Armin Kleibert

Paul Scherrer Institut | PSI · Swiss Light Source (SLS)

X-ray photoemission electron microscopy combined with x-ray magnetic circular dichroism is used to study the magnetic properties of individual iron nanoparticles with sizes ranging from 20 down to 8 nm. While the magnetocrystalline anisotropy of bulk iron suggests superparamagnetic behavior in this size range, ferromagnetically blocked particles ar...

Magnetic nanoparticles are important building blocks for future technologies ranging from nano-medicine to spintronics. Many related applications require nanoparticles with tailored magnetic properties. However, despite significant efforts undertaken towards this goal, a broad and poorly-understood dispersion of magnetic properties is reported, eve...

Laser-induced manipulation of magnetism at the nanoscale is a rapidly growing research topic with potential for applications in spintronics. In this work, we address the role of the scattering cross section, thermal effects, and laser fluence on the magnetic, structural, and chemical stability of individual magnetic nanoparticles excited by single...

Magnetic nanoparticles are of great interest for applications in fields ranging from biomedicine to spintronics. However, despite considerable work, their size-dependent magnetic properties are still poorly understood. In this chapter, we will introduce x-ray photoemission electron microscopy (XPEEM) as a spectromicroscopy technique ideally suited...

Understanding chemical reactivity and magnetism of 3d transition metal nanoparticles is of fundamental interest for applications in fields ranging from spintronics to catalysis. Here, we present an atomistic picture of the early stage of the oxidation mechanism and its impact on the magnetism of Co nanoparticles. Our experiments reveal a two-step p...

In this work, we investigated cyclohexane oxidative dehydrogenation (ODH) catalyzed by cobalt ferrite nanoparticles supported on reduced graphene oxide (RGO). We aim to identify the active sites that are specifically responsible for full and partial dehydrogenation using advanced spectroscopic techniques such as X-ray photoelectron emission microsc...

Hard x-ray angle-resolved photoemission spectroscopy reveals the momentum-resolved band structure in an epitaxial Mn2Au(001) film capped by a 2-nm-thick ferromagnetic permalloy layer. By magnetizing the permalloy capping layer, the exceptionally strong exchange bias aligns the Néel vector in the Mn2Au(001) film accordingly. Uncompensated interface...

Soft X-ray ptychography was employed to simultaneously image the ferroelectric and antiferromagnetic domains in an 80 nm thick freestanding multiferroic BiFeO3. The antiferromagnetic spin cycloid was resolved by reconstructing the resonant elastic X-ray scattering and visualised together with mosaic-like ferroelectric domains in a linear dichroic c...

The relationship between magnetization and light has been the subject of intensive research for the past century, focusing on the impact of magnetic moments on light polarization. Conversely, the manipulation of magnetism through polarized light is being investigated to achieve all-optical control of magnetism in spintronics. While remarkable disco...

Hard X-ray angle-resolved photoemission spectroscopy reveals the momentum-resolved band structure in an epitaxial Mn2Au(001) film capped by a 2 nm thick ferromagnetic Permalloy layer. By magnetizing the Permalloy capping layer, the exceptionally strong exchange bias aligns the Neel vector in the Mn2Au(001) film accordingly. Uncompensated interface...

The antiferromagnetic order in heterostructures of NiO/Pt thin films can be modified by optical pulses. After the irradiation with laser light, the optically induced creation of antiferromagnetic domains can be observed by imaging the created domain structure utilizing the X‐ray magnetic linear dichroism effect. The effect of different laser polari...

Hydrogen spillover from metal nanoparticles to oxides is an essential process in hydrogenation catalysis and other applications such as hydrogen storage. It is important to understand how far this process is reaching over the surface of the oxide. Here, we present a combination of advanced sample fabrication of a model system and in situ X-ray phot...

Van der Waals (vdW) magnets are an ideal platform for tailoring 2D magnetism with immense potential for spintronics applications and are intensively investigated. However, little is known about the microscopic origin of magnetic order in these antiferromagnetic systems. X‐ray photoemission electron microscopy is used to address the electronic and m...

The absence of stray fields, their insensitivity to external magnetic fields, and ultrafast dynamics make antiferromagnets promising candidates for active elements in spintronic devices. Here, we demonstrate manipulation of the Néel vector in the metallic collinear antiferromagnet Mn2Au by combining strain and femtosecond laser excitation. Applying...

Van der Waals (vdW) magnets are an ideal platform for tailoring two-dimensional (2D) magnetism with immense potential for spintronics applications and are intensively investigated. However, little is known about the microscopic origin of magnetic order in these antiferromagnetic systems. We used X-ray photoemission electron microscopy to address th...

We demonstrate how the antiferromagnetic order in heterostructures of NiO/Pt thin films can be modified by optical pulses. We irradiate our samples with laser light and identify an optically induced switching of the antiferromagnetic order by imaging the created domain structure utilizing the X-ray magnetic linear dichroism effect. We study the eff...

