The SEHRS and SERS spectra analysis of 4,4'-Bipyridine indicated existence of strong lines with vibrations transforming after a unit irreducible representation for probable geometries with D-2 and D-2h symmetry groups. They are associated with a strong quadrupole light-molecule interaction existing in this system. In addition, there are the lines caused by contributions from both the vibrations transforming after the unit irreducible representations A or A(g) and the representations B-1 and B-1u. This result is associated with the molecule geometry, when the indicated vibrations can be nearly degenerated and cannot be resolved by the SEHRS and SERS spectra analysis. (C) 2016 Elsevier B.V. All rights reserved.