Support for the tetrameric model as well as detailed analysis of the origin of enantioselection in the Soai reaction was recently reported by Denmark, Houk and coworkers. 37 As was shown in Scheme 6a, Soai had reported autocatalysis without chiral amplification for unsubstituted pyridine carbaldehyde; however, they never revisited this reaction with substituted pyridine carbaldehydes. Interestingly, Denmark found that pyridine-based carbaldehyde substrate 15 with bulky substitution para to the aldehyde group not only acted as a tetrameric autocatalyst but also exhibited amplification of ee beyond that predicted by the stochastic model (Figure ). This work helps to demonstrate how para substitution increases enantioselection beyond that predicted by the stochastic model. Calculations found that in this case the heterochiral tetramer is more stable by 2.1 kcal/mol, and it is inactive as a catalyst. This work provides a detailed interpretation of how three phenomena -autocatalysis, nonlinear effects, and enantioselection -combine to rationalize the emergence of homochirality in the Soai autocatalytic reaction. They suggest that their analysis may serve as a platform for further studies and explorations in the asymmetric autocatalysis.