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Abstract In alignment with the Materials Genome Initiative and as the product of a workshop sponsored by the US National Science Foundation, we define a vision for materials laboratories of the future in alloys, amorphous materials, and composite materials; chart a roadmap for realizing this vision; identify technical bottlenecks and barriers to access; and propose pathways to equitable and democratic access to integrated toolsets in a manner that addresses urgent societal needs, accelerates technological innovation, and enhances manufacturing competitiveness. Spanning three important materials classes, this article summarizes the areas of alignment and unifying themes, distinctive needs of different materials research communities, key science drivers that cannot be accomplished within the capabilities of current materials laboratories, and open questions that need further community input. Here, we provide a broader context for the workshop, synopsize the salient findings, outline a shared vision for democratizing access and accelerating materials discovery, highlight some case studies across the three different materials classes, and identify significant issues that need further discussion. Graphical abstract 

The analytical chemistry of phosphorus-containing materials is often impeded by the long measurement times and relatively large sample masses needed for 31 P NMR spectroscopy, by the scarcity and access limitations of synchrotron beamlines operating in the energy range of the P K-edge, by the challenges posed by species interconversion during liquid extraction, and by the considerable air-sensitivity typical of many phosphorus-containing materials and nanophases. To this end, we report the design and operation of a new laboratory-based spectrometer to simultaneously perform P Kα and Kβ X-ray emission spectroscopy (XES) while being housed in a research-grade controlled-atmosphere glovebox. Demonstration studies on nickel phosphide nanophases illustrate the importance of air-free XES and the value of simultaneous Kα and Kβ spectroscopy for identifying the P oxidation state and for investigating nanoscale influences on valence level electronic structures. 

We report a comprehensive computational study of unsupervised machine learning for extraction of chemically relevant information in X-ray absorption near edge structure (XANES) and in valence-to-core X-ray emission spectra (VtC-XES) for classification of a broad ensemble of sulphorganic molecules. By progressively decreasing the constraining assumptions of the unsupervised machine learning algorithm, moving from principal component analysis (PCA) to a variational autoencoder (VAE) to t-distributed stochastic neighbour embedding (t-SNE), we find improved sensitivity to steadily more refined chemical information. Surprisingly, when embedding the ensemble of spectra in merely two dimensions, t-SNE distinguishes not just oxidation state and general sulphur bonding environment but also the aromaticity of the bonding radical group with 87% accuracy as well as identifying even finer details in electronic structure within aromatic or aliphatic sub-classes. We find that the chemical information in XANES and VtC-XES is very similar in character and content, although they unexpectedly have different sensitivity within a given molecular class. We also discuss likely benefits from further effort with unsupervised machine learning and from the interplay between supervised and unsupervised machine learning for X-ray spectroscopies. Our overall results, i.e. , the ability to reliably classify without user bias and to discover unexpected chemical signatures for XANES and VtC-XES, likely generalize to other systems as well as to other one-dimensional chemical spectroscopies. 

Generating oxygen vacancies (Vö) in vanadium pentoxide (V 2 O 5 ) has been demonstrated as an effective approach to tailor its electrochemical properties. The present study investigates three different kinds of conductive polymer (CP = PPy, PEDOT, and PANI) coated V 2 O 5 nanofibers with Vö generated at the interface during the polymerization process. Surface Vö form a local electric field and promote the charge transfer kinetics of the resulting Vö-V 2 O 5 /CP nanocables, and the accompanying V 4+ and V 3+ ions may also catalyze the redox reactions and improve the supercapacitor performance. The differences and similarities of three different CP coatings have been compared and discussed, and are dependent on their polymerization conditions and coating thickness. The distribution of Vö in the surface layer and in the bulk has been elaborated and the corresponding effects on the electrochemical properties and supercapacitor performance have also been investigated. Vö-V 2 O 5 /CP can deliver a high capacity of up to 614 F g −1 at a current rate of 0.5 A g −1 and supercapacitors with Vö-V 2 O 5 /CP demonstrated excellent cycling stability over 15 000 cycles at a rate of 10 A g −1 .