We present a detailed atomistic picture of the oxidation mechanism of Co nanoparticles and its impact on magnetism by experimentally following the evolution of the structure, chemical composition, and magnetism of individual, gas-phase grown Co nanoparticles during controlled oxidation. The early stage oxidation occurs in a twostep process characte...

We have studied the structural and magnetic properties of Tb(Fe0.2Mn0.2Co0.2Cr0.2Ni0.2)O3 (T5BO) high-entropy oxide perovskite (HEOP) thin films. Using synchrotron-based x-ray absorption spectroscopy, employing x-ray magnetic circular dichroism, we performed an element-sensitive study of epitaxial T5BO thin films. The measurements reveal a magnetic...

One material containing kagome bilayers and featuring both exceptional magnetism and electron transport is the ferromagnetic metal Fe3Sn2. Notwithstanding the widespread interest in Fe3Sn2, crystal twinning, difficulties in distinguishing surface from bulk states, and a large unit cell have until now prevented the synchrotron-based spectroscopic ob...

In frustrated spin systems, magnetic phase transitions underpin the formation of exotic, frustration-driven magnetic phases. Of great importance is the ability to manipulate these transitions to access specific phases, which in turn provides a means to discover and control novel phenomena. Artificial spin systems incorporating lithographically fabr...

A novel transparent conductive support structure for scalable integration of 2D materials is demonstrated, providing an electronically passive 2D–3D interface while also enabling facile interfacial charge transport. This structure, which comprises an evaporated nanocrystalline carbon (nc‐C) film beneath nanometer‐thin atomic layer deposited AlOx, i...

The absence of stray fields, their insensitivity to external magnetic fields, and ultrafast dynamics make antiferromagnets promising candidates for active elements in spintronic devices. Here, we demonstrate manipulation of the N\'{e}el vector in the metallic collinear antiferromagnet Mn$_2$Au by combining strain and femtosecond laser excitation. A...

Spin glasses, generally defined as disordered systems with randomized competing interactions1,2, are a widely investigated complex system. Theoretical models describing spin glasses are broadly used in other complex systems, such as those describing brain function3,4, error-correcting codes5 or stock-market dynamics6. This wide interest in spin gla...

Passive 2D–3D Interfaces In article number 2111343, Alex Henning, Ian D. Sharp, and co‐workers develop a novel transparent and conductive support structure for the scalable integration and direct growth of 2D materials. The structure comprises a nanocrystalline carbon layer coated with nanometer‐thin alumina and provides an electronically passive 2...

Spin glasses, generally defined as disordered systems with randomized competing interactions, are a widely investigated complex system. Theoretical models describing spin glasses are broadly used in other complex systems, such as those describing brain function, error-correcting codes, or stock-market dynamics. This wide interest in spin glasses pr...

Prior studies of the thin film deposition of the metal-organic compound of Fe(pz)Pt[CN]4 (pz = pyrazine) using the matrix-assisted pulsed laser evaporation (MAPLE) method, provided evidence for laser-induced decomposition of the molecular structure resulting in a significant downshift of the spin transition temperature. In this work we report new r...

We present a novel transparent conductive support structure for two-dimensional (2D) materials that provides an electronically passive 2D/3D interface while also enabling facile interfacial charge transport. This structure, which comprises an evaporated nanocrystalline carbon (nc-C) film beneath an atomic layer deposited alumina (ALD AlOx) layer, i...

In frustrated spin systems, magnetic phase transitions underpin the formation of exotic, frustration-driven magnetic phases. Of great importance is the ability to manipulate these transitions to access specific phases, which in turn provides a means to discover and control novel phenomena. Artificial spin systems, incorporating lithographically-fab...

Néel skyrmions are generally realized in asymmetric multilayers made of heavy metals (HMs) and ultrathin ferromagnets possessing strong interfacial Dzyaloshinskii-Moriya interactions (iDMIs). Depending on the relative strengths of iDMIs at the interfaces, various types of Néel skyrmions have been suggested, which are typified with characteristicall...

We introduce and explore low-energy configurations in two-dimensional arrays consisting of Ising-type dipolar coupled nanomagnets lithographically defined onto three-nanomagnet vertices arranged in a triangular coordination. Thus, the system is dubbed the trimerized triangular lattice. Employing synchrotron-based photoe-mission electron microscopy,...

Long-range magnetic ordering can be stabilized in arrays of single-domain nanomagnets through dipolar interactions. In these metamaterials, the magnetic properties are determined by geometric parameters such as the nanomagnet shape and lattice symmetry. Here, we demonstrate engineering of the anisotropy in a dipolar magnetic metamaterial by tuning...

