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The electronic Seebeck response in a conductor involves the energy-dependent mean free path of the charge carriers and is affected by crystal structure, scattering from boundaries and defects, and strain. Previous photothermoelectric (PTE) studies have suggested that the thermoelectric properties of polycrystalline metal nanowires are related to grain structure, although direct evidence linking crystal microstructure to the PTE response is difficult to elucidate. Here, we show that room temperature scanning PTE measurements are sensitive probes that can detect subtle changes in the local Seebeck coefficient of gold tied to the underlying defects and strain that mediate crystal deformation. This connection is revealed through a combination of scanning PTE and electron microscopy measurements of single-crystal and bicrystal gold microscale devices. Unexpectedly, the photovoltage maps strongly correlate with gradually varying crystallographic misorientations detected by electron backscatter diffraction. The effects of individual grain boundaries and differing grain orientations on the PTE signal are minimal. This scanning PTE technique shows promise for identifying minor structural distortions in nanoscale materials and devices.

Conformal artificial electromagnetic media that feature tailorable responses as a function of incidence wavelength and angle represent universal components for optical engineering. Conformal grayscale metamaterials are introduced as a new class of volumetric electromagnetic media capable of supporting highly multiplexed responses and arbitrary, curvilinear form factors. Subwavelength‐scale voxels based on irregular shapes are designed to accommodate a continuum of dielectric values, enabling the freeform design process to reliably converge to exceptionally high figures of merit (FOMs) for a given multi‐objective design problem. Through additive manufacturing of ceramic–polymer composites, microwave metamaterials, designed for the radio‐frequency range of 8–12 GHz, are experimentally fabricated and devices with extreme dispersion profiles, an airfoil‐shaped beam‐steering device, and a broadband, broad‐angle conformal carpet cloak, are demonstrated. It is anticipated that conformal volumetric metamaterials will lead to new classes of compact and multifunctional imaging, sensing, and communications systems.

The study of grain boundaries is the foundation to understanding many of the intrinsic physical properties of bulk metals. Here, the preparation of microscale thin‐film gold bicrystals, using rapid melt growth, is presented as a model system for studies of single grain boundaries. This material platform utilizes standard fabrication tools and supports the high‐yield growth of thousands of bicrystals per wafer, each containing a grain boundary with a unique <111> tilt character. The crystal growth dynamics of the gold grains in each bicrystal are mediated by platinum gradients, which originate from the gold–platinum seeds responsible for gold crystal nucleation. This crystallization mechanism leads to a decoupling between crystal nucleation and crystal growth, and it ensures that the grain boundaries form at the middle of the gold microstructures and possess a uniform distribution of misorientation angles. It is envisioned that these bicrystals will enable the systematic study of the electrical, optical, chemical, thermal, and mechanical properties of individual grain boundary types.