Publication date: 15th May 2025
Inorganic nanocrystals (NCs) and related nanomaterials have attracted considerable attention for light-harvesting and catalytic applications due to their large extinction coefficients and tunable optical properties. Realizing these applications often require replacing the native, inert ligands on NC surfaces with functional molecules without compromising the structural or electronic integrity of the nanomaterials. However, the heterogeneous nature of NC surfaces and complex ligand–ligand and ligand–surface interactions make it challenging to achieve precise control over ligand placement and organization. In this work, we examine how ligand design and the surface binding landscape influence the organization of functional ligands at the inorganic–organic interface and modulate charge and energy transfer between NC donors and molecular acceptors. In a blue-to-UV photon upconversion system sensitized by CsPbBr₃ NCs, we studied structural isomers of naphthalene ligands to identify design principles that facilitate efficient energy transfer and upconversion. Ligands with nonplanar geometries and carboxylate anchoring groups exhibit enhanced binding affinity and donor–acceptor electronic coupling, leading to accelerated energy transfer. To further examine the role of ligand–surface interactions, we investigated how size-dependent surface morphologies of PbS NCs influence the binding behavior of perylene diimide (PDI) ligands. Based on experimental results and Monte Carlo simulations, PDI ligands preferentially bind at vertex and edge sites, promoting aggregation and slowing electron transfer even when larger NCs provide much more surface binding sites. Together, these examples highlight how spatial and chemical control over the ligands plays a crucial role in enabling efficient energy and charge transport at the inhomogeneous NC interfaces.
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