Giulliana Materzanini^1,2*, Leonid Kahle^1,2*, Aris Marcolongo^3,2*, Nicola Marzari^1,2*

1 Theory and Simulations of Materials (THEOS), École Polytechnique Fedérale de Lausanne, 1015 Lausanne, Switzerland

2 National Centre for Computational Design and Discovery of Novel Materials (MARVEL), 1015 Lausanne, Switzerland

3 IBM RSM Zurich Research Laboratory, Zurich, Switzerland

* Corresponding authors emails: giuliana.materzanini@epfl.ch, leonid.kahle@gmail.com, aris.marcolongo@gmail.com, nicola.marzari@gmail.com

DOI10.24435/materialscloud:rs-1t [version v1]

Publication date: Jan 22, 2021

How to cite this record

Giulliana Materzanini, Leonid Kahle, Aris Marcolongo, Nicola Marzari, High Li-ion conductivity in tetragonal LGPO: a comparative first-principles study against known LISICON and LGPS phases, Materials Cloud Archive 2021.15 (2021), doi: 10.24435/materialscloud:rs-1t.

Description

This work presents extensive first-principles (Car-Parrinello) molecular dynamics simulations of the solid-state electrolyte Li10GeP2O12 (LGPO) in a tetragonal phase -not synthesized so far- that is isostructural to the highly Li-ion conductive tetragonal phase of the sulfide analogue Li10GeP2S12 (LGPS). We provide comparative simulations of the experimentally known orthorhombic phase of LGPO (that we call here LISICON, from the family of superionic conductors to which LGPO belongs) and of the two experimentally known phases of LGPS, quasi-orthorhombic (called thio-LISICON) and tetragonal. We extract diffusion coefficients from fixed-cell simulations in the canonical ensemble and we study dynamical stability from variable-cell simulations in the isobaric-isothermal ensemble. The main outcome of this work is that, according to these simulations, although tetragonal LGPO is less stable than its orthorhombic allotrope, it exhibits a much higher conductivity, comparable to that presently estimated for both phases of LGPS. These results indicate that hypothetical tetragonal LGPO, if synthesized, could make a very attractive Li-ion conductor.

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File name	Size	Description
STRUCTURES.tar.gz MD5md5:b56fa800b7e854344b8a3bc2c531916a	15.4 KiB	Structural data of the LGPO and LGPS phases studied in the record
TRAJECTORIES.tar.gz MD5md5:da3da23fce1d918c8b46ba30016a838f	14.1 GiB	Data of the first-principles molecular dynamics simulations presented and discussed in the record
README.txt MD5md5:80095946214bf0ea85a3826beafc5cd9	2.6 KiB	Brief description of "STRUCTURES.tar.gz" and "TRAJECTORIES.tar.gz" archives content

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Keywords

solid-state electrolytes first-principles molecular dynamics LISICON LGPO LGPS ionic transport dynamical stability ionic conductivity MARVEL/Inc1 SNSF CSCS