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The BaAl4 prototype crystal structure is the most populous of all structure types, and is the building block for a diverse set of sub-structures including the famous ThCr2Si2 family that hosts high-temperature superconductivity and numerous magnetic and strongly correlated electron systems. The MA4 family of materials (M = Sr, Ba, Eu; A = Al, Ga, In) themselves present an intriguing set of ground states including charge and spin orders, but have largely been considered as uninteresting metals. We predict the exemplary compound BaAl4 to harbor a three-dimensional Dirac spectrum with non-trivial topology and possible nodal lines crossing the Brillouin zone, wherein one pair of semi-Dirac points with linear dispersion along the kz direction and quadratic dispersion along the kx/ky direction resides on the rotational axis with C4v point group symmetry. An extremely large, unsaturating positive magnetoresistance in BaAl4 despite an uncompensated band structure is revealed, and quantum oscillations and angle-resolved photoemission spectroscopy measurements confirm the predicted multiband semimetal structure with pockets of Dirac holes and a Van Hove singularity (VHS) remarkably consistent with the theoretical prediction. We thus present BaAl4 as a topological semimetal, casting its prototype status into a role as a building block for a vast array of topological materials.

While long-theorized, the direct observation of multiple highly dispersive C60 valence bands has eluded researchers for more than two decades due to a variety of intrinsic and extrinsic factors. Here we report a realization of multiple highly dispersive (330-520 meV) valence bands in pure thin film C60 on a novel substrate - the three-dimensional topological insulator Bi2Se3 - through the use of angle-resolved photoemission spectroscopy (ARPES) and first-principles calculations. The effects of this novel substrate reducing C60 rotational disorder are discussed. Our results provide important considerations for past and future band structure studies as well as the increasingly popular C60 electronic device applications, especially those making use of heterostructures.

Recent direct experimental observation of multiple highly dispersive C 60 valence bands has allowed for a detailed analysis of the unusual photoemission traits of these features through photon energy- and polarization-dependent measurements. Previously obscured dispersions and strong photoemission traits are now revealed by specific light polarizations. The observed intensity effects prove the locking in place of the C 60 molecules at low temperatures and the existence of an orientational order imposed by the substrate chosen. Most importantly, photon energy- and polarization-dependent effects are shown to be intimately linked with the orbital character of the C 60 band manifolds which allow for a more precise determination of the orbital character within the third highest occupied molecular orbital (HOMO-2). Our observations and analysis provide important considerations for the connection between molecular and crystalline C 60 electronic structure, past and future band structure studies, and for increasingly popular C 60 electronic device applications, especially those making use of heterostructures.

Charge transfer at the interface between dissimilar materials is at the heart of electronics and photovoltaics. Here we study the molecular orientation, electronic structure, and local charge transfer at the interface region of C 60 deposited on graphene, with and without supporting substrates such as hexagonal boron nitride. We employ ab initio density functional theory with van der Waals interactions and experimentally characterize interface devices using high-resolution transmission electron microscopy and electronic transport. Charge transfer between C 60 and the graphene is found to be sensitive to the nature of the underlying supporting substrate and to the crystallinity and local orientation of the C 60 . Even at room temperature, C 60 molecules interfaced to graphene are orientationally locked into position. High electron and hole mobilities are preserved in graphene with crystalline C 60 overlayers, which has ramifications for organic high-mobility field-effect devices.