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Register a new userAccessing the spectral function of in operando devices by angle-resolved photoemission spectroscopy
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Philip Hofmann
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Progress in performing angle-resolved photoemission spectroscopy (ARPES) with high spatial resolution in the order of 1~$mu$m or less (nanoARPES) has opened the possibility to map the spectral function of solids on this tiny scale and thereby obtain detailed information on the materials emph{local} electronic band structure and many-body interactions. Recently, nanoARPES has been used to study simple electronic devices, based on two-dimensional materials, with the possibility of tuning the carrier type and density by field effect-gating, and while passing a current through the device. It was demonstrated that nanoARPES can detect possible changes in the materials electronic structure in these situations and that it can map the local doping, conductance and mobility. This article reviews these first emph{in operando} ARPES results on devices, discusses the resulting new insights, as well as the perspectives for future developments of the technique.
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Samples of Nd(2-x)Ce(x)CuO(4), an electron-doped high temperature superconducting cuprate (HTSC), near optimal doping at x = 0.155 were measured via angle resolved photoemission (ARPES). We report a renormalization feature in the self energy (kink) in the band dispersion at 50 - 60 meV present in nodal and antinodal cuts across the Fermi surface. Specifically, while the kink had previously only been seen in the antinodal region, it is now observed also in the nodal region, reminiscent of what has been observed in hole-doped cuprates.
The presence of an electrical transport current in a material is one of the simplest and most important realisations of non-equilibrium physics. The current density breaks the crystalline symmetry and can give rise to dramatic phenomena, such as sliding charge density waves [1], insulator-to-metal transitions [2,3] or gap openings in topologically protected states [4]. Almost nothing is known about how a current influences the electron spectral function, which characterizes most of the solids electronic, optical and chemical properties. Here we show that angle-resolved photoemission spectroscopy with a nano-scale light spot (nanoARPES) provides not only a wealth of information on local equilibrium properties, but also opens the possibility to access the local non-equilibrium spectral function in the presence of a transport current. Unifying spectroscopic and transport measurements in this way allows non-invasive local measurements of the composition, structure, many-body effects and carrier mobility in the presence of high current densities.
We have developed the numerical software package $chinook$, designed for the simulation of photoemission matrix elements. This quantity encodes a depth of information regarding the orbital structure of the underlying wavefunctions from which photoemission occurs. Extraction of this information is often nontrivial, owing to the influence of the experimental geometry and photoelectron interference, precluding straightforward solutions. The $chinook$ code has been designed to simulate and predict the ARPES intensity measured for arbitrary experimental configuration, including photon-energy, polarization and spin-projection, as well as consideration of both surface-projected slab and bulk models. This framework then facilitates an efficient interpretation of the photoemission experiment, allowing for a deeper understanding of the electronic structure in addition to the design of new experiments which leverage the matrix element effects towards the objective of selective photoemission from states of particular interest.
The connection between the Fermi surface and charge-density wave (CDW) order is revisited in 2H-TaSe2. Using angle-resolved photoemission spectroscopy, ab initio band structure calculations, and an accurate tight-binding model, we develop the empirical k-resolved susceptibility function, which we use to highlight states that contribute to the susceptibility for a particular q-vector. We show that although the Fermi surface is involved in the peaks in the susceptibility associated with CDW order, it is not through conventional Fermi surface nesting, but rather through finite energy transitions from states located far from the Fermi level. Comparison with monolayer TaSe2 illustrates the different mechanisms that are involved in the absence of bilayer splitting.
The localized-to-itinerant transition of f electrons lies at the heart of heavy-fermion physics, but has only been directly observed in single-layer Ce-based materials. Here, we report a comprehensive study on the electronic structure and nature of the Ce 4f electrons in the heavy-fermion superconductor Ce2PdIn8, a typical n=2 CenMmIn3n+2m compound, using high-resolution and 4d-4f resonance photoemission spectroscopies. The electronic structure of this material has been studied over a wide temperature range, and hybridization between f and conduction electrons can be clearly observed to form a Kondo resonance near the Fermi level at low temperatures. The characteristic temperature of the localized-to-itinerant transition is around 120K, which is much higher than its coherence temperature Tcoh~30K.
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