arXiv subjects

Martin Aeschlimann

Publications and source records attributed to Martin Aeschlimann.

At least 37 records · Page 2Linked to original sources

arXiv2023

Multiorbital exciton formation in an organic semiconductor

Harnessing the optoelectronic response of organic semiconductors requires a thorough understanding of the fundamental light-matter interaction that is dominated by the excitation of correlated electron-hole pairs, i.e. excitons. The nature of these excitons would be fully captured by knowing the quantum-mechanical wavefunction, which, however, is difficult to access both theoretically and experimentally. Here, we use femtosecond photoemission orbital tomography in combination with many-body perturbation theory to gain access to exciton wavefunctions in organic semiconductors. We find that the coherent sum of multiple electron-hole pair contributions that typically make up a single exciton can be experimentally evidenced by photoelectron spectroscopy. For the prototypical organic semiconductor buckminsterfullerene (C$_{60}$), we show how to disentangle such multiorbital contributions and thereby access key properties of the exciton wavefunctions including localization, charge-transfer character, and ultrafast exciton formation and relaxation dynamics.

cond-mat.mes-hall↗

arXiv2023

Laser-induced Creation of antiferromagnetic 180-degree domains in NiO/Pt bilayers

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 creation of antiferromagnetic domains by imaging the created domain structure utilizing the X-ray magnetic linear dichroism effect. We study the effect of different laser polarizations on the domain formation and identify a polarization-independent creation of 180° domain walls and domains with 180° different Néel vector orientation. By varying the irradiation parameters, we determine the switching mechanism to be thermally induced and demonstrate the reversibility. We thus demonstrate experimentally the possibility to optically create antiferromagnetic domains, an important step towards future functionalization of all optical switching mechanisms in antiferromagnets.

cond-mat.mtrl-sci↗

arXiv2022

Twisted light affects ultrafast demagnetization

Irradiation with an ultrashort laser pulse can completely destroy the magnetic order of ferromagnetic thin films on the femtosecond timescale. This phenomenon holds great potential for ultrafast spintronics and information processing and is an active field of research. It is still an open question if the angular momentum of light can support this effect. While it has been shown that the spin of light only has a negligible influence, we experimentally demonstrate the influence of ultrashort laser pulses with orbital angular momentum (OAM) on the magnetization dynamics of a thin nickel film. Our results reveal that the photonic OAM affects the demagnetization behavior within the first hundreds of femtoseconds depending on the handedness of the OAM with respect to the direction of the sample magnetization.

physics.optics↗

arXiv2022

Indirect optical manipulation of the antiferromagnetic order of insulating NiO by ultrafast interfacial energy transfer

We report the ultrafast, (sub)picosecond reduction of the antiferromagnetic order of the insulating NiO thin film in a Pt/NiO bilayer. This reduction of the antiferromagnetic order is not present in pure NiO thin films after a strong optical excitation. This ultrafast phenomenon is attributed to an ultrafast and highly efficient energy transfer from the optically excited electron system of the Pt layer into the NiO spin system. We propose that this energy transfer is mediated by a stochastic exchange scattering of hot Pt electrons at the Pt/NiO interface.

cond-mat.mtrl-sci↗

arXiv2022

FAIR data enabling new horizons for materials research

The prosperity and lifestyle of our society are very much governed by achievements in condensed matter physics, chemistry and materials science, because new products for sectors such as energy, the environment, health, mobility and information technology (IT) rely largely on improved or even new materials. Examples include solid-state lighting, touchscreens, batteries, implants, drug delivery and many more. The enormous amount of research data produced every day in these fields represents a gold mine of the twenty-first century. This gold mine is, however, of little value if these data are not comprehensively characterized and made available. How can we refine this feedstock; that is, turn data into knowledge and value? For this, a FAIR (findable, accessible, interoperable and reusable) data infrastructure is a must. Only then can data be readily shared and explored using data analytics and artificial intelligence (AI) methods. Making data 'findable and AI ready' (a forward-looking interpretation of the acronym) will change the way in which science is carried out today. In this Perspective, we discuss how we can prepare to make this happen for the field of materials science.

