arXiv subjects

Friedrich Reinert

Publications and source records attributed to Friedrich Reinert.

32 records · Page 2Linked to original sources

arXiv2020

Ubiquitous impact of localised impurity states on the exchange coupling mechanism in magnetic topological insulators

Since the discovery of the quantum anomalous Hall effect in the magnetically doped topological insulators (MTI) Cr:(Bi,Sb)$_2$Te$_3$ and V:(Bi,Sb)$_2$Te$_3$, the search for the exchange coupling mechanisms underlying the onset of ferromagnetism has been a central issue, and a variety of different scenarios have been put forward. By combining resonant photoemission, X-ray magnetic dichroism and multiplet ligand field theory, we determine the local electronic and magnetic configurations of V and Cr impurities in (Bi,Sb)$_2$Te$_3$. While strong pd hybridisation is found for both dopant types, their 3d densities of states show pronounced differences. State-of-the-art first-principles calculations show how these impurity states mediate characteristic short-range pd exchange interactions, whose strength sensitively varies with the position of the 3d states relative to the Fermi level. Measurements on films with varying host stoichiometry support this trend. Our results establish the essential role of impurity-state mediated exchange interactions in the magnetism of MTI.

cond-mat.str-el↗

arXiv2019

Topological electronic structure and intrinsic magnetization in MnBi$_4$Te$_7$: a Bi$_2$Te$_3$-derivative with a periodic Mn sublattice

Combinations of non-trivial band topology and long-range magnetic order hold promise for realizations of novel spintronic phenomena, such as the quantum anomalous Hall effect and the topological magnetoelectric effect. Following theoretical advances material candidates are emerging. Yet, a compound with a band-inverted electronic structure and an intrinsic net magnetization remains unrealized. MnBi$_2$Te$_4$ is a candidate for the first antiferromagnetic topological insulator and the progenitor of a modular (Bi$_2$Te$_3$)$_n$(MnBi$_2$Te$_4$) series. For $n$ = 1, we confirm a non-stoichiometric composition proximate to MnBi$_4$Te$_7$ and establish an antiferromagnetic state below 13 K followed by a state with net magnetization and ferromagnetic-like hysteresis below 5 K. Angle-resolved photoemission experiments and density-functional calculations reveal a topological surface state on the MnBi$_4$Te$_7$(0001) surface, analogous to the non-magnetic parent compound Bi$_2$Te$_3$. Our results render MnBi$_4$Te$_7$ as a band-inverted material with an intrinsic net magnetization and a complex magnetic phase diagram providing a versatile platform for the realization of different topological phases.

cond-mat.mtrl-sci↗

arXiv2019

Orbital-driven Rashba effect in a binary honeycomb monolayer AgTe

The Rashba effect is fundamental to the physics of two-dimensional electron systems and underlies a variety of spintronic phenomena. It has been proposed that the formation of Rashba-type spin splittings originates microscopically from the existence of orbital angular momentum (OAM) in the Bloch wave functions. Here, we present detailed experimental evidence for this OAM-based origin of the Rashba effect by angle-resolved photoemission (ARPES) and two-photon photoemission (2PPE) experiments for a monolayer AgTe on Ag(111). Using quantitative low-energy electron diffraction (LEED) analysis we determine the structural parameters and the stacking of the honeycomb overlayer with picometer precision. Based on an orbital-symmetry analysis in ARPES and supported by first-principles calculations, we unequivocally relate the presence and absence of Rashba-type spin splittings in different bands of AgTe to the existence of OAM.

cond-mat.mtrl-sci↗

arXiv2018

Chemical Aspects of the Antiferromagnetic Topological Insulator MnBi$_{2}$Te$_{4}$

Crystal growth of MnBi$_{2}$Te$_{4}$ has delivered the first experimental corroboration of the 3D antiferromagnetic topological insulator state. Our present results confirm that the synthesis of MnBi$_{2}$Te$_{4}$ can be scaled-up and strengthen it as a promising experimental platform for studies of a crossover between magnetic ordering and non-trivial topology. High-quality single crystals of MnBi$_{2}$Te$_{4}$ are grown by slow cooling within a narrow range between the melting points of Bi$_{2}$Te$_{3}$ (586 °C) and MnBi$_{2}$Te$_{4}$ (600 °C). Single crystal X-ray diffraction and electron microscopy reveal ubiquitous antisite defects in both cation sites and, possibly, Mn vacancies. Powders of MnBi$_{2}$Te$_{4}$ can be obtained at subsolidus temperatures, and a complementary thermochemical study establishes a limited high-temperature range of phase stability. Nevertheless, quenched powders are stable at room temperature and exhibit long-range antiferromagnetic ordering below 24 K. The expected Mn(II) out-of-plane magnetic state is confirmed by the magnetization, X-ray photoemission, X-ray absorption and linear dichroism data. MnBi$_{2}$Te$_{4}$ exhibits a metallic type of resistivity in the range 4.5-300 K. The compound is an n-type conductor that reaches a thermoelectric figure of merit up to ZT = 0.17. Angle-resolved photoemission experiments provide evidence for a surface state forming a gapped Dirac cone.

