“…The Raman spectra of 2 – 6 measured at 150 K and 290 K are shown in Figure . The broad overlapped peaks between 3,100 and 3,300 cm −1 are all due to hydrogen‐bonded NH stretching in the tape, as confirmed via N ‐deuteration of 2 and previous studies (Figure S3 and Table S2). Deuteration also leads to the peak at 1,621 cm −1 in 2 splitting into a peak at 1,609 cm −1 , assigned to ring deformation, and a new peak at 1,187 cm −1 for ND deformation, indicating that peaks in the range 1,604–1,627 cm −1 in all derivatives can be assigned to overlapping NH deformation, CN stretching, and in‐plane ring deformation modes.…”