arXiv subjects

Claus M. Schneider

Publications and source records attributed to Claus M. Schneider.

At least 19 recordsLinked to original sources

arXiv2024

Ultrafast demagnetization in ferromagnetic materials: Origins and progress

Since the discovery of ultrafast demagnetization in Ni thin films in 1996, laser-induced ultrafast spin dynamics have become a prominent research topic in the field of magnetism and spintronics. This development offers new possibilities for the advancement of spintronics and magnetic storage technology. The subject has drawn a substantial number of researchers, leading to a series of research endeavors. Various models have been proposed to elucidate the physical processes underlying laser-induced ultrafast spin dynamics in ferromagnetic materials. However, the potential origins of these processes across different material systems and the true contributions of these different origins remain challenging in the realm of ultrafast spin dynamics. This predicament also hinders the development of spintronic terahertz emitters. In this review, we initially introduce the different experimental methods used in laser-induced ultrafast spin dynamics. We then systematically explore the magnetization precession process and present seven models of ultrafast demagnetization in ferromagnetic materials. Subsequently, we discuss the physical processes and research status of four ultrafast demagnetization origins (including spin-flipping, spin transport, non-thermal electronic distribution, and laser-induced lattice strain). Since attosecond laser technique and antiferromagnetic materials exhibit promising applications in ultrahigh-frequency spintronics, we acknowledge the emerging studies used by attosecond pules and studies on ultrafast spin dynamics in antiferromagnets, noting the significant challenges that need to be addressed in these burgeoning field.

cond-mat.mtrl-sci↗

arXiv2024

Scattering makes a difference in circular dichroic angle-resolved photoemission

Recent years have witnessed a steady progress towards blending 2D quantum materials into technology, with future applications often rooted in the electronic structure. Since crossings and inversions of electronic bands with different orbital characters determine intrinsic quantum transport properties, knowledge of the orbital character is essential. Here, we benchmark angle-resolved photoelectron emission spectroscopy (ARPES) as a tool to experimentally derive orbital characters. For this purpose we study the valence electronic structure of two technologically relevant quantum materials, graphene and WSe$_2$, and focus on circular dichroism that is believed to provide sensitivity to the orbital angular momentum. We analyze the contributions related to angular atomic photoionization profiles, interatomic interference, and multiple scattering. Regimes in which initial-state properties could be disentangled from the ARPES maps are critically discussed and the potential of using circular-dichroic ARPES as a tool to investigate the spin polarization of initial bands is explored. For the purpose of generalization, results from two additional materials, GdMn$_6$Sn$_6$ and PtTe$_2$ are presented in addition. This research demonstrates rich complexity of the underlying physics of circular-dichroic ARPES, providing new insights that will shape the interpretation of both past and future circular-dichroic ARPES studies.

cond-mat.mtrl-sci↗

arXiv2023

Enantioselective adsorption on magnetic surfaces

From the beginning of molecular theory, the interplay of chirality and magnetism has intrigued scientists. There is still the question if enantiospecific adsorption of chiral molecules occurs on magnetic surfaces. Enantiomer discrimination was conjectured to arise from chirality-induced spin separation within the molecules and exchange interaction with the substrate's magnetization. Here we show that single helical aromatic hydrocarbons undergo enantioselective adsorption on ferromagnetic cobalt surfaces. Spin and chirality sensitive scanning tunneling microscopy reveals that molecules of opposite handedness prefer adsorption onto cobalt islands with opposite out-of-plane magnetization. As mobility ceases in the final chemisorbed state, it is concluded that enantioselection must occur in a physisorbed transient precursor state. State-of-the-art spin-resolved ab initio simulations support this scenario by refuting enantio-dependent chemisorption energies. These findings demonstrate that van der Waals interaction should also include spin-fluctuations which are crucial for molecular magnetochiral processes.

cond-mat.mtrl-sci↗

arXiv2023

Noise-dependent bias in quantitative STEM-EMCD experiments revealed by bootstrapping

