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Exploring the First High-Entropy Thin Film Libraries: Composition Spread-Controlled Crystalline Structure.

ABSTRACT: Thin films of two types of high-entropy oxides (HEOs) have been deposited on 76.2 mm Si wafers using combinatorial sputter deposition. In one type of the oxides, (MgZnMnCoNi)O_x, all the metals have a stable divalent oxidation state and similar cationic radii. In the second type of oxides, (CrFeMnCoNi)O_x, the metals are more diverse in the atomic radius and valence state, and have good solubility in their sub-binary and ternary oxide systems. The resulting HEO thin films were characterized using several high-throughput analytical techniques. The microstructure, composition, and electrical conductivity obtained on defined grid maps were obtained for the first time across large compositional ranges. The crystalline structure of the films was observed as a function of the metallic elements in the composition spreads, that is, the Mn and Zn in (MgZnMnCoNi)O_x and Mn and Ni in (CrFeMnCoNi)O_x. The (MgZnMnCoNi)O_x sample was observed to form two-phase structures, except single spinel structure was found in (MgZnMnCoNi)O_x over a range of Mn > 12 at. % and Zn < 44 at. %, while (CrFeMnCoNi)O_x was always observed to form two-phase structures. Composition-controlled crystalline structure is not only experimentally demonstrated but also supported by density function theory calculation.

SUBMITTER: Nguyen TX

PROVIDER: S-EPMC8415495 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:The key impact and significance of a multilayer polymer-based dielectric system on the remarkable photoresponse properties of zinc phthalocyanine (ZnPc)-based photosensitive organic field-effect transistors (PS-OFETs) have been systematically analyzed at various incident optical powers. A combination of inorganic aluminum oxide (Al2O3) and organic nonpolar poly(methyl methacrylate) (PMMA) is used as the bilayer dielectric configuration, whereas in the trilayer dielectric system, a bilayer polymer dielectric, consisting of PMMA, as the low-k dielectric polymer, on top of poly(vinyl alcohol) (PVA), the high-k polar dielectric, has been fabricated along with Al2O3 as the third layer. Before fabricating the OFETs, a systematic optimization of the nature of growth of the ZnPc molecules, deposited on PMMA-coated glass substrates at different substrate temperatures (T s) was performed and examined by atomic-force microscopy, field-emission scanning electron microscopy, X-ray diffraction, and Raman analysis. At 90 °C, the fabricated PS-OFETs with the Al2O3/PVA/PMMA trilayer dielectric configuration showed the best p-channel behavior, with an enhanced and remarkable photoresponsivity of R ∼ 9689.39 A W-1 compared to that of the Al2O3/PMMA bilayer dielectric system (R ∼ 2679.40 A W-1) due to the polarization of the dipoles inside the polar PVA dielectric, which increases the charge transport through the channel. The charge carrier mobility of the device also improved by one order (μh ∼ 1.3 × 10-2 cm2 V-1 s-1) compared to that of the bilayer dielectric configuration (μh ∼ 3.5 × 10-3 cm2 V-1 s-1). The observed specific detectivity (D*) and NEP values of the bilayer dielectric system were 6.01 × 1013 Jones and 2.655 × 10-17 W Hz-1/2, whereas for the trilayer dielectric system, the observed D* and NEP values were 5.13 × 1014 Jones and 1.043 × 10-17 W Hz-1/2, respectively. Additionally, the operating voltage of each of the fabricated devices was also very low (-10 V) due to the influence of the inorganic high-k Al2O3 dielectric layer. The electrical stability of all of the fabricated devices was also investigated by bias stress analysis under both light and dark conditions in vacuum. To the best of our knowledge, the photoresponsivity (R) reported here with an Al2O3/PVA/PMMA trilayer dielectric configuration is the highest reported value for thin film-based PS-OFETs, at a remarkably low operating voltage of -10 V, on low-cost glass substrates without indium tin oxide or/and Si/SiO2.

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Exploring the First High-Entropy Thin Film Libraries: Composition Spread-Controlled Crystalline Structure.

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