Hybrid Conjugated Nanostructures of Polythiophene and Carbon Allotropes: Simulation‐Based Probing of Structural and Electronic Interplay

ABSTRACT The understanding of molecular interactions and charge delocalization mechanisms under polythiophene system environments is essential to improving their catalytic function in energy and electronic capacities. In this study a more holistic computational research approach is used to assess the conformational dynamics and interfacial compatibility of polythiophene with different carbon nanomaterials: graphene, carbon nanotubes (CNTs), fullerene (C60), and carbon nanoparticles. Interaction energies (Eint) and structural conformations were evaluated using quantum mechanical density functional theory (DFT) and reactive force field (ReaxFF) simulations in Materials Studio to further rationalize electronic coupling and charge delocalization. Polythiophene–graphene interface exhibited a highly favorable interaction energy (−205.94 kJ/mol) among those studied, favoring π–π stacking and making charge transfer highly effective, with CNTs being the next most favorable (−39.11 kJ/mol) compared to fullerene (−25.29 kJ/mol) and carbon nanoparticles (−21.97 kJ/mol). These findings offer valuable molecular‐level insights for the rational design of polythiophene‐based catalytic composites, paving the way for improved performance in photocatalysis, electrocatalysis, and molecular electronics.