Tor M. Pedersen

Dimensionality and electronic correlations are crucial elements of many quantum material properties. An example is the change of the electronic structure accompanied by the loss of quasiparticles when a metal is reduced from three dimensions to a lower dimension, where the Coulomb interaction between carriers becomes poorly screened. Here, using angle-resolved photoemission spectroscopy, we report an orbital-selective decoherence of spectral density in the perovskite nickelate LaNi O 3 toward the monolayer limit. The spectral weight of the d z 2 band vanishes much faster than that of the d x 2 − y 2 band as the thickness of the LaNi O 3 layer is decreased to a single unit cell, indicating a stronger correlation effect for the former upon dimensional confinement. Dynamical mean-field theory calculations show an orbital-selective Mott transition largely due to the localization of d z 2 electrons along the c axis in the monolayer limit. This orbital-selective correlation effect underpins many macroscopic properties of nickelates, such as metal-to-insulator transition and superconductivity, where most theories are built upon a d x 2 − y 2 – d z 2 two-band model.

We report evidence for superconductivity with onset temperatures up to 11 K in thin films of the infinite-layer nickelate parent compound NdNiO 2 . A combination of oxide molecular beam epitaxy and atomic hydrogen reduction yields samples with high crystallinity and low residual resistivities, a substantial fraction of which exhibit superconducting transitions. We survey a large series of samples with a variety of techniques, including electrical transport, scanning transmission electron microscopy, x-ray absorption spectroscopy, and resonant inelastic x-ray scattering, to investigate the possible origins of superconductivity. We propose that superconductivity could be intrinsic to the undoped infinite-layer nickelates but suppressed by disorder due to a possibly sign-changing order parameter, a finding which would necessitate a reconsideration of the nickelate phase diagram. Another possible hypothesis is that the parent materials can be hole doped from randomly dispersed apical oxygen atoms, which would suggest an alternative pathway for achieving superconductivity.

FeSe_1−xS_x remains one of the most enigmatic systems of Fe-based superconductors. While much is known about the orthorhombic parent compound, FeSe, the tetragonal samples, FeSe_1−xS_x with x > 0.17, remain relatively unexplored. Here, we provide an in-depth investigation of the electronic states of tetragonal FeSe_0.81S_0.19, using scanning tunneling microscopy and spectroscopy (STM/S) measurements, supported by angle-resolved photoemission spectroscopy (ARPES) and theoretical modeling. We analyze modulations of the local density of states (LDOS) near and away from Fe vacancy defects separately and identify quasiparticle interference (QPI) signals originating from multiple regions of the Brillouin zone, including the bands at the zone corners. We also observe that QPI signals coexist with a much stronger LDOS modulation for states near the Fermi level whose period is independent of energy. Our measurements further reveal that this strong pattern appears in the STS measurements as short range stripe patterns that are locally two-fold symmetric. Since these stripe patterns coexist with four-fold symmetric QPI around Fe-vacancies, the origin of their local two-fold symmetry must be distinct from that of nematic states in orthorhombic samples. We explore several aspects related to the stripes, such as the role of S and Fe-vacancy defects, and whether they can be explained by QPI. We consider the possibility that the observed stripe patterns may represent incipient charge order correlations, similar to those observed in the cuprates.

Machine learning has recently been applied and deployed at several light source facilities in the domain of accelerator physics. Here, an approach based on machine learning to produce a fast-executing model is introduced that predicts the polarization and energy of the radiated light produced at an insertion device. This paper demonstrates how a machine learning model can be trained on simulated data and later calibrated to a smaller, limited measured data set, a technique referred to as transfer learning. This result will enable users to efficiently determine the insertion device settings for achieving arbitrary beam characteristics.

Among the iron-based superconductors, LiFeAs is unrivaled in the simplicity of its crystal structure and phase diagram. However, our understanding of this canonical compound suffers from conflict between mutually incompatible descriptions of the material's electronic structure, as derived from contradictory interpretations of the photoemission record. Here we explore the challenge of interpretation in such experiments. By combining comprehensive photon energy- and polarization-dependent angle-resolved photoemission spectroscopy (ARPES) measurements with numerical simulations, we establish the providence of several contradictions in the present understanding of this and related materials. We identify a confluence of surface-related issues which have precluded unambiguous identification of both the number and the dimensionality of the Fermi-surface sheets. Ultimately, we arrive at a scenario which supports indications of topologically nontrivial states while also being incompatible with superconductivity as a spin-fluctuation-driven Fermi-surface instability.

Electronic correlation is of fundamental importance to high temperature superconductivity. While the low energy electronic states in cuprates are dominantly affected by correlation effects across the phase diagram, observation of correlation-driven changes in fermiology amongst the iron-based superconductors remains rare. Here we present experimental evidence for a correlation-driven reconstruction of the Fermi surface tuned independently by two orthogonal axes of temperature and Se/Te ratio in the iron chalcogenide family FeTe_1−xSe_x. We demonstrate that this reconstruction is driven by the de-hybridization of a strongly renormalized d_xy orbital with the remaining itinerant iron 3d orbitals in the emergence of an orbital-selective Mott phase. Our observations are further supported by our theoretical calculations to be salient spectroscopic signatures of such a non-thermal evolution from a strongly correlated metallic phase into an orbital-selective Mott phase in d_xy as Se concentration is reduced.

The mechanism of the enhanced superconductivity in monolayer FeSe/SrTiO₃ has been enthusiastically studied and debated over the past decade. One specific observation has been taken to be of central importance: the replica bands in the photoemission spectrum. Although suggestive of electron-phonon interaction in the material, the essence of these spectroscopic features remains highly controversial. In this work, we conduct angle-resolved photoemission spectroscopy measurements on monolayer FeSe/SrTiO₃ using linearly polarized photons. This configuration enables unambiguous characterization of the valence electronic structure with a suppression of the spectral background. We consistently observe high-order replica bands derived from various Fe 3d bands, similar to those observed on bare SrTiO₃. The intensity of the replica bands is unexpectedly high and different between d_xy and d_yz bands. Our results provide new insights on the electronic structure of this high-temperature superconductor and the physical origin of the photoemission replica bands.