Electron magnetic circular dichroism (EMCD) is a powerful technique for estimating element-specific magnetic moments of materials on nanoscale with the potential to reach atomic resolution in transmission electron microscopes. However, the fundamentally weak EMCD signal strength complicates quantification of magnetic moments, as this requires very high precision, especially in the denominator of the sum rules. Here, we employ a statistical resampling technique known as bootstrapping to an experimental EMCD dataset to produce an empirical estimate of the noise dependent error distribution resulting from application of EMCD sum rules to bcc iron in a 3 beam orientation. We observe clear experimental evidence that noisy EMCD signals preferentially bias the estimation of magnetic moments, further supporting this with error distributions produced by Monte-Carlo simulations. Finally, we propose guidelines for the recognition and minimization of this bias in the estimation of magnetic moments.

cond-mat.mtrl-sci↗

arXiv2023

Spin-Selective Electron Transport Through Single Chiral Molecules

The interplay between chirality and magnetism has been a source of fascination among scientists for over a century. In recent years, chirality-induced spin selectivity (CISS) has attracted renewed interest. It has been observed that electron transport through layers of homochiral molecules leads to a significant spin polarization of several tens of percent. Despite the abundant experimental evidence gathered through mesoscopic transport measurements, the exact mechanism behind CISS remains elusive. In this study, we report spin-selective electron transport through single helical aromatic hydrocarbons that were sublimed in vacuo onto ferromagnetic cobalt surfaces and examined with spin-polarized scanning tunneling microscopy (SP-STM) at a temperature of 5 K. Direct comparison of two enantiomers under otherwise identical conditions revealed magnetochiral conductance asymmetries of up to 50% when either the molecular handedness was exchanged or the magnetization direction of the STM tip or Co substrate was reversed. Importantly, our results rule out electron-phonon coupling and ensemble effects as primary mechanisms responsible for CISS.

cond-mat.mes-hall↗

arXiv2023

Independent and coherent transitions between antiferromagnetic states of few-molecule systems

Spin-electronic devices are poised to become part of mainstream microelectronic technology .Downsizing them, however, faces the intrinsic difficulty that as ferromagnets become smaller, it becomes more difficult to stabilize their magnetic moment. Antiferromagnets are much more stable, and thus research on antiferromagnetic spintronics has developed into a fast-growing field. Here, we provide proof of concept data that allows us to expand the area of antiferromagnetic spintronics to the hitherto elusive level of individual molecules. In contrast to all previous work on molecular spintronics, our detection scheme of the molecule's spin state does not rely on a magnetic moment. Instead, we use field-effect transistor devices constituting of an isolated, contacted single-wall carbon nanotube covalently bound to a limited number of molecular antiferromagnets incorporating four Mn(II) or Co(II) ions. Time-dependent quantum transport measurement along the functionalized nanotube show step-like transitions between several distinct current levels, which we attribute to transitions between different antiferromagnetic states of individual molecular complexes grafted on the nanotube. A statistical analysis of the switching events using factorial cumulants indicates that the cobalt complexes switch independently from each other, while a coherent superposition of the antiferromagnetic spin states of the molecules along the nanotube is observed for the manganese complexes. The long coherence time (several seconds at 100 mK) is made possible by the absence of spin and orbital momentum in the relevant states of the manganese complex, while the cobalt complex includes a significant orbital momentum contribution due to the pseudo-octahedral d$^7$ metal centers.

cond-mat.mes-hall↗

arXiv2023

Twist angle dependent interlayer transfer of valley polarization from excitons to free charge carriers in WSe$_2$/MoSe$_2$ heterobilayers

We identify an optical excitation mechanism that transfers a valley polarization from photo-excited electron-hole pairs to free charge carriers in twisted WSe$_2$/MoSe$_2$ heterobilayers. For small twist angles, the valley lifetimes of the charge carriers are surprisingly short, despite the occurrence of interlayer excitons with their presumably long recombination and polarization lifetimes. For large twist angles, we measure an increase in both the valley polarization and its respective lifetime by more than two orders of magnitude. Interestingly, in such heterobilayers we observe an interlayer transfer of valley polarization from the WSe$_2$ layer into the MoSe$_2$ layer. This mechanism enables the creation of a photo-induced valley polarization of free charge carriers in MoSe$_2$, which amplitude scales with the gate-induced charge carrier density. This is in contrast to monolayer MoSe$_2$, where such a gate-tunable valley polarization cannot be achieved. By combining time-resolved Kerr rotation, photoluminesence and angle-resolved photoemission spectroscopy measurements with first principles calculations, we show that these findings can be explained by twist angle dependent interlayer scattering mechanisms involving the Q- and $Γ$-valleys.

