Jalem, RRJalemNakayama, MMNakayamaManalastas, WWManalastasKilner, JAJAKilnerGrimes, RWRWGrimesKasuga, TTKasugaKanamura, KKKanamura2016-05-052015-08-182016-05-052015-08-18Journal of Physical Chemistry C, 2015, 119 (36), pp.20783-207911932-7455http://hdl.handle.net/10044/1/32076© 2015 American Chemical Society.Garnet-type solid electrolytes are a class of materials that could potentially revolutionize Li-ion battery technology. In this work, ab-initio-based MD simulations have been performed to investigate the ion dynamics in pure garnet-type cubic Li<inf>5</inf>La<inf>3</inf>Ta<inf>2</inf>O<inf>12</inf> (LLTaO) over the temperature range from 873 to 1773 K. A strong tendency for disorder in the Li sublattice was verified for LLTaO that explains the relative ease of stabilizing the reported cubic phase for this material. The Li⁺ conduction mechanism was determined to be facilitated by a cooperative hopping process characterized by long, multiple-site successive hops with a very small time scale for fluctuations at intermediate positions. A comparative study is also carried out between LLTaO and garnet-type Li<inf>7</inf>La<inf>3</inf>Zr<inf>2</inf>O<inf>12</inf> (LLZrO), another candidate solid electrolyte.This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.Physical Chemistry09 Engineering03 Chemical Sciences10 TechnologyJournal Articlehttps://www.dx.doi.org/10.1021/acs.jpcc.5b050681932-7455