Abstract
The deployment of organic molecules in high-performance devices strongly relies on the formation of well-ordered domains, which is often complicated by the dynamic and sensitive nature of supramolecular interactions. Here, we engineered the assembly of water-processable, optoelectronic π-conjugated peptides into well-defined organic-inorganic heterointerfaced assemblies by leveraging the long-range anisotropic ordering of 1D van der Waals (vdW) crystals composed of subnanometer-thick transition metal sulfide chains (MS(3); M = Nb, Ta) as assembly templates. We found that the monomers can readily form 1D supramolecular assemblies onto the underlying crystal surface, owing to the structural correspondence between the π-π interactions of the quaterthiophene (4T)-based peptide units (DDD-4T) and sulfur atom ordering along the NbS(3) (100) surface. The heterointerfaced assemblies exhibited substantially red-shifted photoluminescence and enhanced visible-range photocurrent generation compared to solution-assembled films. Our results underscore the role of lattice matching in forming ordered supramolecular assemblies, offering an emergent approach to assembling organic building blocks endowed with improved physical properties.