cond-mat.mtrl-sci↗

arXiv2022

Atomic and mesoscopic structure of Dy-based surface alloys on noble metals

Surface alloys are a highly tunable class of low dimensional materials with the opportunity to tune and control the spin and charge carrier functionalities on the nanoscale. Here, we focus on the atomic and mesoscopic structural details of three distinctive binary rare-earth-noble metals (RE/NM) surface alloys by employing scanning tunneling microscopy (STM) and low energy electron diffraction (LEED). Using Dysprosium as the guest element on fcc(111) noble metal substrates, we identify the formation of non-commensurate surface alloy superstructures which exhibit homogeneous moiré patterns for DyCu2/Cu (111) and DyAu2/Au(111), while an inhomogeneous one is found for DyAg2/Ag(111). The variations in the local structure are analyzed for all three surface alloys and the observed differences are discussed in the light of the lattice mismatches of the alloy layer with respect to the underlying substrate. For the particularly intriguing case of a Dy-Ag surface alloy, the surface alloy layer does not show a uniform long-range periodic structure, but consists of local hexagonal tiles separated by extended domain walls. These domain walls exist to relief the in-plane strain within the DyAg2 surface alloy layer. Our findings clearly demonstrate that surface alloying is an intriguing tool to tailor both the local atomic, but also the mesoscopic moiré structures of metallic heterostructures.

cond-mat.mtrl-sci↗

arXiv2021

Control of transport phenomena in magnetic heterostructures by wavelength modulation

We demonstrate the tuneablity of the ultrafast energy flow in magnetic/non-magnetic bilayer structures by changing the wavelength of the optical excitation. This is achieved by an advanced description of the temperature based $μ$T-model that explicitly considers the wavelength- and layer-dependent absorption profile within multilayer structures. For the exemplary case of a Ni/Au bilayer, our simulations predict that the energy flow from Ni to Au is reversed when changing the wavelength of the excitation from the infrared to the ultraviolet spectral range. These predictions are fully supported by characteristic signatures in the magneto-optical Kerr traces of the Ni/Au model system. Our results will open up new avenues to steer and control the energy transport in designed magnetic multilayer for ultrafast spintronic applications.

cond-mat.mes-hall↗

arXiv2021

Energy and Momentum Distribution of Surface Plasmon-induced Hot Carriers Isolated via Spatiotemporal Separation

Understanding the differences between photon-induced and plasmon-induced hot electrons is essential for the construction of devices for plasmonic energy conversion. The mechanism of the plasmonic enhancement in photochemistry, photocatalysis, and light-harvesting and especially the role of hot carriers is still heavily discussed. The question remains, if plasmon-induced and photon-induced hot carriers are fundamentally different, or if plasmonic enhancement is only an effect of field concentration producing these carriers in greater numbers. For the bulk plasmon resonance, a fundamental difference is known, yet for the technologically important surface plasmons this is far from being settled. The direct imaging of surface plasmon-induced hot carriers could provide essential insight, but the separation of the influence of driving laser, field-enhancement, and fundamental plasmon decay has proven to be difficult. Here, we present an approach using a two-color femtosecond pump-probe scheme in time-resolved 2-photon-photoemission (tr-2PPE), supported by a theoretical analysis of the light and plasmon energy flow. We separate the energy and momentum distribution of the plasmon-induced hot electrons from the one of photoexcited electrons by following the spatial evolution of photoemitted electrons with energy-resolved Photoemission Electron Microscopy (PEEM) and Momentum Microscopy during the propagation of a Surface Plasmon Polariton (SPP) pulse along a gold surface. With this scheme, we realize a direct experimental access to plasmon-induced hot electrons. We find a plasmonic enhancement towards high excitation energies and small in-plane momenta, which suggests a fundamentally different mechanism of hot electron generation, as previously unknown for surface plasmons.

cond-mat.mes-hall↗

arXiv2021

Spectroscopic evidence for a new type of surface resonance at noble metal surfaces

We investigate the surface- and bulk-like properties of the pristine (110)-surface of silver using threshold photoemission by excitation with light of 5.9 eV. Using a momentum microscope, we identified two distinct transitions along the $\overlineΓ\,\overline{\textrm{Y}}$-direction of the crystal. The first one is a so far unknown surface resonance for the (110) noble metal surface, exhibiting an exceptionally large bulk character, that has so far been elusive in surface sensitive experiments. The second one stems from the well known bulk-like Mahan cone oriented along the $ΓL$-direction inside the crystal but projected onto the (110)-surface cut. The existence of the new state is confirmed by photocurrent calculations and its character analyzed.

cond-mat.mtrl-sci↗

arXiv2021

Functional meta lenses for compound plasmonic vortex field generation and control

