The chemical bond is an important local concept to understand chemical compounds and processes. Unfortunately, like most local concepts, the chemical bond and the bond order do not correspond to any physical observable and thus cannot be determined as an expectation value of a quantum chemical operator. We recently demonstrated [Boguslawski et al., J. Chem. Theory Comput., 2013, 9, 2959-2973] that one- and two-orbital-based entanglement measures can be applied to interpret electronic wave functions in terms of orbital correlation. Orbital entanglement emerged as a powerful tool to provide a qualitative understanding of bond-forming and bond-breaking processes, and allowed for an estimation of bond orders of simple diatomic molecules beyond the classical bonding models. In this article we demonstrate that the orbital entanglement analysis can be extended to polyatomic molecules to understand chemical bonding.

Superior stability and safety are key promises attributed to all-solid-state batteries (ASSBs) containing solid-state electrolyte (SSE) compared to their conventional counterparts utilizing liquid electrolyte. To unleash the full potential of ASSBs, SSE materials that are stable when in contact with the low and high potential electrodes are required. The electrochemical stability window is conveniently used to assess the SSE-electrode interface stability. In the present work, we review the most important methods to compute the SSE stability window. Our analysis reveals that the stoichiometry stability method represents a bridge between HOMO-LUMO method and phase stability method (grand canonical phase diagram). Moreover, we provide computational implementations of these methods for SSE material screening. We compare 1 arXiv:1901.02251v2 [cond-mat.mtrl-sci] 25 Oct 2019 their results for the relevant Li-and Na-SSE materials LGPS, LIPON, LLZO, LLTO, LATP, LISICON, and NASICON, and we discuss their relation to published experimental stability windows.

To shed light on the impact of doping on the conductivity of garnet-type electrolytes, we use molecular dynamics with an ab-initio designed force-field to investigate the complex interplay between the carrier concentration and the kinetic and thermodynamic changes induced by the addition of hypervalent dopants. We particularly focus on the effect of the distribution of the doping agents and find that there is a need to perform a proper average over the frozen disorder introduced by the doping. We observe the competing effect between the decrease in concentration

Molecular modeling using polarizable force fields of W-doped lithium containing garnets to understand the various aspect of the impact of doping on the lithium dynamics and conductivity.<br>

No abstract

Molecular modeling using polarizable force fields of W-doped lithium containing garnets to understand the various aspect of the impact of doping on the lithium dynamics and conductivity.<br>