cond-mat.mtrl-sci↗

arXiv2022

Geometry-induced spin-filtering in photoemission maps from WTe$_2$ surface states

We demonstrate that an important quantum material WTe$_2$ exhibits a new type of geometry-induced spin-filtering effect in photoemission, stemming from low symmetry that is responsible for its exotic transport properties. Through the laser-driven spin-polarized angle-resolved photoemission Fermi surface mapping, we showcase highly asymmetric spin textures of electrons photoemitted from the surface states of WTe$_2$. Such asymmetries are not present in the initial state spin textures, which are bound by the time-reversal and crystal lattice mirror plane symmetries. The findings are reproduced qualitatively by theoretical modeling within the one-step model photoemission formalism. The effect could be understood within the free-electron final state model as an interference due to emission from different atomic sites. The observed effect is a manifestation of time-reversal symmetry breaking of the initial state in the photoemission process, and as such it cannot be eliminated, but only its magnitude influenced, by special experimental geometries.

cond-mat.mtrl-sci↗

arXiv2022

Temperature-dependent spin-resolved electronic structure of EuO thin films

The electronic structure of the ferromagnetic semiconductor EuO is investigated by means of spin- and angle-resolved photoemission spectroscopy (spin-ARPES) and density functional theory. EuO exhibits unique properties of hosting both weakly-dispersive nearly fully polarized Eu $4f$ bands, as well as O $2p$ levels indirectly exchange-split by the interaction with Eu nearest neighbors. Our temperature-dependent spin-ARPES data directly demonstrates the exchange splitting in O $2p$ and its vanishing at the Curie temperature. Our calculations with a Hubbard $U$ term reveal a complex nature of the local exchange splitting on the oxygen site and in conduction bands. We discuss the mechanisms of the indirect exchange in the O 2p levels by analyzing orbital-resolved band characters in ferromagnetic and antiferromagnetic phases. The directional effects due to spin-orbit coupling are predicted theoretically to be significant in particular in the Eu 4f band manifold. The analysis of the shape of spin-resolved spectra in the Eu $4f$ spectral region reveals signatures of hybridization with O $2p$, in agreement with the theoretical predictions. We also analyze spectral changes in the spin-integrated spectra throughout the Curie temperature and demonstrate they derive from both the magnetic phase transition and effects due to sample aging, unavoidable for this highly reactive material.

cond-mat.mtrl-sci↗

arXiv2021

Orbital contributions in the element-resolved valence electronic structure of Bi2Se3

In this work, we studied the bulk band structure of a topological insulator (TI) Bi2Se3 and determined the contributions of the Bi and Se orbital states to the valence bands using standing wave-excited hard x-ray photoemission spectroscopy (SW-HAXPES). This SW technique can provide the element-resolved information and extract individual Bi and Se contributions to the Bi2Se3 valence band. Comparisons with density functional theory (DFT) calculations (LDA and GW) reveal that the Bi 6s, Bi 6p, and Se 4p states are dominant in the Bi2Se3 HAXPES valence band. These findings pave a way for studying the element-resolved band structure and orbital contributions of this class of TIs.

cond-mat.mtrl-sci↗

arXiv2021

Near total reflection X-ray photoelectron spectroscopy: Quantifying chemistry at solid/liquid and solid/solid interfaces

