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Contemporary materials discovery requires intricate sequences of synthesis, formulation, and characterization that often span multiple locations with specialized expertise or instrumentation. To accelerate these workflows, we present a cloud-based strategy that enabled delocalized and asynchronous design-make-test-analyze cycles. We showcased this approach through the exploration of molecular gain materials for organic solid-state lasers as a frontier application in molecular optoelectronics. Distributed robotic synthesis and in-line property characterization, orchestrated by a cloud-based artificial intelligence experiment planner, resulted in the discovery of 21 new state-of-the-art materials. Gram-scale synthesis ultimately allowed for the verification of best-in-class stimulated emission in a thin-film device. Demonstrating the asynchronous integration of five laboratories across the globe, this workflow provides a blueprint for delocalizing-and democratizing-scientific discovery.

General conditions for organic reactions are important but rare, and efforts to identify them usually consider only narrow regions of chemical space. Discovering more general reaction conditions requires considering vast regions of chemical space derived from a large matrix of substrates crossed with a high-dimensional matrix of reaction conditions, rendering exhaustive experimentation impractical. Here, we report a simple closed-loop workflow that leverages data-guided matrix down-selection, uncertainty-minimizing machine learning, and robotic experimentation to discover general reaction conditions. Application to the challenging and consequential problem of heteroaryl Suzuki-Miyaura cross-coupling identified conditions that double the average yield relative to a widely used benchmark that was previously developed using traditional approaches. This study provides a practical road map for solving multidimensional chemical optimization problems with large search spaces.

The challenge of prebiotic chemistry is to trace the syntheses of life's key building blocks from a handful of primordial substrates. Here we report a forward-synthesis algorithm that generates a full network of prebiotic chemical reactions accessible from these substrates under generally accepted conditions. This network contains both reported and previously unidentified routes to biotic targets, as well as plausible syntheses of abiotic molecules. It also exhibits three forms of nontrivial chemical emergence, as the molecules within the network can act as catalysts of downstream reaction types; form functional chemical systems, including self-regenerating cycles; and produce surfactants relevant to primitive forms of biological compartmentalization. To support these claims, computer-predicted, prebiotic syntheses of several biotic molecules as well as a multistep, self-regenerative cycle of iminodiacetic acid were validated by experiment., (Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works.)

Mechanically flexible, easy-to-process, and environmentally benign materials capable of current rectification are interesting alternatives to "hard" silicon-based devices. Among these materials are metallic/charged-organic nanoparticles in which electronic currents though metal cores are modulated by the gradients of counterions surrounding the organic ligands. Although layers of oppositely charged particles can respond to both electronic and chemical signals and can function even under significant mechanical deformation, the rectification ratios of these "chemoelectronic" elements have been, so far, low. This work shows that significantly steeper counterion gradients and significantly higher rectification ratios can be achieved with nanoparticles of only one polarity but in contact with a porous electrode serving as a counterion "sink." These composite structures act as rectifiers even at radio frequencies, providing a new means of interfacing counterions' dynamics with high-frequency electronic currents.

Even minute quantities of electric charge accumulating on polymer surfaces can cause shocks, explosions, and multibillion-dollar losses to electronic circuitry. This paper demonstrates that to remove static electricity, it is not at all necessary to "target" the charges themselves. Instead, the way to discharge a polymer is to remove radicals from its surface. These radicals colocalize with and stabilize the charges; when they are scavenged, the surfaces discharge rapidly. This radical-charge interplay allows for controlling static electricity by doping common polymers with small amounts of radical-scavenging molecules, including the familiar vitamin E. The effectiveness of this approach is demonstrated by rendering common polymers dust-mitigating and also by using them as coatings that prevent the failure of electronic circuitry.

When dielectric materials are brought into contact and then separated, they develop static electricity. For centuries, it has been assumed that such contact charging derives from the spatially homogeneous material properties (along the material's surface) and that within a given pair of materials, one charges uniformly positively and the other negatively. We demonstrate that this picture of contact charging is incorrect. Whereas each contact-electrified piece develops a net charge of either positive or negative polarity, each surface supports a random "mosaic" of oppositely charged regions of nanoscopic dimensions. These mosaics of surface charge have the same topological characteristics for different types of electrified dielectrics and accommodate significantly more charge per unit area than previously thought.

Deformable, spherical aggregates of metal nanoparticles connected by long-chain dithiol ligands self-assemble into nanostructured materials of macroscopic dimensions. These materials are plastic and moldable against arbitrarily shaped masters and can be thermally hardened into polycrystalline metal structures of controllable porosity. In addition, in both plastic and hardened states, the assemblies are electrically conductive and exhibit Ohmic characteristics down to approximately 20 volts per meter. The self-assembly method leading to such materials is applicable both to pure metals and to bimetallic structures of various elemental compositions.

Self-assembly of charged, equally sized metal nanoparticles of two types (gold and silver) leads to the formation of large, sphalerite (diamond-like) crystals, in which each nanoparticle has four oppositely charged neighbors. Formation of these non-close-packed structures is a consequence of electrostatic effects specific to the nanoscale, where the thickness of the screening layer is commensurate with the dimensions of the assembling objects. Because of electrostatic stabilization of larger crystallizing particles by smaller ones, better-quality crystals can be obtained from more polydisperse nanoparticle solutions.

An object spinning at the surface of a liquid creates a chiral vortex. If the spinning object is itself chiral, its shape modifies the characteristics of the vortex; interactions between that vortex and other vortices then depend on the chirality of the objects that produce them. This paper describes the aggregation of millimeter-sized, chiral magnetized plates floating at a liquid-air interface and rotating under the influence of a rotating external magnetic field. This external field confines all the plates at densities that cause the vortices they generate to interact strongly. For one set of plates investigated, plates of one chirality attract one another, and plates of the other chirality repel other plates of both chiralities.