Surface plasmon polaritons carrying orbital angular momentum are of great fundamental and applied interest. However, common approaches for their generation are restricted to having a weak dependence on the properties of the plasmon-generating illumination, providing a limited degree of control over the amount of delivered orbital angular momentum. Here we experimentally show that by tailoring local and global geometries of vortex generators, a change in circular polarization handedness of light imposes arbitrary large switching in the delivered plasmonic angular momentum. Using time-resolved photoemission electron microscopy we demonstrate pristine control over the generation and rotation direction of high-order plasmonic vortices. We generalize our approach to create complex topological fields and exemplify it by studying and controlling a "bright vortex", exhibiting the breakdown of a high-order vortex into a mosaic of unity-order vortices while maintaining the overall angular momentum density. Our results provide tools for plasmonic manipulation and could be utilized in lab-on-a-chip devices.

physics.optics↗

arXiv2021

Adsorption-induced modification of the hot electron lifetime in a Pb/Ag111 quantum well system

The interfacial band structures of multilayer systems play a crucial role for the ultrafast charge and spin carrier dynamics at interfaces. Here, we study the energy- and momentum-dependent quasiparticle lifetimes of excited states of a lead monolayer film on Ag(111) prior and after the adsorption of a monolayer of 3,4,9,10-perylene-tetracarboxylic-dianhydride (PTCDA). Using time-resolved two-photon momentum microscopy, we show that the electron dynamics of the bare Pb/Ag(111) bilayer system is dominated by isotropic intraband scattering processes within the quantum well state as well as interband scattering processes from the QWS into the Pb sideband. After the adsorption of PTCDA on the Pb monolayer, the interband scattering is suppressed and the electron dynamics is solely determined by intraband or inelastic scattering processes. Our findings hence uncover a new possibility to selectively tune and control scattering processes of quantum well systems by the adsorption of organic molecules.

cond-mat.mes-hall↗

arXiv2020

Orbital angular momentum multiplication in plasmonic vortex cavities

Orbital angular momentum of light is a core feature in photonics. Its confinement to surfaces using plasmonics has unlocked many phenomena and potential applications. Here we introduce the reflection from structural boundaries as a new degree of freedom to generate and control plasmonic orbital angular momentum. We experimentally demonstrate plasmonic vortex cavities, generating a succession of vortex pulses with increasing topological charge as a function of time. We track the spatio-temporal dynamics of these angularly decelerating plasmon pulse train within the cavities for over 300 femtoseconds using time-resolved Photoemission Electron Microscopy, showing that the angular momentum grows by multiples of the chiral order of the cavity. The introduction of this degree of freedom to tame orbital angular momentum delivered by plasmonic vortices, could miniaturize pump-probe-like quantum initialization schemes, increase the torque exerted by plasmonic tweezers and potentially achieve vortex lattice cavities with dynamically evolving topology.

physics.optics↗

arXiv2020

Progress on band structure engineering of twisted bilayer and two-dimensional moiré heterostructures

Artificially constructed van der Waals heterostructures (vdWHs) provide an ideal platform for realizing emerging quantum phenomena in condensed matter physics. Two methods for building vdWHs have been developed: stacking two-dimensional (2D) materials into a bilayer structure with different lattice constants, or with different orientations. The interlayer coupling stemming from commensurate or incommensurate superlattice pattern plays an important role in vdWHs for modulating the band structures and generating new electronic states. In this article, we review a series of novel quantum states discovered in two model vdWH systems -- graphene/hexagonal boron nitride (hBN) hetero-bilayer and twisted bilayer graphene (tBLG), and discuss how the electronic structures are modified by such stacking and twisting. We also provide perspectives for future studies on hetero-bilayer materials, from which an expansion of 2D material phase library is expected.

cond-mat.mtrl-sci↗

arXiv2020

Signatures of an Atomic Crystal in the Band Structure of a Molecular Thin Film

Transport phenomena in molecular materials are intrinsically linked to the orbital character and the degree of localization of the valence states. Here, we combine angle-resolved photoemission with photoemission tomography to determine the spatial distribution of all molecular states of the valence band structure of a C$_{60}$ thin film. While the two most frontier valence states exhibit a strong band dispersion, the states at larger binding energies are characterized by distinct emission patterns in energy and momentum space. Our findings demonstrate the formation of an atomic crystal-like band structure in a molecular solid with delocalized $π$-like valence states and strongly localized $σ$-states at larger binding energies.

cond-mat.mes-hall↗

arXiv2020

Modification of the charge and magnetic order of a low dimensional ferromagnet by molecule-surface bonding

