The C=C stretching modes in resonance Raman spectra and infrared reflectivity were measured at temperatures between 15 K and 300 K using various polarizations in k-(BEDT-TTF)_2Cu[N(CN)_2]Br, its fully and partially deuterated analogues, and ^{13}C-substituted analogue. The infrared- and Raman-active bands were re-assigned based on the factor group analysis. We found a Raman-active EMV-coupled u_3 mode near 1420 cm_{-1}, which shows a large downshift and broadening through the inter-dimer EMV interaction. The mixing of the bridge and ring C=C stretching vibrations depends upon the symmetry of the crystal mode. In contrast to deuterated crystals, the non-deuterated crystals show a splitting in the u_2, u_3, and u_{27} bands.
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