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Regarding the origin of diastereo- and enantioselectivity. Computations have been performed at the MN12SX/Def2TZVPPthf(SMD) level after geometry optimization performed with the ONIOM method M06L/Def2SVP:UFFthf(PCM); Ar = 2,6-(iPr)2C6H3. See the Supporting Information for details.
