Wide-Surface Furnace for In Situ X-Ray Diffraction of Combinatorial Samples using a High-Throughput Approach

The quest for more efficient materials follows a pattern that changed little over the years, often involving poorly automated steps, such as synthesis, characterizations, and measurements of functional properties, sometimes coupled with ab initio modeling. While this approach has proven effective in generating knowledge and discovering promising formulations, it remains inefficient due to its extremely time-consuming nature and limited coverage of compositions. High-throughput approaches have demonstrated their efficiency in fields such as genomics, health, and pharmaceutics over the past decades and have been recently gained recognition in materials science. The Materials Genome Initiative (MGI), launched in the USA in 2011, aimed to reduce the time-to-market for materials development by a factor of 2. Since then, both experimental and computational aspects of MGI have attracted global attention from academia, government, and industry. High-throughput calculations have emerged as a powerful tool to rapidly identifying materials with desired properties among vast compositional space, in fields such as photocatalysis, 1 Liion batteries, 2 thermoelectrics, or p-type transparent conducting oxides. 3 This approach enabled the creation of huge databases, such as the Materials Project, 4 AFLOW initiative, 5 NOMAD (Novel Materials Discovery), 6 Max (Materials Design at the Exascale) 7 , or OPTIMADE (Open Databases Integration for Materials Design) 8 . In parallel to this modeling-centered approach, experimental facilities have been developed to explore the high-throughput synthesis and characterization of materials for specific applications, such as at NIST and NREL. 9 The substantial amount of experimental data generated is made available to the scientific community following the FAIR principles: Findable, Accessible, Interoperable, and Reusable. This approach complements experimental databases COD, 10 ROD, 11 or MPOD, 12 where crystallographic data, Raman spectra, and materials properties are collaboratively produced by the scientific community. High-throughput experimentation (HTE) is divided into two main categories: (1) automation, which involves parallel or sequential synthesis and characterization of samples, and (2) combinatorial research, which consists of producing single samples containing multiple compositions in patterns or compositional gradients. Combinatorial samples, also known as material libraries, contain information about broad compositional spaces, such as ternary diagrams. Although the concept dates back to 1965, 13 only recent advances in modern characterization tools and computational methods for large datasets have made HTE practical and valueable. 14 Please do not adjust margins Please do not adjust margins several commercial facilities exist for characterizing combinatorial samples at room temperature, such as XYresolved X-ray diffraction (XRD), Raman Spectroscopy, UV-Visible spectroscopy. A noteworthy example is the combined Xray diffraction and fluorescence (XRD/XRF) experiment conducted at the Stanford Synchrotron Radiation Lightsource (SSRL) by J. M. Gregoire et al. in 2014 on combinatorial libraries deposited on 100 mm silicon substrates. 15 This setup was optimized for texture analysis at room temperature under ambient conditions. Synchrotron X-ray absorption near edge spectroscopy (XANES) has also been used to study large combinatorial libraries for solar light absorbers in ambient air. 16 However, the in situ characterization of combinatorial libraries at high temperatures remains challenging, regardless of the target properties. J. Wolfman's group at Greman laboratory in Tours developed combinatorial procedures using 10 mm side square samples to explore electrical properties of oxides for microelectronics above room temperature (i.e., 400 K). 17 Yet, typical combinatorial libraries are deposited on 100 mm substrates, which complicates measurements due to the lack of commercial equipment for such large sample sizes. A few specialized devices have been developed specifically to address this challenge: (1) MicroXact, a commercial company, offers a probe system for measuring target properties at high temperatures under controlled atmospheres. Their device supports motorized or semi-automated testing of 100 mm or larger wafers up to 700 °C in vacuum or 650 °C at atmospheric pressure. 18 This equipment was adapted at IREC for hightemperature electrochemical impedance spectroscopy (EIS) of 75 mm combinatorial libraries. 19,20 (2) Yan et al. developed a thermoelectric screening tool capable of measuring the Seebeck coefficient and electrical resistivity from 300 K to 800 K on 76.2 mm diameter combinatorial thin films. 21 (3) Papac et al. demonstrated an instrument for spatially resolved hightemperature EIS of 50 mm libraries. 22 We recently demonstrated the feasibility of HTE using a combinatorial material library produced by pulsed laser deposition (PLD) and characterized by XY-resol

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