Ultrashort optical pulses can trigger a variety of non-equilibrium processes in magnetic thin films affecting electrons and spins on femtosecond timescales. In order to probe the charge and magnetic degrees of freedom simultaneously, we developed an X-ray streaking technique that has the advantage of providing a jitter-free picture of absorption cr...

Ultrashort optical pulses can trigger a variety of non-equilibrium processes in magnetic thin films affecting electrons and spins on femtosecond timescales. In order to probe the charge and magnetic degrees of freedom simultaneously, we developed an x-ray streaking technique that has the advantage of providing a jitter-free picture of absorption cr...

The availability of intense soft x-ray beams with tunable energy and polarization has pushed the development of highly sensitive, element-specific, and noninvasive microscopy techniques to investigate condensed matter with high spatial and temporal resolution. The short wavelengths of soft x-rays promise to reach spatial resolutions in the deep sin...

Laser-induced manipulation of magnetism at the nanoscale is a rapidly growing research topic with potential for applications in spintronics. In this work, we address the role of the scattering cross section, thermal effects, and laser fluence on the magnetic, structural, and chemical stability of individual magnetic nanoparticles excited by single...

Artificial kagome spin ice exhibits exotic magnetic correlations driven by a combination of geometric frustration and dipolar interactions that, at low-enough temperature, can result in ordered phases. This order, whether it is the ground state of several kagome rings, or the theoretically predicted long-range order of an extended array, has yet to...

Amorphous Tb x Co 100−x magnetic alloys exhibit a list of intriguing properties, such as perpendicular magnetic anisotropy, high magneto-optical activity, and magnetization switching using ultrashort optical pulses. Varying the Tb:Co ratio in these alloys allows for tuning properties such as the saturation magnetic moment, coercive field, and the p...

Understanding the metal-support interaction (MSI) is crucial to comprehend how the catalyst support affects performance and whether this interaction can be exploited in order to design new catalysts with enhanced properties. Spatially resolved soft X-ray absorption spectroscopy (XAS) in combination with Atomic Force Microscopy (AFM) and Scanning He...

The control of emergent magnetic monopoles for the generation of monopole currents in artificial spin ice is essential for their use in nanomagnet-based device applications. Here we present a scheme to inject monopole currents into an artificial square ice at specific locations, which provides a means to control the propagation of the generated eme...

Ultrafast phenomena on a femtosecond timescale are commonly examined by pump-probe experiments. This implies multiple measurements, where the sample under investigation is pumped with a short light pulse and then probed with a second pulse at various time delays to follow its dynamics. Recently, the principle of streaking extreme ultraviolet (XUV)...

We investigate spin dynamics of microstates in artificial spin ice (ASI) in Ni_{81}Fe_{19} nanomagnets arranged in an interconnected kagome lattice using microfocus Brillouin light scattering, broadband ferromagnetic resonance, magnetic force microscopy, x-ray photoemission electron microscopy, and simulations. We experimentally reconfigure microst...

X-ray free-electron lasers (XFELs) are paving the way towards new experiments in many scientific fields, such as ultrafast science, nonlinear spectroscopy, and coherent imaging. However, the strong intensity fluctuations inherent to the lasing process in these sources often lead to problems in signal normalization. In order to address this challeng...

Laser-induced manipulation of magnetism at the nanoscale is a rapidly growing research topic with potential for applications in spintronics. In this work, we address the role of the scattering cross section, thermal effects, and laser fluence on the magnetic, structural, and chemical stability of individual magnetic nanoparticles excited by single...

Ultrafast phenomena on a femtosecond timescale are commonly examined by pump-probe experiments. This implies multiple measurements where the sample under investigation is pumped with a short light pulse and has to be probed with a second pulse at various time delays to follow its dynamics. Recently, the principle of streaking extreme ultraviolet (X...

This chapter focuses on the ability of X-ray photoemission electron microscopy (XPEEM) to provide local spectroscopic information and therefore of probing the electronic structure of materials down to the nm scale. It provides a brief description of the working principles of XPEEM and illustrates with examples from the literature the gamut of possi...

Amorphous TbCo magnetic alloys exhibit a list of intriguing properties, such as perpendicular magnetic anisotropy, high magneto-optical activity and magnetization switching using ultrashort optical pulses. Varying the Tb:Co ratio in these alloys allows for tuning properties such as the saturation magnetic moment, coercive field and the performance...

Artificial spin ices are a class of metamaterials consisting of magnetostatically coupled nanomagnets whose interactions often give rise to remarkable emergent behavior and which have the potential to be harnessed for the creation of functional materials. Consequently, the ability to map the stray field of such systems can be decisive for gaining u...

Using state-of-the-art electron-beam lithography, Ising-type nanomagnets may be defined onto nearly any two-dimensional pattern imaginable. The ability to directly observe magnetic configurations achieved in such artificial spin systems makes them a perfect playground for the realization of artificial spin glasses. However, no experimental realizat...

