Raman and fluorescence contributions to resonant inelastic soft x-ray scattering on LaAlO3_3/SrTiO3_3 heterostructures

We present a detailed study of the Ti 3$d$ carriers at the interface of LaAlO$_3$/SrTiO$_3$ heterostructures by high-resolution resonant inelastic soft x-ray scattering (RIXS), with special focus on the roles of overlayer thickness and oxygen vacancies. Our measurements show the existence of interfacial Ti 3$d$ electrons already below the critical thickness for conductivity and an increase of the total interface charge up to a LaAlO$_3$ overlayer thickness of 6 unit cells before it levels out. By comparing stoichiometric and oxygen deficient samples we observe strong Ti 3$d$ charge carrier doping by oxygen vacancies. The RIXS data combined with photoelectron spectroscopy and transport measurements indicate the simultaneous presence of localized and itinerant charge carriers. However, it is demonstrated that the relative amount of localized and itinerant Ti $3d$ electrons in the ground state cannot be deduced from the relative intensities of the Raman and fluorescence peaks in excitation energy dependent RIXS measurements, in contrast to previous interpretations. Rather, we attribute the observation of either the Raman or the fluorescence signal to the spatial extension of the intermediate state reached in the RIXS excitation process.Comment: 9 pages, 6 figure

High-energy photoemission on Fe3O4: Small polaron physics and the Verwey transition

We have studied the electronic structure and charge ordering (Verwey) transition of magnetite (Fe3O4) by soft x-ray photoemission. Due to the enhanced probing depth and the use of different surface preparations we are able to distinguish surface and volume effects in the spectra. The pseudogap behavior of the intrinsic spectra and its temperature dependence give evidence for the existence of strongly bound small polarons consistent with both dc and optical conductivity. Together with other recent structural and theoretical results our findings support a picture in which the Verwey transition contains elements of a cooperative Jahn-Teller effect, stabilized by local Coulomb interaction

ARPES Line Shapes in FL and non-FL Quasi-Low-Dimensional Inorganic Metals

Quasi-low-dimensional (quasi-low-D) inorganic materials are not only ideally suited for angle resolved photoemission spectroscopy (ARPES) but also they offer a rich ground for studying key concepts for the emerging paradigm of non-Fermi liquid (non-FL) physics. In this article, we discuss the ARPES technique applied to three quasi-low-D inorganic metals: a paradigm Fermi liquid (FL) material TiTe$_{2}$, a well-known quasi-1D charge density wave (CDW) material K$_{0.3}$MoO$_{3}$ and a quasi-1D non-CDW material Li$_{0.9}$Mo$_{6}$O$_{17}$. With TiTe$_2$, we establish that a many body theoretical interpretation of the ARPES line shape is possible. We also address the fundamental question of how to accurately determine the {\bf k}$_F$ value from ARPES. Both K$_{0.3}$MoO$_{3}$ and Li$_{0.9}$Mo$_{6}$O$_{17}$ show quasi-1D electronic structures with non-FL line shapes. A CDW gap opening is observed for K$_{0.3}$MoO$_{3}$, whereas no gap is observed for Li$_{0.9}$Mo$_{6}$O$_{17}$. We show, however, that the standard CDW theory, even with strong fluctuations, is not sufficient to describe the non-FL line shapes of K$_{0.3}$MoO$_{3}$. We argue that a Luttinger liquid (LL) model is relevant for both bronzes, but also point out difficulties encountered in comparing data with theory. We interpret this situation to mean that a more complete and realistic theory is necessary to understand these data.Comment: 23 pages, including 21 figures; to appear in a special issue of J. Elec. Spectr. Rel. Pheno

Electronic structure of the quasi-one-dimensional organic conductor TTF-TCNQ

We study the electronic structure of the quasi-one-dimensional organic conductor TTF-TCNQ by means of density-functional band theory, Hubbard model calculations, and angle-resolved photoelectron spectroscopy (ARPES). The experimental spectra reveal significant quantitative and qualitative discrepancies to band theory. We demonstrate that the dispersive behavior as well as the temperature-dependence of the spectra can be consistently explained by the finite-energy physics of the one-dimensional Hubbard model at metallic doping. The model description can even be made quantitative, if one accounts for an enhanced hopping integral at the surface, most likely caused by a relaxation of the topmost molecular layer. Within this interpretation the ARPES data provide spectroscopic evidence for the existence of spin-charge separation on an energy scale of the conduction band width. The failure of the one-dimensional Hubbard model for the {\it low-energy} spectral behavior is attributed to interchain coupling and the additional effect of electron-phonon interaction.Comment: 18 pages, 9 figure

Non-fermi-liquid single particle lineshape of the quasi-one-dimensional non-CDW metal Li_{0.9}Mo_{6}O_{17} : comparison to the Luttinger liquid

We report the detailed non-Fermi liquid (NFL) lineshape of the dispersing excitation which defines the Fermi surface (FS) for quasi-one-dimensional Li_{0.9}Mo_{6}O_{17}. The properties of Li_{0.9}Mo_{6}O_{17} strongly suggest that the NFL behavior has a purely electronic origin. Relative to the theoretical Luttinger liquid lineshape, we identify significant similarities, but also important differences.Comment: 5 pages, 3 eps figure

Microscopic origin of the mobility enhancement at a spinel/perovskite oxide heterointerface revealed by photoemission spectroscopy

The spinel/perovskite heterointerface $\gamma$-Al$_2$O$_3$/SrTiO$_3$ hosts a two-dimensional electron system (2DES) with electron mobilities exceeding those in its all-perovskite counterpart LaAlO$_3$/SrTiO$_3$ by more than an order of magnitude despite the abundance of oxygen vacancies which act as electron donors as well as scattering sites. By means of resonant soft x-ray photoemission spectroscopy and \textit{ab initio} calculations we reveal the presence of a sharply localized type of oxygen vacancies at the very interface due to the local breaking of the perovskite symmetry. We explain the extraordinarily high mobilities by reduced scattering resulting from the preferential formation of interfacial oxygen vacancies and spatial separation of the resulting 2DES in deeper SrTiO$_3$ layers. Our findings comply with transport studies and pave the way towards defect engineering at interfaces of oxides with different crystal structures.Comment: Accepted as Rapid Communications in Physical Review

Surface characterization and surface electronic structure of organic quasi-one-dimensional charge transfer salts

We have thoroughly characterized the surfaces of the organic charge-transfer salts TTF-TCNQ and (TMTSF)2PF6 which are generally acknowledged as prototypical examples of one-dimensional conductors. In particular x-ray induced photoemission spectroscopy turns out to be a valuable non-destructive diagnostic tool. We show that the observation of generic one-dimensional signatures in photoemission spectra of the valence band close to the Fermi level can be strongly affected by surface effects. Especially, great care must be exercised taking evidence for an unusual one-dimensional many-body state exclusively from the observation of a pseudogap.Comment: 11 pages, 12 figures, v2: minor changes in text and figure labellin

Remnant Fermi surface in the presence of an underlying instability in layered 1T-TaS_2

We report high resolution angle-scanned photoemission and Fermi surface (FS) mapping experiments on the layered transition-metal dichalcogenide 1T-TaS_2 in the quasi commensurate (QC) and the commensurate (C) charge-density-wave (CDW) phase. Instead of a nesting induced partially removed FS in the CDW phase we find a pseudogap over large portions of the FS. This remnant FS exhibits the symmetry of the one-particle normal state FS even when passing from the QC-phase to the C-phase. Possibly, this Mott localization induced transition represents the underlying instability responsible for the pseudogapped FS