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Charge transfer between a metal and its ligand is fundamental for the structure and reactivity of a metal complex as it directly dictates the distribution of electron density within the complex. To better understand such charge transfer interactions, we studied the vibrational spectra of mass-selected MOH(H2O)(+) (M = Mn, Fe, Co, Ni, Cu, or Zn) complexes, acquired using cryogenic ion infrared predissociation spectroscopy. We find that there is a partial charge transfer from the hydroxide anion to the metal center for these first-row transition metals, the extent of which is in the order of Mn &lt; Fe &lt; Co &lt; Ni &lt; Cu &gt; Zn, dictated by the 2nd ionization energy of the bare metal. This gradual change across the metal series points to the complexity in the electronic structures of these transition metal complexes. Interestingly, the hydroxide ligand in these complexes can serves as a sensitive in situ probe of this charge transfer. Its vibrational frequency varies by &gt;150 cm(-1) for different metal species, and it is dependent on the electric field produced by the charged metal center. This dramatic vibrational Stark shift is further modulated by the charge present on the hydroxide itself, providing a well-defined relationship between the observed hydroxide frequency and the effective electric field.

Charge transfer in MOH(H2O)+ (M = Mn, Fe, Co, Ni, Cu, Zn) complexes revealed by vibrational spectroscopy of mass-selected ions

Charge transfer in MOH(H₂O)⁺ (M = Mn, Fe, Co, Ni, Cu, Zn) complexes revealed by vibrational spectroscopy of mass-selected ions