Spectroscopic Investigations of Complex Transition Metal Oxides

In this dissertation, I present spectroscopic studies of several model electronic and magnetic materials. Compounds of interest include VOx nanoscrolls, VOHPO4¢ 1 2H2O, and (La0:4Pr0:6)1:2Sr1:8Mn2O7. These materials are attractive systems for the investigation of optical gap tuning, lattice and charge dynamics, spin-lattice-charge coupling, and hydrogen bonding effects. I measured the optical properties of VOx nano- scrolls and the ion-exchanged derivatives to investigate the lattice and charge degrees of freedom. Selected V-O-V stretching modes sharpen and redshift with increasing amine size, which are microscopic manifestations of strain. We observed bound carrier localization in the metal exchanged nanoscrolls, indicating they are weakly metallic in their bulk form. I also investigated the variable temperature vibrational properties of single crystals of the S = 1/2 Heisenberg antiferromagnet VOHPO4¢ 1 2H2O. In order to explain the activation and polarization dependence of the singlet-to-triplet gap in the far-infrared response, we invoke a dynamic Dzyaloshinskii-Moriya mechanism and we identify the low-energy phonons that likely facilitate this coupling. Vibrational mode splitting of VOHPO4¢ 1 2H2O also points toward a weak local symmetry breaking near 180 K, and the low-temperature redshift of V-O and H-O related modes demonstrates enhanced low-temperature hydrogen bonding. Finally, I measured the magneto-optical response of (La0:4Pr0:6)1:2Sr1:8Mn2O7 to investigate the microscopic aspects of the magnetic field driven spin-glass insulator to ferromagnetic metal transition. Application of a magnetic field recovers the ferromagnetic state with an overall redshift of the electronic structure, growth of the bound carrier localization associated with ferromagnetic domains, development of a pseudogap, and softening of the Mn-O stretching and bending modes that indicate a structural change. By exploiting the electronic mechanisms, we can induce large high energy magnetodielectric contrast in (La0:4Pr0:6)1:2Sr1:8Mn2O7. The dielectric contrast is over 100% near 0.8 eV at 4.2 K. Remnants of the transition also drive the high energy magnetodielectric effect at room temperature.