The spectral characteristics of near-field thermal emission from nanoparticle arrays are explained by comparison to the dispersions for propagating modes. Using the coupled dipole model, we analytically calculate the spectral emission from single particles, chains, planes, and three-dimensional arrays of $\mathrm{Si}{\mathrm{O}}_2$ and SiC. We show that the differences in their spectra are due to the existence or absence of propagating surface phonon polariton modes and that the emission is dominated by these modes when they are present. This work paves the way for understanding and control of near-field radiation in nanofluids, nanoparticle beds, and certain metamaterials.

This work reports a rigorous and comprehensive three-dimensional electromagnetic computation to investigate and design photoluminescence enhancement from a single silicon-vacancy center (SVC) in a nanodiamond crystal embedded in various metallic nanoantennae, each having a different geometry. The study demonstrates how each antenna design enhances the photoluminescence of SVCs in diamond. In particular, our report discusses how the 2D or 3D curvature of the nanoantenna and the control of the local environment of the SVC can lead to significant field enhancement of its optical field. Our calculated optimal photoluminescence for each design enhances the emission intensity by $15\text{–}300\times$ that of a single SVC without antenna. The enhancement mechanisms are investigated using four representative structures that can be fabricated under feasible and realistic growth conditions, i.e., spherical-, nanorod-, nanodisk-dimer, and bow-tie nanoantennae. These results demonstrate a method for rationally designing arbitrary metallic nanoantenna/emitter assemblies to achieve optimal SVC photoluminescence.

Thorough characterization of the thermomechanical properties of materials requires difficult and time-consuming experiments. This severely limits the availability of data and is one of the main obstacles for the development of effective accelerated materials design strategies. The rapid screening of new potential materials requires highly integrated, sophisticated, and robust computational approaches. We tackled the challenge by developing an automated, integrated workflow with robust error-correction within the AFLOW framework which combines the newly developed “Automatic Elasticity Library” with the previously implemented GIBBS method. The first extracts the mechanical properties from automatic self-consistent stress-strain calculations, while the latter employs those mechanical properties to evaluate the thermodynamics within the Debye model. This new thermoelastic workflow is benchmarked against a set of 74 experimentally characterized systems to pinpoint a robust computational methodology for the evaluation of bulk and shear moduli, Poisson ratios, Debye temperatures, Grüneisen parameters, and thermal conductivities of a wide variety of materials. The effect of different choices of equations of state and exchange-correlation functionals is examined and the optimum combination of properties for the Leibfried-Schlömann prediction of thermal conductivity is identified, leading to improved agreement with experimental results than the GIBBS-only approach. The framework has been applied to the AFLOW.org data repositories to compute the thermoelastic properties of over 3500 unique materials. The results are now available online by using an expanded version of the REST-API described in the Appendix.

Pyrite $\mathrm{Fe}{\mathrm{S}}_2$ has outstanding potential as an earth-abundant, low-cost, nontoxic photovoltaic, but underperforms dramatically in solar cells. While the full reasons for this are not clear, one certain factor is the inability to understand and control doping in $\mathrm{Fe}{\mathrm{S}}_2$. This is exemplified by the widely accepted but unexplained observation that unintentionally doped $\mathrm{Fe}{\mathrm{S}}_2$ single crystals are predominantly $n$ type, whereas thin films are $p$ type. Here we provide a potential resolution to this “doping puzzle,” arrived at via Hall effect, thermopower, and resistivity measurements on a large set of $\mathrm{Fe}{\mathrm{S}}_2$ single crystals and films that span five orders of magnitude in mobility. The results reveal three main findings. First, in addition to crystals, the highest mobility thin films in this study are shown to be definitively $n$ type, from both Hall effect and thermopower. Second, as mobility decreases an apparent crossover to $p$ type occurs, first in thermopower, then in Hall measurements. This can be understood, however, in terms of the crossover from diffusive to hopping transport that is clearly reflected in resistivity. Third, universal behavior is found for both crystals and films, suggesting a common $n$ dopant, possibly sulfur vacancies. We thus argue that $n$-type doping is facile in $\mathrm{Fe}{\mathrm{S}}_2$ films, that apparent $p$-type behavior in low mobility samples can be an artifact of hopping, and that the prevailing notion of predominantly $p$-type films must be revised. These conclusions have deep implications, both for interpretation of prior work on $\mathrm{Fe}{\mathrm{S}}_2$ solar cells and for the design of future studies.

We have measured in situ the progression of dewetting from a large number of holes in immiscible polymer bilayer films. Using x-ray photon correlation spectroscopy (XPCS) in grazing incidence we probe independently the evolving dewetting process both at the top surface and the buried interface of the bilayer. At an early stage, differences in the evolution of the velocities measured by XPCS between the surface and buried interface indicate that the holes do not penetrate the bottom layer. The rim velocity at late stages decays according to a wave-vector-dependent power law, which indicates inhomogeneous flows in the film. The changes in the static scattering show that observed slow-down of the dewetting velocity is correlated with the changing roughness at the buried interface of the polymer bilayer.

For soft materials with Young's moduli below 100 kPa, quantifying mechanical and interfacial properties by small scale indentation is challenging because in addition to adhesion and elasticity, surface tension plays a critical role. Until now, microscale contact of very soft materials has only been studied by static experiments under zero external loading. Here we introduce a combination of the colloidal probe technique and confocal microscopy to characterize the force-indentation and force-contact radius relationships during microindentation of soft silicones. We confirm that the widespread Johnson-Kendall-Roberts theory must be extended to predict the mechanical contact for soft materials. Typically a liquid component is found within very soft materials. With a simple analytical model, we illustrate that accounting for this liquid surface tension can capture the contact behavior. Our results highlight the importance of considering liquid that is often associated with soft materials during small scale contact.