Butterfly Magnetoresistance, Quasi-2D Dirac Fermi Surfaces, and a Topological Phase Transition in ZrSiS

Magnetoresistance (MR), the change of a material's electrical resistance in response to an applied magnetic field, is a technologically important property that has been the topic of intense study for more than a quarter century. Here we report the observation of an unusual "butterfly" shaped titanic angular magnetoresistance (AMR) in the non-magnetic, Dirac material, ZrSiS. The MR is large and positive, reaching nearly 1.8 x 10^5 percent at 9 T and 2 K at an angle of 45o between the applied current (along the a-axis) and the applied field (90o is H parallel to the c-axis). Approaching 90o, a "dip" is seen in the AMR which can be traced to an angle dependent deviation from the H^2 law. By analyzing the SdH oscillations at different angles, we find that ZrSiS has a combination of 2D and 3D Dirac pockets comprising its Fermi surface and that the anomalous transport behavior coincides with a topological phase transition whose robust signature is evident despite transport contributions from other parts of the Fermi surface. We also find that as a function of angle, the temperature dependent resistivity in high field displays a broad peak-like behavior, unlike any known Dirac/Weyl material. The combination of very high mobility carriers and multiple Fermi surfaces in ZrSiS allow for large bulk property changes to occur as a function of angle between applied fields makes it a promising platform to study the physics stemming from the coexistence of 2D and 3D Dirac electrons.