x([Li][NTf 2 ]) = 0.75, this method was not applied at any temperature. This was due to the decreased mobility of these mixtures and the long simulation length needed to achieve comparable statistical accuracy for all OrthoBoXY simulations. On this account, all simulations that would require simulation lengths of more than 5 µs were omitted. The simulations were performed under N pT conditions analogous to the cubic systems given above. Here, the system sizes were scaled by a factor of 1/4 for the systems with x([Li][NTf 2 ]) = 0.037 to 0.33 and by a factor of 1/6 for x([Li][NTf 2 ]) = 0.40 to 0.50, given the system-size independence of D 0 . The resized cubic boxes were equilibrated for 2 ns and then reshaped into orthorhombic box geometries with box length ratios of L z /L x = L z /L y ≈ 2.7933596497. For exemplary snapshots, see the SI. The simulation lengths for each system were determined following the suggestions of Busch and Paschek, factoring in self-diffusion coefficients obtained from cubic systems as well as the average diameter of the molecules in the mixtures. All simulation lengths are given in Table of the SI. Simulations were divided into 40 segments, and properties were calculated for each segment to estimate uncertainties using standard statistical methods.