TY - DATA T1 - Local Structure and Dynamics of Lithium Garnet Ionic Conductors: A Model Material Li5La3Ta2O12 PY - 2014/10/14 AU - Yuxing Wang AU - Matthew Klenk AU - Katharine Page AU - Wei Lai UR - https://acs.figshare.com/articles/media/Local_Structure_and_Dynamics_of_Lithium_Garnet_Ionic_Conductors_A_Model_Material_Li_sub_5_sub_La_sub_3_sub_Ta_sub_2_sub_O_sub_12_sub_/2245360 DO - 10.1021/cm502133c.s002 L4 - https://ndownloader.figshare.com/files/3881317 KW - lithium conduction path KW - lithium atoms KW - lithium atoms hop KW - dynamic KW - garnet oxide Li 5La KW - Td KW - lithium distribution KW - lithium structure KW - lithium clusters KW - RMC KW - bottleneck KW - conduction mechanism KW - Lithium Garnet KW - MD studies support KW - cage KW - 3 D KW - structure instability KW - Local Structure KW - Model Material Li 5La N2 - In this article, we combined two complementary structure/dynamics probes, i.e., total-scattering/reverse Monte Carlo (RMC) modeling and classical molecular dynamics (MD), in order to understand local lithium structure and dynamics in a model disordered garnet oxide Li5La3Ta2O12. By examining the configurations from RMC and trajectories from MD, we individually and statistically analyzed the lithium distribution and dynamics within tetrahedral (Td) cages, octahedral (Oh) cages, and triangular bottlenecks. We found that lithium atoms within either Td or Oh cages prefer to stay at the off-center positions and close to one of the triangular bottlenecks. This is likely caused by the uneven Li–Li interaction in the form of lithium clusters, and such geometrical frustration leads to the local structure instability and fast ionic conduction. Both RMC and MD studies support that the lithium conduction path goes through the triangular bottleneck in a 3D continuous network of Td/Oh cages, without a direct Oh to Oh jump. However, the conduction mechanism should not be generalized, as it is greatly influenced by the local environment or temperature. Broadly speaking, lithium atoms hop through the bottleneck from an edge-passing mechanism at low temperatures to a center-passing mechanism at higher temperatures. ER -