An <i>ab initio</i> Langevin dynamics approach is developed based on stochastic density functional theory (sDFT) within a new embedded saturated fragment formalism, applicable to covalently bonded systems. The forces on the nuclei generated by sDFT contain a random component natural to Langevin dynamics and its standard deviation is used to estimate the friction term on each atom by satisfying the fluctuation-dissipation relation. The overall approach scales linearly with system size even if the density matrix is not local and is thus applicable to ordered as well as disordered extended systems. We implement the approach for a series of silicon nanocrystals (NCs) of varying size with a diameter of up to 3 nm corresponding to N<sub>e</sub>=3000 electrons and generate a set of configurations that are distributed canonically at a fixed temperature, ranging from cryogenic to room temperature. We also analyze the structure properties of the NCs and discuss the reconstruction of the surface geometry. The method is extended to periodic boundary conditions and is shown higly efficient for studying warm dense matter. We show that the pressure-density and bulk moduls can be determined for WDM silicon. A transition from elastic to plastic material is described.

Stochastic adventures in density functional theory and beyond

255th National Meeting (2018)

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