Bypassing the Energy Functional in Density Functional Theory: Direct Calculation of Electronic Energies from Conditional Probability Densities.

Density functional calculations can fail for want of an accurate exchange-correlation approximation. The energy can instead be extracted from a sequence of density functional calculations of conditional probabilities (CP DFT). Simple CP approximations yield usefully accurate results for two-electron ions, the hydrogen dimer, and the uniform gas at all temperatures. CP DFT has no self-interaction error for one electron, and correctly dissociates H_{2}, both major challenges. For warm dense matter, classical CP DFT calculations can overcome the convergence problems of Kohn-Sham DFT.

Modeling the transport of nanoparticle-filled binary fluids through micropores.

Understanding the transport of multicomponent fluids through porous medium is of great importance for a number of technological applications, ranging from ink jet printing and the production of textiles to enhanced oil recovery. The process of capillary filling is relatively well understood for a single-component fluid; much less attention, however, has been devoted to investigating capillary filling processes that involve multiphase fluids, and especially nanoparticle-filled fluids. Here, we examine the behavior of binary fluids containing nanoparticles that are driven by capillary forces to fill well-defined pores or microchannels. To carry out these studies, we use a hybrid computational approach that combines the lattice Boltzmann model for binary fluids with a Brownian dynamics model for the nanoparticles. This hybrid approach allows us to capture the interactions among the fluids, nanoparticles, and pore walls. We show that the nanoparticles can dynamically alter the interfacial tension between the two fluids and the contact angle at the pore walls; this, in turn, strongly affects the dynamics of the capillary filling. We demonstrate that by tailoring the wetting properties of the nanoparticles, one can effectively control the filling velocities. Our findings provide fundamental insights into the dynamics of this complex multicomponent system, as well as potential guidelines for a number of technological processes that involve capillary filling with nanoparticles in porous media.

Shear and extensional deformation of droplets containing polymers and nanoparticles.

We investigate the effects of polymer chains and nanoparticles on the deformation of a droplet in shear and extensional flow using computational modeling that accounts for both the solid and fluid phases explicitly. We show that under shear flow, both the nanoparticles and the encapsulated polymers reduce the shear-induced deformation of the droplet at intermediate capillary numbers. At high capillary numbers, however, long polymer chains can induce the breakup of the droplet. We find that the latter behavior is dependent on the nature of the imposed flow. Specifically, under extensional flow, long polymers inhibit the droplet breakup and reduce deformation. Overall, the findings provide guidelines for tailoring the stability of filled droplets under an imposed flow, and thus, the results can provide useful design rules in a range of technological applications.