Fig. 1. (a) Building block content and molecular patterns previously identified.14 (b) Structure of the oligo-dynablock proposed here based upon solid-state NMR analysis. (c) 2D DCP ¹⁵N–¹³C HETCOR spectrum for partially ¹³C and fully ¹⁵N enriched DM^A₂(CO₂)*. Correlations between nitrogen atoms (black labels) and carbon atoms (red labels) are indicated by dashed lines. (d) 100 K DNP-enhanced 2D refocused INADEQUATE ¹³C–¹³C correlation spectrum (aromatic region only) acquired from natural isotopic abundance DM^A₂(CO₂) impregnated with a 16 mM solution of TEKPol in 1,1,2,2-tetrachloroethane. Correlations/connectivity are indicated by solid orange lines and provide iterative assignment of green labels. (e) Aliphatic region of the 2D refocused INADEQUATE ¹³C–¹³C correlation spectrum (provides unambiguous assignments of purple labels). By combining the information in the 2D DCP ¹⁵N–¹³C HETCOR spectrum and the 2D refocused INADEQUATE ¹³C–¹³C correlation spectrum it is possible to completely assign the spectra and propose the model chemical structure for the oligo-dynablock shown in (b). Carbon resonances are numbered on the spectra and assigned to the proposed structure of DM^A₂(CO₂).