cond-mat.mtrl-sci↗

arXiv2017

Strong Linear Dichroism in Spin-Polarized Photoemission from Spin-Orbit-Coupled Surface States

A comprehensive understanding of spin-polarized photoemission is crucial for accessing the electronic structure of spin-orbit coupled materials. Yet, the impact of the final state in the photoemission process on the photoelectron spin has been difficult to assess in these systems. We present experiments for the spin-orbit split states in a Bi-Ag surface alloy showing that the alteration of the final state with energy may cause a complete reversal of the photoelectron spin polarization. We explain the effect on the basis of ab initio one-step photoemission theory and describe how it originates from linear dichroism in the angular distribution of photoelectrons. Our analysis shows that the modulated photoelectron spin polarization reflects the intrinsic spin density of the surface state being sampled differently depending on the final state, and it indicates linear dichroism as a natural probe of spin-orbit coupling at surfaces.

cond-mat.str-el↗

arXiv2017

Irreversible proliferation of magnetic moments at cleaved surfaces of the topological Kondo insulator SmB6

The compound SmB$_6$ is the best established realization of a topological Kondo insulator, in which a topological insulator state is obtained through Kondo coherence. Recent studies have found evidence that the surface of SmB$_6$ hosts ferromagnetic domains, creating an intrinsic platform for unidirectional ballistic transport at the domain boundaries. Here, surface-sensitive X-ray absorption (XAS) and bulk-sensitive resonant inelastic X-ray scattering (RIXS) spectra are measured at the Sm N$_{4,5}$-edge, and used to evaluate electronic symmetries, excitations and temperature dependence near the surface of cleaved samples. The XAS data show that the density of large-moment atomic multiplet states on a cleaved surface grows irreversibly over time, to a degree that likely exceeds a related change that has recently been observed in the surface 4f orbital occupation.

cond-mat.str-el↗

arXiv2016

Impurity states in the magnetic topological insulator V:(Bi,Sb)$_2$Te$_3$

The ferromagnetic topological insulator V:(Bi,Sb)$_2$Te$_3$ has been recently reported as a quantum anomalous Hall (QAH) system. Yet the microscopic origins of the QAH effect and the ferromagnetism remain unclear. One key aspect is the contribution of the V atoms to the electronic structure. Here the valence band of V:(Bi,Sb)$_2$Te$_3$ thin films was probed in an element-specific way by resonant photoemission spectroscopy. The signature of the V $3d$ impurity band was extracted, and exhibits a high density of states near Fermi level. First-principles calculations support the experimental results and indicate the coexistence of ferromagnetic superexchange and double exchange interactions. The observed impurity band is thus expected to contribute to the ferromagnetism via the interplay of different mechanisms.

cond-mat.str-el↗

arXiv2015

Termination-dependent surface properties in the giant-Rashba semiconductors BiTeX (X = Cl, Br, I)

The non-centrosymmetric semiconductors BiTeX (X = Cl, Br, I) show large Rashba-type spin-orbit splittings in their electronic structure making them candidate materials for spin-based electronics. However, BiTeI(0001) single crystal surfaces usually consist of stacking-fault-induced domains of Te and I terminations implying a spatially inhomogeneous electronic structure. Here we combine scanning tunneling microscopy (STM), photoelectron spectroscopy (ARPES, XPS) and density functional theory (DFT) calculations to systematically investigate the structural and electronic properties of BiTeX(0001) surfaces. For X = Cl, Br we observe macroscopic single-terminated surfaces. We discuss chemical characteristics among the three materials in terms of bonding character, surface electronic structure, and surface morphology.

cond-mat.mtrl-sci↗

arXiv2014

Interface originated modification of electron-vibration coupling in resonant photoelectron spectroscopy