The ability to design and control the spin and charge order of low dimensional materials on the molecular scale offers an intriguing pathway towards the miniaturization of spintronic technology towards the nanometer scale. In this work, we focus on the adsorption induced modifications of the magnetic and electronic properties of a low dimensional ferromagnetic surface alloy after the adsorption of the prototypical organic molecule perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA). For this metal-organic interface, we observe the formation of a localized $σ$-like bond between the functional molecular groups and the surface alloy atoms. This strong chemical bonding coincides with a lifting of the characteristic surface alloy band structure and a reduction of the magnitude of the local magnetic moments of the Dy atoms by 18%. We attribute both findings to a mixing of spin-degenerate molecular states with spin-split states of the Dy-Ag surface alloy via the sigma-like bonds between PTCDA and the Dy surface alloy atoms. Our findings clearly demonstrate the potential of tailored molecule-surface sigma-bonds to control not only the electronic but also the magnetic order of low dimensional materials.

cond-mat.mes-hall↗

arXiv2020

Ultrafast charge carrier separation in Potassium-intercalated endohedral metallofullerene Sc$_3$N@C$_{80}$ thin films

Molecular materials have emerged as highly tunable materials for photovoltaic and light-harvesting applications. The most severe challenge of this class of materials is the trapping of charge carriers in bound electron-hole pairs, which severely limits the free charge carrier generation. Here, we demonstrate a significant modification of the exciton dynamics of thin films of endohedral metallofullerene complexes upon alkali metal intercalation. For the exemplary case of Sc$_3$N@C$_{80}$ thin films, we show that potassium intercalation results in an additional relaxation channel for the optically excited charge-transfer excitons that prevents the trapping of excitons in a long-lived Frenkel exciton-like state. Instead, K intercalation leads to an ultrafast exciton dissociation coinciding most likely with the generation of free charge carriers. In this way, we propose alkali metal doping of molecular films as a novel approach to enhance the light to-charge carrier conversion efficiency in photovoltaic materials.

cond-mat.mes-hall↗

arXiv2020

Ultrafast charge-transfer exciton dynamics in C$_{60}$ thin films

The high flexibility of organic molecules offers great potential for designing the optical properties of light-active materials for the next generation of optoelectronic and photonic applications. However, despite successful implementations of molecular materials in todays' display and photovoltaic technology, many fundamental aspects of the light-to-charge conversion have still to be uncovered. Here, we focus on the ultrafast dynamics of optically excited excitons in C$_{60}$ thin films depending on the molecular coverage and the light-polarization of the optical excitons. Using time- and momentum-resolved photoemission with fs-XUV radiation, we follow the depopulation dynamics in the excited states while simultaneously monitoring the signatures of the excitonic charge character in the molecular valence states. Optical excitation with visible light results in the instantaneous formation of charge-transfer (CT) excitons, which transform stepwise into energetically lower Frenkel-like excitons. While the number and energetic position of energy levels within this cascade process are independent of the molecular coverage and the light polarization of the optical excitation, we find quantitative differences in the depopulation times and the optical excitation efficiency. Our comprehensive study reveals the crucial role of CT excitons for the excited state dynamics of homo-molecular fullerene materials and thin films.

cond-mat.mes-hall↗

arXiv2020

Vertical bonding distances and interfacial band structure of PTCDA on a Sn-Ag surface alloy

Molecular materials enable a vast variety of functionalities for novel electronic and spintronic devices. The unique possibility to alter or substitute organic molecules or metallic substrates offers the opportunity to modify and optimize interfacial properties for almost any desired field of application. For this reason, we extend the successful approach to control molecular interfaces by surface alloying. We present a comprehensive characterization of the structural and electronic properties of the interface formed between the prototypical molecule PTCDA and a Sn-Ag surface alloy grown on an Ag(111) single crystal surface. We monitor the changes of adsorption height of the surface alloy atoms and electronic valence band structure upon adsorption of one layer of PTCDA using the normal incidence x-ray standing wave technique in combination with momentum-resolved photoelectron spectroscopy. We find that the vertical buckling and the surface band structure of the SnAg$_2$ surface alloy is not altered by the adsorption of one layer of PTCDA, in contrast to our recent study of PTCDA on a PbAg$_2$ surface alloy [Phys. Rev. Lett. 117, 096805 (2016)] . In addition, the vertical adsorption geometry of PTCDA and the interfacial energy level alignment indicate the absence of any chemical interaction between the molecule and the surface alloy. We attribute the different interactions at these PTCDA/surface alloy interfaces to the presence or absence of local $σ$-bonds between the PTCDA oxygen atoms and the surface atoms. Combining our findings with results from literature, we are able to propose an empiric rule for engineering the surface band structure of alloys by adsorption of organic molecules.

cond-mat.mes-hall↗