Unveiling the high reactivity of experimental pseudodiradical azomethine ylides within molecular electron density theoryElectronic supplementary information (ESI) available: Fig. S1 shows the ELF topological analysis of N-phenyl and N-benzyl AYs 23 and 24. Table S1 includes ωB97X-D/6-311G(d) total energies of the stationary points involved in the 32CA reactions of AY 18 with styrene 25, benzaldehyde 26, and MFB 21, in the gas phase and in benzene. Table S2 includes ωB97X-D/6-311G(d) absolute thermodynamic data of the three reactions. Table S3 gathers C1–C(O)4 and C3–C5 distances at the ωB97X-D/6-311G(d) optimized geometries of the TSs in the gas phase and in solvent. Table S4 includes the BET data along the exo stereoisomeric path of the 32CA reaction between AY 18 and styrene 25. Table S5 includes the BET data along the endo stereoisomeric path of the 32CA reaction between AY 18 and benzaldehyde 26. Fig. S2 shows the ELF topological analysis of S1 associated with the exo and endo steroisomeric reaction paths of the 32CA reactions of AY 18 with styrene 25 and benzaldeyde 26. See DOI: https://doi.org/10.1039/d2cp05032c

Unveiling the high reactivity of experimental pseudodiradical azomethine ylides within molecular electron density theoryElectronic supplementary information (ESI) available: Fig. S1 shows the ELF topological analysis of N-phenyl and N-benzyl AYs 23 and 24. Table S1 includes ωB97X-D/6-311G(d) total energies of the stationary points involved in the 32CA reactions of AY 18 with styrene 25, benzaldehyde 26, and MFB 21, in the gas phase and in benzene. Table S2 includes ωB97X-D/6-311G(d) absolute thermodynamic data of the three reactions. Table S3 gathers C1–C(O)4 and C3–C5 distances at the ωB97X-D/6-311G(d) optimized geometries of the TSs in the gas phase and in solvent. Table S4 includes the BET data along the exo stereoisomeric path of the 32CA reaction between AY 18 and styrene 25. Table S5 includes the BET data along the endo stereoisomeric path of the 32CA reaction between AY 18 and benzaldehyde 26. Fig. S2 shows the ELF topological analysis of S1 associated with the exo and endo steroisomeric reaction paths of the 32CA reactions of AY 18 with styrene 25 and benzaldeyde 26. See DOI: https://doi.org/10.1039/d2cp05032c