We present a comprehensive study of the photon energy ($h ν$) dependent line-shape evolution of molecular orbital signals of large $π$-conjugated molecules by resonant photoelectron spectroscopy (RPES). A comparison to RPES data of small molecules suggests that the excitation into different vibrational levels on the intermediate state potential energy surface of the electronic excitation is responsible for the observed effect. In this simplified picture of electron-vibration couping the character of the potential energy surfaces involved in the RPES process determines the line-shape of the molecular orbital signal for a particular $h ν$. We use the sensitivity of this effect to probe the influence of different interfaces on the electron-vibration coupling in the investigated systems. The magnitude of the variation in line-shape throughout the particular $h ν$ region allows to reveal significant differences within the physisorptive regime.

cond-mat.mtrl-sci↗

arXiv2013

Observation of a molecule-metal interface charge transfer state by resonant photoelectron spectroscopy

We report the discovery of a novel charge transfer (CT) state at a molecule-metal interface by the application of resonant photoelectron spectroscopy (ResPES). This interface feature is neither present for molecular bulk samples nor for the clean substrate. Within a simplified two-step model this signal is assigned to a particular final state that is invisible in direct photoelectron spectroscopy but in ResPES revealed through relative resonant enhancement. A detailed analysis of the spectroscopic signature of the CT state shows characteristics of electronic interaction not found in other electron spectroscopic techniques. Our study demonstrates the sensitivity of ResPES to such interactions and constitutes a new way to investigate CT at molecule-metal interfaces.

cond-mat.mtrl-sci↗

arXiv2012

Single Dirac-cone on the Cs-covered topological insulator surface Sb2Te3(0001)

Using angle-resolved photoelectron spectroscopy we investigate the surface electronic structure of the three-dimensional topological insulator (TI) Sb2Te3(0001). Our data show the presence of a topological surface state in the bulk energy gap with the Dirac-point located above the Fermi level. The adsorption of Cs-atoms on Sb2Te3(0001) gives rise to a downward energy shift of the electronic valence band states which saturates at a value of ~200 meV. For the saturation coverage the Dirac-point of the linearly dispersive surface state resides in close proximity to the Fermi level. The electronic structure of the Cs/Sb2Te3 interface therefore considerably deviates from previously studied metal-TI interfaces based on the isostructural compound Bi2Se3 which points to the importance of atomic composition in these hetero systems.

cond-mat.mes-hall↗

arXiv2012

Direct Observation of Interband Spin-Orbit Coupling in a Two-Dimensional Electron System

We report the direct observation of interband spin-orbit (SO) coupling in a two-dimensional (2D) surface electron system, in addition to the anticipated Rashba spin splitting. Using angle-resolved photoemission experiments and first-principles calculations on Bi/Ag/Au heterostructures we show that the effect strongly modifies the dispersion as well as the orbital and spin character of the 2D electronic states, thus giving rise to considerable deviations from the Rashba model. The strength of the interband SO coupling is tuned by the thickness of the thin film structures.

cond-mat.mes-hall↗

arXiv2012

Interplay of electronic structure and atomic ordering on surfaces: Momentum-resolved measurements of Cs atoms adsorbed on a Ag(111) substrate

Surface-state mediated interactions between adsorbates on surfaces can be exploited for the fabrication of self-organized nanostructures such as two-dimensional superlattices of adatoms. Using angle-resolved photoemission we provide experimental evidence that these interactions can be drastically modified by adsorbate-induced alterations in the surface potential barrier. This, in turn, will cause significant changes in the ordering of the adsorbates. For the studied case example of Cs adatoms on Ag(111) our momentum-resolved measurements reveal the surface state Fermi wave vector to be increased by as much as $\sim$100% for coverages around 0.03 ML. Our results unravel the origin for the hitherto puzzling and unexpectedly small lattice constant in the adatom superlattice observed for this system.

cond-mat.mtrl-sci↗

arXiv2010

Energetics of Excited States in the Conjugated Polymer Poly(3-hexylthiophene)

There is an enormous potential in applying conjugated polymers in novel organic opto-electronic devices such as light emitting diodes and solar cells. Although prototypes and first products exist, a comprehensive understanding of the fundamental processes and energetics involved during photoexcitation is still lacking and limits further device optimisations. Here we report on a unique analysis of the excited states involved in charge generation by photoexcitation. On the model system poly(3-hexylthiophene) (P3HT), we demonstrate the general applicability of our novel approach. From photoemission spectroscopy of occupied and unoccupied states we determine the transport gap to 2.6 eV, which we show to be in agreement with the onset of photoconductivity by spectrally resolved photocurrent measurements. For photogenerated singlet exciton at the absorption edge, 0.7 eV of excess energy are required to overcome the binding energy; the intermediate charge transfer state is situated only 0.3 eV above the singlet exciton. Our results give direct evidence of energy levels involved in the photogeneration and charge transport within conjugated polymers.

cond-mat.mtrl-sci↗