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In Situ Microgravimetric Study of Ion Exchanges in the Ternary Cu-In-S System Prepared by Atomic Layer Deposition.

ABSTRACT: Reaction mechanisms during the growth of multinary compounds by atomic layer deposition can be complex, especially for sulfide materials. For instance, the deposition of copper indium disulfide (CuInS2) shows a non-direct correlation between the cycle ratio, the growth per cycle of each binary growth cycles, i.e., CuxS and In2S3, and the film composition. This evidences side reactions that compete with the direct Atomic Layer Deposition (ALD) growth reactions and makes the deposition of large films very challenging. To develop a robust upscalable recipe, it is essential to understand the chemical surface reactions. In this study, reaction mechanisms in the Cu-In-S ternary system were investigated in-situ by using a quartz crystal microbalance system to monitor mass variations. Pure binary indium sulfide (In2S3) and copper sulfide (CuxS) thin film depositions on Al2O3 substrate were first studied. Then, precursors were transported to react on CuxS and In2S3 substrates. In this paper, gas-phase ion exchanges are discussed based on the recorded mass variations. A cation exchange between the copper precursor and the In2S3 is highlighted, and a solution to reduce it by controlling the thickness deposited for each stack of binary materials during the CuInS2 deposition is finally proposed.

SUBMITTER: Le Tulzo H

PROVIDER: S-EPMC7041370 | biostudies-literature | 2020 Feb

REPOSITORIES: biostudies-literature

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In Situ Microgravimetric Study of Ion Exchanges in the Ternary Cu-In-S System Prepared by Atomic Layer Deposition.

Le Tulzo Harold H Schneider Nathanaelle N Donsanti Frédérique F

Materials (Basel, Switzerland) 20200201 3

Reaction mechanisms during the growth of multinary compounds by atomic layer deposition can be complex, especially for sulfide materials. For instance, the deposition of copper indium disulfide (CuInS2) shows a non-direct correlation between the cycle ratio, the growth per cycle of each binary growth cycles, i.e., CuxS and In2S3, and the film composition. This evidences side reactions that compete with the direct Atomic Layer Deposition (ALD) growth re ...[more]

PMID: 32024105

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Project description:Atomic layer deposition (ALD) of alumina using trimethylaluminum (TMA) has technological importance in microelectronics. This process has demonstrated a high potential in applications of protective coatings on Cu surfaces for control of diffusion of Cu in Cu2S films in photovoltaic devices and sintering of Cu-based nanoparticles in liquid phase hydrogenation reactions. With this motivation in mind, the reaction between TMA and oxygen was investigated on Cu(111) and Cu2O/Cu(111) surfaces. TMA did not adsorb on the Cu(111) surface, a result consistent with density functional theory (DFT) calculations predicting that TMA adsorption and decomposition are thermodynamically unfavorable on pure Cu(111). On the other hand, TMA readily adsorbed on the Cu2O/Cu(111) surface at 473 K resulting in the reduction of some surface Cu(1+) to metallic copper (Cu(0)) and the formation of a copper aluminate, most likely CuAlO2. The reaction is limited by the amount of surface oxygen. After the first TMA half-cycle on Cu2O/Cu(111), two-dimensional (2D) islands of the aluminate were observed on the surface by scanning tunneling microscopy (STM). According to DFT calculations, TMA decomposed completely on Cu2O/Cu(111). High-resolution electron energy loss spectroscopy (HREELS) was used to distinguish between tetrahedrally (Altet) and octahedrally (Aloct) coordinated Al(3+) in surface adlayers. TMA dosing produced an aluminum oxide film, which contained more octahedrally coordinated Al(3+) (Altet/Aloct HREELS peak area ratio ? 0.3) than did dosing O2 (Altet/Aloct HREELS peak area ratio ? 0.5). After the first ALD cycle, TMA reacted with both Cu2O and aluminum oxide surfaces in the absence of hydroxyl groups until film closure by the fourth ALD cycle. Then, TMA continued to react with surface Al-O, forming stoichiometric Al2O3. O2 half-cycles at 623 K were more effective for carbon removal than O2 half-cycles at 473 K or water half-cycles at 623 K. The growth rate was approximately 3-4 Å/cycle for TMA+O2 ALD (O2 half-cycles at 623 K). No preferential growth of Al2O3 on the steps of Cu(111) was observed. According to STM, Al2O3 grows homogeneously on Cu(111) terraces.

Dataset Information

In Situ Microgravimetric Study of Ion Exchanges in the Ternary Cu-In-S System Prepared by Atomic Layer Deposition.

Publications

In Situ Microgravimetric Study of Ion Exchanges in the Ternary Cu-In-S System Prepared by Atomic Layer Deposition.

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