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Abstract Graphene is a privileged 2D platform for hosting confined light-matter excitations known as surface plasmon polaritons (SPPs), as it possesses low intrinsic losses and a high degree of optical confinement. However, the isotropic nature of graphene limits its ability to guide and focus SPPs, making it less suitable than anisotropic elliptical and hyperbolic materials for polaritonic lensing and canalization. Here, we present graphene/CrSBr as an engineered 2D interface that hosts highly anisotropic SPP propagation across mid-infrared and terahertz energies. Using scanning tunneling microscopy, scattering-type scanning near-field optical microscopy, and first-principles calculations, we demonstrate mutual doping in excess of 10¹³cm^–2holes/electrons between the interfacial layers of graphene/CrSBr. SPPs in graphene activated by charge transfer interact with charge-induced electronic anisotropy in the interfacial doped CrSBr, leading to preferential SPP propagation along the quasi-1D chains that compose each CrSBr layer. This multifaceted proximity effect both creates SPPs and endows them with anisotropic propagation lengths that differ by an order-of-magnitude between the in-plane crystallographic axes of CrSBr. 

Abstract In this manuscript, we report the first demonstration of controlled helicity in extended graphene nanoribbons (GNRs). We present a wealth of new graphene nanoribbons that are a direct consequence of the high‐yielding and robust synthetic method revealed in this study. We created a series of defect‐free, ultralong, chiral cove‐edged graphene nanoribbons where helical twisting of the graphene nanoribbon backbone is tuned through functionalization with chiral side chains.S‐configured point chiral centers in the side chains transfer their chiral information to induce a helically chiral, right‐handed twist in the graphene nanoribbon. As the backbone is extended, these helically twisted graphene nanoribbons exhibit a substantial increase in their circular dichroic response. The longest variant synthesized consists of an average of 268 linearly fused rings, reaching 65 nm in average length with nearly 10 full end‐to‐end helical rotations. The structure exhibits an extraordinary |Δε| value of 6780 M⁻¹cm⁻¹at 550 nm—the highest recorded for an organic molecule in the visible wavelength range. This new chiroptic material acts as room‐temperature spin filters in thin films due to its chirality‐induced spin selectivity.