In an effort to scale down electronic devices to atomic dimensions, the use of transition-metal oxides may provide advantages over conventional semiconductors. Their high carrier densities and short electronic length scales are desirable for miniaturization, while strong interactions that mediate exotic phase diagrams open new avenues for engineering emergent properties. Nevertheless, understanding how their correlated electronic states can be manipulated at the nanoscale remains challenging. Here, we use angle-resolved photoemission spectroscopy to uncover an abrupt destruction of Fermi liquid-like quasiparticles in the correlated metal LaNiO₃ when confined to a critical film thickness of two unit cells. This is accompanied by the onset of an insulating phase as measured by electrical transport. We show how this is driven by an instability to an incipient order of the underlying quantum many-body system, demonstrating the power of artificial confinement to harness control over competing phases in complex oxides with atomic-scale precision.
We employ reactive molecular-beam epitaxy to synthesize the metastable perovskite SrIrO3 and utilize in situ angle-resolved photoemission to reveal its electronic structure as an exotic narrowband semimetal. We discover remarkably narrow bands which originate from a confluence of strong spin-orbit interactions, dimensionality, and both in-and out-of-plane IrO6 octahedral rotations. The partial occupation of numerous bands with strongly mixed orbital characters signals the breakdown of the single-band Mott picture that characterizes its insulating two-dimensional counterpart, Sr2IrO4, illustrating the power of structure-property relations for manipulating the subtle balance between spin-orbit interactions and electron-electron interactions. PACS numbers: Keywords:The combination of strong spin-orbit interactions (SOIs) with electron-electron correlations has recently been predicted to realize a variety of novel quantum states of matter, including topological Mott insulators [1, 2], quantum spin Hall, quantum anomalous Hall, and axion insulators [3-6], Weyl semimetals [7], and even high temperature superconductors [8]. Although typically viewed to be disparate properties, the recent discovery that SOI can sufficiently enhance the effective role of electron correlations to stabilize a Mott-like insulating state in the quasi-two-dimensional 5d transition metal oxide Sr 2 IrO 4 [9, 10] has opened a new frontier for exploring the rare interplay between these 2 degrees of freedom. Its three-dimensional perovskite analogue, SrIrO 3 , has been theoretically proposed as a key building block for engineering topological phases at interfaces and in superlattices [3,11,12]. In bulk, SrIrO 3 is believed to lie in close proximity to a metal-insulator transition [13,14], yet little is known of its electronic structure to date.Here we reveal the momentum-resolved electronic structure of SrIrO 3 using a combination of reactive oxide molecular-beam epitaxy (MBE) and in situ angleresolved photoemission spectroscopy (ARPES). Our measurements uncover an exotic semimetallic ground state, hosting an unusual coexistence of heavy holelike and light electronlike bands. Contrary to conventional expectations that increased coordination leads to broader bands in higher-dimensional materials [13], we find that the bandwidths of SrIrO 3 are, instead, narrower than its insulating two-dimensional counterpart. By combining first-principles calculations with spectroscopic measurements, we uncover the surprising interplay of spinorbit interactions, dimensionality, and octahedral rotations which drives the narrow-band, semimetallic state in SrIrO 3 . Our results indicate that subtle changes in the structure and rotation angles should drive substantial changes in the electronic structure and physical properties of SrIrO 3 . This highlights the important structure-property relationships in correlated quantum materials [15,16], much like in ferroelectrics and multiferroics [17]. This Letter also underscores that simple toy models which neglect these str...
We report the scalable growth of aligned graphene and hexagonal boron nitride on commercial copper foils, where each film originates from multiple nucleations yet exhibits a single orientation. Thorough characterization of our graphene reveals uniform crystallographic and electronic structures on length scales ranging from nanometers to tens of centimeters. As we demonstrate with artificial twisted graphene bilayers, these inexpensive and versatile films are ideal building blocks for large-scale layered heterostructures with angle-tunable optoelectronic properties.
Angle-resolved photoemission reveals the emergence of complex orbital texture concomitant with spin splitting in the Rashba compound BiTeI.
The transition temperature Tc of unconventional superconductivity is often tunable. For a monolayer of FeSe, for example, the sweet spot is uniquely bound to titanium-oxide substrates. By contrast for La2−xSrxCuO4 thin films, such substrates are sub-optimal and the highest Tc is instead obtained using LaSrAlO4. An outstanding challenge is thus to understand the optimal conditions for superconductivity in thin films: which microscopic parameters drive the change in Tc and how can we tune them? Here we demonstrate, by a combination of x-ray absorption and resonant inelastic x-ray scattering spectroscopy, how the Coulomb and magnetic-exchange interaction of La2CuO4 thin films can be enhanced by compressive strain. Our experiments and theoretical calculations establish that the substrate producing the largest Tc under doping also generates the largest nearest neighbour hopping integral, Coulomb and magnetic-exchange interaction. We hence suggest optimising the parent Mott state as a strategy for enhancing the superconducting transition temperature in cuprates.
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