prepare nanostructured surface layers. Prior to the infiltration, the PS- b -MH had been self-assembled into 12 nm pattern periodicity. Scanning electron microscopy indicated that horizontal alumina-like cylinders of 4.9 nm diameter were formed after eight infiltration cycles, while vertical cylinders were 1.3 nm larger. Using homopolymer hydroxyl-terminated poly(styrene) (PS–OH) and MH films, specular neutron reflectometry revealed a preferential reaction of precursors in the MH compared to PS–OH. The infiltration depth into the maltoheptaose homopolymer film was found to be 2.0 nm after the first couple of cycles. It reached 2.5 nm after eight infiltration cycles, and the alumina incorporation within this infiltrated layer corresponded to 23 vol % Al 2 O 3 . The alumina-like material, resulting from PS- b -MH infiltration, was used as an etch mask to transfer the sub-10 nm pattern into the underlying silicon substrate, to an aspect ratio of approximately 2:1. These results demonstrate the potential of exploiting SIS into carbohydrate-based polymers for nanofabrication and high pattern density applications, such as transistor devices.

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Reversible and Irreversible Reactions of Trimethylaluminum with Common Organic Functional Groups as a Model for Molecular Layer Deposition and Vapor Phase Infiltration

Cited by 42 publications

References 72 publications

Fracture Mechanics and Oxygen Gas Barrier Properties of Al2O3/ZnO Nanolaminates on PET Deposited by Atomic Layer Deposition

Fracture Mechanics and Oxygen Gas Barrier Properties of Al2O3/ZnO Nanolaminates on PET Deposited by Atomic Layer Deposition

Structurally Stable Manganese Alkoxide Films Grown by Hybrid Molecular Layer Deposition for Electrochemical Applications

Poly(styrene)-block-Maltoheptaose Films for Sub-10 nm Pattern Transfer: Implications for Transistor Fabrication

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