Near total reflection regime has been widely used in X-ray science, specifically in grazing incidence small angle X-ray scattering and in hard X-ray photoelectron spectroscopy. In this work, we introduce some practical aspects of using near total reflection in ambient pressure X-ray photoelectron spectroscopy and apply this technique to study chemical concentration gradients in a substrate/photoresist system. Experimental data are accompanied by X-ray optical and photoemission simulations to quantitatively probe the photoresist and the interface with the depth accuracy of ~1 nm. Together, our calculations and experiments confirm that near total reflection X-ray photoelectron spectroscopy is a suitable method to extract information from buried interfaces with highest depth-resolution, which can help address open research questions regarding our understanding of concentration profiles, electrical gradients, and charge transfer phenomena at such interfaces. The presented methodology is especially attractive for solid/liquid interface studies, since it provides all the strengths of a Bragg-reflection standing-wave spectroscopy without the need of an artificial multilayer mirror serving as a standing wave generator, thus dramatically simplifying the sample synthesis.

physics.app-ph↗

arXiv2021

Spanning Fermi arcs in a two-dimensional magnet

The discovery of topological states of matter has led to a revolution in materials research. When external or intrinsic parameters break certain symmetries, global properties of topological materials change drastically. A paramount example is the emergence of Weyl nodes under broken inversion symmetry, acting like magnetic monopoles in momentum space. However, while a rich variety of non-trivial quantum phases could in principle also originate from broken time-reversal symmetry, realizing systems that combine magnetism with complex topological properties is remarkably elusive due to both considerable experimental and theoretical challenges. Here, we demonstrate that giant open Fermi arcs are created at the surface of ultrathin hybrid magnets. The Fermi-surface topology of an atomically thin ferromagnet is substantially modified by the hybridization with a heavy-metal substrate, giving rise to Fermi-surface discontinuities that are bridged by the Fermi arcs. Due to the interplay between magnetism and topology, we can control both the shape and the location of the Fermi arcs by tuning the magnetization direction. The hybridization points in the Fermi surface can be attributed to a non-trivial "mixed" topology and induce hot spots in the Berry curvature, dominating spin and charge transport as well as magneto-electric coupling effects.

cond-mat.mtrl-sci↗

arXiv2020

Two-dimensional electron systems in perovskite oxide heterostructures: Role of the polarity-induced substitutional defects

The discovery of a two-dimensional electron system (2DES) at the interfaces of perovskite oxides such as LaAlO3 and SrTiO3 has motivated enormous efforts in engineering interfacial functionalities with this type of oxide heterostructures. However, its fundamental origins are still not understood, e.g. the microscopic mechanisms of coexisting interface conductivity and magnetism. Here we report a comprehensive spectroscopic investigation of the depth profile of 2DES-relevant Ti 3d interface carriers using depth- and element-specific techniques, standing-wave excited photoemission and resonant inelastic scattering. We found that one type of Ti 3d interface carriers, which give rise to the 2DES are located within 3 unit cells from the n-type interface in the SrTiO3 layer. Unexpectedly, another type of interface carriers, which are polarity-induced Ti-on-Al antisite defects, reside in the first 3 unit cells of the opposing LaAlO3 layer (~10 Å). Our findings provide a microscopic picture of how the localized and mobile Ti 3d interface carriers distribute across the interface and suggest that the 2DES and 2D magnetism at the LaAlO3/SrTiO3 interface have disparate explanations as originating from different types of interface carriers.

cond-mat.mtrl-sci↗

arXiv2020

Evaluation of molecular orbital symmetry via oxygen-induced charge transfer quenching at a metal-organic interface

Thin molecular films under model conditions are often exploited as benchmarks and case studies to investigate the electronic and structural changes occurring on the surface of metallic electrodes. Here we show that the modification of a metallic surface induced by oxygen adsorption allows the preservation of the geometry of a molecular adlayer, giving access to the determination of molecular orbital symmetries by means of near-edge x-ray absorption fine structure spectroscopy, NEXAFS. As a prototypical example, we exploited Nickel Tetraphenyl Porphyrin molecules deposited on a bare and on an oxygen pre-covered Cu(100) surface. We find that adsorbed atomic oxygen quenches the charge transfer at the metal-organic interface but, in contrast to a thin film sample, maintains the ordered adsorption geometry of the organic molecules. In this way, it is possible to disentangle π* and σ* symmetry orbitals, hence estimating the relative oscillator strength of core level transitions directly from the experimental data, as well as to evaluate and localize the degree of charge transfer in a coupled system. In particular, we neatly single out the σ* contribution associated with the N 1s transition to the mixed N 2px,y-Ni 3dx2-y2 orbital, which falls close to the leading π*-symmetry LUMO resonance.

