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The on‐surface synthesis of graphene nanoribbons (GNRs) allows for the fabrication of atomically precise narrow GNRs. Despite their exceptional properties which can be tuned by ribbon width and edge structure, significant challenges remain for GNR processing and characterization. Herein, Raman spectroscopy is used to characterize different types of GNRs on their growth substrate and track their quality upon substrate transfer. A Raman‐optimized (RO) device substrate and an optimized mapping approach are presented that allow for the acquisition of high‐resolution Raman spectra, achieving enhancement factors as high as 120 with respect to signals measured on standard SiO 2 /Si substrates. This approach is well suited to routinely monitor the geometry‐dependent low‐frequency modes of GNRs. In particular, the radial breathing‐like mode (RBLM) and the shear‐like mode (SLM) for 5‐, 7‐, and 9‐atom‐wide armchair GNRs (AGNRs) are tracked and their frequencies are compared with first‐principles calculations.

Optimized Substrates and Measurement Approaches for Raman Spectroscopy of Graphene Nanoribbons