Showing papers by "Julien E. Rault published in 2020"

Electron-polaron dichotomy of charge carriers in perovskite oxides

Abstract: Many transition metal oxides (TMOs) are Mott insulators due to strong Coulomb repulsion between electrons, and exhibit metal-insulator transitions (MITs) whose mechanisms are not always fully understood. Unlike most TMOs, minute doping in CaMnO3 induces a metallic state without any structural transformations. This material is thus an ideal platform to explore band formation through the MIT. Here, we use angle-resolved photoemission spectroscopy to visualize how electrons delocalize and couple to phonons in CaMnO3. We show the development of a Fermi surface where mobile electrons coexist with heavier carriers, strongly coupled polarons. The latter originate from a boost of the electron-phonon interaction (EPI). This finding brings to light the role that the EPI can play in MITs even caused by purely electronic mechanisms. Our discovery of the EPI-induced dichotomy of the charge carriers explains the transport response of Ce-doped CaMnO3 and suggests strategies to engineer quantum matter from TMOs. The underlying mechanisms of the metal-insulator transition in correlated oxides are a rich source of interesting physics and a topic of long-standing investigation. Here, the authors use angle-resolved photoelectron spectroscopy to investigate changes in charge carrier properties and electron-phonon interactions as a function of Ce-doping across the metal-insulator transition in CaMnO3.

Tunable two-dimensional electron system at the (110) surface of SnO 2

Abstract: We report the observation of a two-dimensional electron system (2DES) at the (110) surface of the transparent bulk insulator ${\mathrm{SnO}}_{2}$ and the tunability of its carrier density by means of temperature or Eu deposition. The 2DES is insensitive to surface reconstructions and, surprisingly, it survives even after exposure to ambient conditions---an extraordinary fact recalling the well known catalytic properties ${\mathrm{SnO}}_{2}$. Our data show that surface oxygen vacancies are at the origin of such 2DES, providing key information about the long-debated origin of $n$-type conductivity in ${\mathrm{SnO}}_{2}$, at the basis of a wide range of applications. Furthermore, our study shows that the emergence of a 2DES in a given oxide depends on a delicate interplay between its crystal structure and the orbital character of its conduction band.

Dispersing and semi-flat bands in the wide band gap two-dimensional semiconductor bilayer silicon oxide

Abstract: Epitaxial bilayer silicon oxide is a transferable two-dimensional material predicted to be a wide band gap semiconductor, with potential applications for deep UV optoelectronics, or as a building block of van der Waals heterostructures. The prerequisite to any sort of such applications is the knowledge of the electronic band structure, which we unveil using angle-resolved photoemission spectroscopy and rationalise with the help of density functional theory calculations. We discover dispersing bands related to electronic delocalisation within the top and bottom planes of the material, and semi-flat bands stemming from the chemical bridges between the two planes. This band structure is robust against exposure to air, and can be controled by exposure to oxygen. We provide an experimental lower-estimate of the band gap size of 5 eV and predict a full gap of 7.36 eV using density functional theory calculations.

Photoemission study on pristine and Ni-doped SrTiO$_{3}$ thin films

Abstract: We combined photoelemission spectroscopy with first-principle calculations to investigate structural and electronic properties of SrTiO$_{3}$ doped with Ni impurities. In SrTiO$_{3}$ polycrystalline thin films, grown by magnetron sputtering, the mean size of the crystallites increases with the concentration of Ni. To determine the electronic band structure of SrTiO$_{3}$ films doped with Ni, high quality ordered pristine and SrTiO3:Ni$_{x}$ films with x=0.06 and 0.12 were prepared by pulsed laser deposition. Electronic band structure calculations for the ground state, as well as one-step model photoemission calculations, which were obtained by means of the Korringa-Khon-Rostoker Greens's function method, predicted the formation of localised $3d$-impurity bands in the band gap of SrTiO$_{3}$ close to the valence band maxima. The measured valence bands at the resonance Ni2p excitation and band dispersion confirm these findings.

Electron-polaron dichotomy of charge carriers in perovskite oxides

Abstract: Many transition metal oxides (TMOs) are Mott insulators due to strong Coulomb repulsion between electrons, and exhibit metal-insulator transitions (MITs) whose mechanisms are not always fully understood. Unlike most TMOs, minute doping in CaMnO3 induces a metallic state without any structural transformations. This material is thus an ideal platform to explore band formation through the MIT. Here, we use angle-resolved photoemission spectroscopy to visualize how electrons delocalize and couple to phonons in CaMnO3. We show the development of a Fermi surface where mobile electrons coexist with heavier carriers, strongly coupled polarons. The latter originate from a boost of the electron-phonon interaction (EPI). This finding brings to light the role that the EPI can play in MITs even caused by purely electronic mechanisms. Our discovery of the EPI-induced dichotomy of the charge carriers explains the transport response of Ce-doped CaMnO3 and suggests strategies to engineer quantum matter from TMOs.