Thesis advisor: Michael J. Naughton / Quasi-one dimensional (Q1D) molecular organic conductors are among the most exciting materials in condensed matter physics, exhibiting nearly every known ground state. They are highly anisotropic, structurally and electronically, and show large oscillatory phenomena in conductivity for magnetic field rotated in different crystalline planes. Several theoretical works have been published to explain these angular magnetoresistance oscillation (AMRO) effects, but the underlying physics remains illunderstood. Here, we present measurements and calculations of magnetotransport in the molecular organic (super)conductor (DMET)₂I₃ which detect and simulate all known AMRO phenomena for Q1D systems. Employing, for the first time, the true triclinic crystal structure in the calculations, these results address the mystery of the putative vanishing of the primary AMRO phenomenon, the Lebed magic angle effect, for orientations in which it is expected to be strongest. They also show a common origin for Lebed and so-called "Lee-Naughton" oscillations, and confirm the generalized nature of AMRO in Q1D systems. Furthermore, we report the temperature dependence of the upper critical magnetic field in (DMET)₂I₃, for magnetic field applied along the intrachain, interchain, and interplane directions. The upper critical field exhibits orbital saturation at low temperature for field in all directions, implying that superconductivity in (DMET)₂I₃ is conventional spin singlet. / Thesis (PhD) — Boston College, 2010. / Submitted to: Boston College. Graduate School of Arts and Sciences. / Discipline: Physics.