The Soret coefficient from a given Langevin NEMD simulation is associated with the mean temperature in the fit region, which is the common practice when handling the rather complicated temperature-dependency of thermodiffusion quantities. Typically, Soret coefficient data from NEMD simulations should be extrapolated to the zero-force regime, 32;80;39 where a linear function can be used. However, MacGowan and Evans estimated zero-force transport coefficients by weighted averaging if a distinct force dependence of a given coefficient could not be detected. On the one hand, the variation of the Soret coefficient is typically small for different thermodynamic driving forces around a given state point in this work (Figure ). On the other hand, the average value of the temperature in the gradient fit region does not exactly match the target temperature (i.e., mean value of imposed high and imposed low temperature), but the deviations are small: a few percent. Furthermore, the Soret coefficient data determined with different gradients and at different temperatures usually exhibit consistent temperature trends (Figure ). Therefore, comparison to EMD predictions, in which the target temperature is reached exactly, was facilitated by interpolation. Specifically, S T and its standard deviation were linearly interpolated in the small window around the target temperature to provide the most likely values at the target temperature. ). The color from blue to orange indicates an increasing relative temperature difference ∆T /T in the Langevin NEMD simulations. Open symbols represent linear interpolations of S T and its standard deviation around the desired target temperature T target . Corresponding plots for the other two Lennard-Jones mixtures are provided in the Supporting Information (Figure ).