cond-mat.mtrl-sci↗

arXiv2019

Single-pass STEM-EMCD on a zone axis using a patterned aperture: progress in experimental and data treatment methods

Measuring magnetic moments in ferromagnetic materials with atomic column resolution is theoretically possible using the electron magnetic circular dichroism (EMCD) technique in a (scanning) transmission electron microscope ((S)TEM). However, experimental and data processing hurdles currently hamper the realization of this goal. Experimentally, the sample must be tilted to a zone-axis orientation, yielding a complex distribution of magnetic scattering intensity, and the same sample region must be scanned multiple times with sub-atomic spatial registration necessary at each pass. Furthermore, the weak nature of the EMCD signal requires advanced data processing techniques to reliably detect and quantify the result. In this manuscript, we detail our experimental and data processing progress towards achieving single-pass zone-axis EMCD using a patterned aperture. First, we provide a comprehensive data acquisition and analysis strategy for this and other EMCD experiments that should scale down to atomic resolution experiments. Second, we demonstrate that, at low spatial resolution, promising EMCD candidate signals can be extracted, and that these are sensitive to both crystallographic orientation and momentum transfer.

cond-mat.mtrl-sci↗

arXiv2018

Element- and momentum-resolved electronic structure of the dilute magnetic semiconductor manganese doped gallium arsenide

The dilute magnetic semiconductors have promise in spin-based electronics applications due to their potential for ferromagnetic order at room temperature, and various unique switching and spin-dependent conductivity properties. However, the precise mechanism by which the transition-metal doping produces ferromagnetism has been controversial. Here we have studied a dilute magnetic semiconductor (5% manganese-doped gallium arsenide) with Bragg-reflection standing-wave hard X-ray angle-resolved photoemission spectroscopy, and resolved its electronic structure into element- and momentum- resolved components. The measured valence band intensities have been projected into element-resolved components using analogous energy scans of Ga 3d, Mn 2p, and As 3d core levels, with results in excellent agreement with element-projected Bloch spectral functions and clarification of the electronic structure of this prototypical material. This technique should be broadly applicable to other multi-element materials.

cond-mat.mtrl-sci↗

arXiv2018

Localized segregation of gold in ultra-thin Fe films on Au(001)

The growth of up to 10 monolayer-thick Fe films on a Au(001) surface was investigated during deposition at room temperature and during annealing using low-energy electron diffraction and x-ray photoemission spectroscopy as well as locally with low-energy electron microscopy and photoemission electron microscopy. The growth proceeds with a submonolayer of Au segregating to the surface of Fe, which is in agreement with previous studies. Annealing was found to be critical for the presence of Au on the Fe surface. Our findings show that Au segregation proceeds by the formation of cracks in the Fe film, starting at the annealing temperature of 190 °C, through which Au diffuses towards the surface. We explain the localized Au segregation with a shadowing effect due to the oblique deposition geometry. As a result, an Fe film with significantly improved roughness, but covered with a Au overlayer, is obtained. This study shows the necessity to employ spatially-resolved techniques to fully understand the growth modes of the layered epitaxial systems.

cond-mat.mtrl-sci↗

arXiv2018

In aqua electrochemistry probed by XPEEM: experimental setup, examples, and challenges

Recent developments in environmental and liquid cells equipped with electron transparent graphene windows have enabled traditional surface science spectromicroscopy tools, such as X-ray photoelectron spectroscopy (XPS), photoemission electron microscopy (PEEM), and scanning electron microscopy (SEM) to be applied to study solid-liquid and liquid-gas interfaces. Here, we focus on the experimental implementation of PEEM to probe electrified graphene-liquid interfaces using electrolyte-filled microchannel arrays as a new sample platform. We demonstrate the important methodological advantage of these multi-sample arrays: they enable the combination of the wide field of view hyperspectral imaging capabilities from PEEM with the use of powerful data mining algorithms to reveal spectroscopic and temporal behaviors at the level of the individual microsample or the entire array ensemble

cond-mat.mtrl-sci↗