An electric current flowing in Pt, a material with strong spin-orbit coupling, leads to spins accumulating at the interfaces by virtue of the spin Hall effect and interfacial charge-spin conversion. We measure the influence of these interfacial magnetic moments onto adjacent 3d transition-metal layers by x-ray absorption spectroscopy and x-ray magn...

Nanomagnetic logic, which makes use of arrays of dipolar-coupled single-domain nanomagnets for computation, holds promise as a low-power alternative to traditional computation with CMOS. Beyond the use of nanomagnets for Boolean logic, nanomagnets can also be exploited for nondeterministic computational schemes such as edge detection in images and...

The successful design, installation and operation of a high spatial resolution X-ray photoelectron spectrometer at the Swiss Light Source is presented. In this instrument, a Fresnel zone plate is used to focus an X-ray beam onto the sample and an electron analyzer positioned at 45° with respect to the incoming beam direction is used to collect phot...

Ultrafast dynamics are generally investigated using stroboscopic pump-probe measurements, which characterize the sample properties for a single, specific time delay. These measurements are then repeated for a series of discrete time delays to reconstruct the overall time trace of the process. As a consequence, this approach is limited to the invest...

An electric current flowing in Pt, a material with strong spin-orbit coupling, leads to spins accumulating at the interfaces by virtue of the spin Hall effect and interfacial charge-spin conversion. We measure the influence of these interfacial magnetic moments onto adjacent 3d transition metal layers by x-ray absorption spectroscopy and x-ray magn...

Magnetic building blocks in two dimensions Artificial magnetic structures can offer a variety of functionalities in spintronics devices. Luo et al. engineered magnetic domains in Pt/Co/AlO x trilayers that had alternating in-plane and out-of-plane magnetizations. The regions interacted laterally through the so-called Dzyaloshinskii-Moriya interacti...

Stable, single-nanometer thin, and free-standing two-dimensional layers with controlled molecular architectures are desired for several applications ranging from (opto-)electronic devices to nanoparticle and single-biomolecule characterization. It is, however, challenging to construct these stable single molecular layers via self-assembly, as the c...

Nanomagnetic logic, which makes use of arrays of dipolar-coupled single domain nanomagnets for computation, holds promise as a low power alternative to traditional computation with CMOS. Beyond the use of nanomagnets for Boolean logic, nanomagnets can also be exploited for non-deterministic computational schemes such as edge detection in images and...

Magnetic skyrmions are knot-like quasiparticles. They are candidates for non-volatile data storage in which information is moved between fixed read and write terminals. The read-out operation of skyrmion-based spintronic devices will rely on the electrical detection of a single magnetic skyrmion within a nanostructure. Here we present Pt/Co/Ir nano...

Ultrafast dynamics are generally investigated using stroboscopic pump-probe measurements, which characterize the sample properties for a single, specific time delay. These measurements are then repeated for a series of discrete time delays to reconstruct the overall time trace of the process. As a consequence, this approach is limited to the invest...

We demonstrate that thick permalloy films exhibiting a weak growth-induced perpendicular magnetic anisotropy can be employed as an ideal test system for the investigation of gyration dynamics in topologically trivial and nontrivial magnetic states ranging from an isolated magnetic skyrmion to more complex nπ spin configurations.

Development of a New Soft X-ray Ptychography Spectro-Microscope at the Swiss Light Source (SLS) - Volume 24 Supplement - Manuel Langer, Carlos A. F. Vaz, Sabina Chiriotti, Anna Bergamaschi, Manuel Guizar-Sicairos, Armin Kleibert, Jorg Raabe

We demonstrated that thick Permalloy films exhibiting a weak growth-induced perpendicular magnetic anisotropy can be employed as an ideal test system for the investigation of gyration dynamics in topologically trivial and non-trivial magnetic states ranging from an isolated magnetic skyrmion to more complex n$\pi$ spin configurations.

We report the observation of the three-dimensional angular dependence of the spin Hall magnetoresistance (SMR) in a bilayer of the epitaxial antiferromagnetic insulator NiO(001) and the heavy metal Pt, without any ferromagnetic element. The detected angular-dependent longitudinal and transverse magnetoresistances are measured by rotating the sample...

While the industrial implementation of extreme ultraviolet lithography for upcoming technology nodes is becoming ever more realistic, a number of challenges have yet to be overcome. Among them is the need for actinic mask inspection. We report on reflective-mode lensless imaging of a patterned multi-layer mask sample at extreme ultraviolet waveleng...

Nanomagnets are a promising low-power alternative to traditional computing. However, the successful implementation of nanomagnets in logic gates has been hindered so far by a lack of reliability. Here, we present a novel design with dipolar-coupled nanomagnets arranged on a square lattice to (i) support transfer of information and (ii) perform logi...