We report the temperature-dependent infrared spectra of pure, deuterated, Zn-doped, and 2,6-dimethyl-substituted samples of the S ) 1 / 2 , one-dimensional Quantum Heisenberg Antiferromagnet (QHAF) copper pyrazine dinitrate (Cu(C 4 H 4 N 2 )(NO 3 ) 2 ). Of the more than 100 vibrational modes observed in the spectra, nearly one-third of them unexpectedly soften throughout the temperature range of investigation (300-5 K). We discuss the temperature dependence of the vibrational spectra in terms of several different models for mode softening. On the basis of detailed structural information and a comparison of the infrared spectra between pure copper pyrazine dinitrate and its chemically modified relatives, we conclude that the unusual softening observed in this low-dimensional molecular magnet is due to enhanced interchain hydrogen bonding with decreasing temperature.