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Aehle, Max ; Alme, Johan ; Banaföldi, Gergely Gábor ; Blühdorn, Johannes ; Bodova, Tea ; Borshchov, Vyacheslav ; Brink, Anthony van den ; Eikeland, Viljar ; Feofilov, Gregory ; Garth, Christoph ; Gauger, Nicolas R. ; Grøttvik, Ola ; Helstrup, Håvard ; Igolkin, Sergey ; Keidel, Ralf ; Kobdaj, Chinorat ; Kortus, Tobias ; Kusch, Lisa ; Leonhardt, Viktor ; Mehendale, Shruti ; Mulawade, Raju Ningappa ; Odland, Odd Harald ; O'Neill, Georg ; Papp, Gábor ; Peitzmann, Thomas ; Seime Pettersen, Helge Egil ; Piersimoni, Pierluigi ; Pochampalli, Rohit ; Protsenko, Maksym ; Rauch, Max ; Ur Rehman, Attiq ; Richter, Matthias ; Röhrich, Dieter ; Sagebaum, Max ; Santana, Joshua ; Schilling, Alexander ; Seco, Joao ; Songmoolnak, Arnon ; Sudár, Ákos ; Tambave, Ganesh ; Tymchuk, Ihor ; Ullaland, Kjetil ; Varga-Kofarago, Monika ; Volz, Lennart ; Wagner, Boris ; Wendzel, Steffen ; Wiebel, Alexander ; Xiao, Ren Zheng ; Yang, Shiming ; Zillien, Sebastian
Objective. Gradient-based optimization using algorithmic derivatives can be a useful technique to improve engineering designs with respect to a computer-implemented objective function. Likewise, uncertainty quantification through computer simulations can be carried out by means of derivatives of the computer simulation. However, the effectiveness of these techniques depends on how 'well-linearizable' the software is. In this study, we assess how promising derivative information of a typical proton computed tomography (pCT) scan computer simulation is for the aforementioned applications. Approach. This study is mainly based on numerical experiments, in which we repeatedly evaluate three representative computational steps with perturbed input values. We support our observations with a review of the algorithmic steps and arithmetic operations performed by the software, using debugging techniques. Main results. The model-based iterative reconstruction (MBIR) subprocedure (at the end of the software pipeline) and the Monte Carlo (MC) simulation (at the beginning) were piecewise differentiable. However, the observed high density and magnitude of jumps was likely to preclude most meaningful uses of the derivatives. Jumps in the MBIR function arose from the discrete computation of the set of voxels intersected by a proton path, and could be reduced in magnitude by a 'fuzzy voxels' approach. The investigated jumps in the MC function arose from local changes in the control flow that affected the amount of consumed random numbers. The tracking algorithm solves an inherently non-differentiable problem. Significance. Besides the technical challenges of merely applying AD to existing software projects, the MC and MBIR codes must be adapted to compute smoother functions. For the MBIR code, we presented one possible approach for this while for the MC code, this will be subject to further research. For the tracking subprocedure, further research on surrogate models is necessary.
We discuss the dynamics of the formation of a Bose polaron when an impurity is injected into a weakly interacting one-dimensional Bose condensate. While for small impurity-boson couplings this process can be described within the Froehlich model as generation, emission and binding of Bogoliubov phonons, this is no longer adequate if the coupling becomes strong. To treat this regime we consider a mean-field approach beyond the Froehlich model which accounts for the backaction to the condensate, complemented with Truncated Wigner simulations to include quantum fluctuation. For the stationary polaron we find a periodic energy-momentum relation and non-monotonous relation between impurity velocity and polaron momentum including regions of negative impurity velocity. Studying the polaron formation after turning on the impurity-boson coupling quasi-adiabatically and in a sudden quench, we find a very rich scenario of dynamical regimes. Due to the build-up of an effective mass, the impurity is slowed down even if its initial velocity is below the Landau critical value. For larger initial velocities we find deceleration and even backscattering caused by emission of density waves or grey solitons and subsequent formation of stationary polaron states in different momentum sectors. In order to analyze the effect of quantum fluctuations we consider a trapped condensate to avoid 1D infrared divergencies. Using Truncated Wigner simulations in this case we show under what conditions the influence of quantum fluctuations is small.
European crayfish species are considered keystone in freshwater ecosystems. As such, their conservation is of paramount importance to prevent biodiversity decline and loss of ecosystem function. Unfortunately, today, European crayfish species are among the most threatened crayfish species worldwide. An especially relevant threat is represented by the invasive pathogen Aphanomyces astaci. This oomycete, native of North America, has been one of the main causes of crayfish population declines across Europe since its first introduction 150 years ago, to the point of causing the local extinction of many populations. Over the years, several introductions of A. astaci strains into Europe took place through translocation of infected North American crayfish, and were followed by mass mortalities across European crayfish populations. However, in the past 20 years, more and more reports emerged of European crayfish populations surviving A. astaci infections or being latently infected with the pathogen. The survival of infected crayfish can be ascribed to both increased resistance of some crayfish populations and decreased virulence of some A. astaci strains. As the relationship between host and pathogen in Europe is changing, it is imperative to gain insights on what shapes these changes to understand the implications for the long-term coexistence of crayfish and A. astaci in Europe. With this thesis, I focused on the virulence of A. astaci, looking for mechanisms, patterns and determinants underlying the pathogen’s virulence variability. In particular, by characterising the virulence of several A. astaci strains, I identified two possible different mechanisms of loss of virulence. I revealed that A. astaci’s virulence variability is not linked to variation of in vitro growth and sporulation, traits classically associated with a pathogen’s virulence. Based on these results, I suggest that the pathogen’s virulence determinants are likely its “virulence effectors”, of which A. astaci genome is enriched. Additionally, with the present work I provided transcriptomic evidence of coevolution between A. astaci and European crayfish. I showed that the haplogroups based on the canonical mitochondrial markers, often used to assess A. astaci’s virulence to inform management actions, do not differ for some of their characterising phenotypical traits, including virulence. Finally, after experimental characterisation of virulence and assessment of its likely phenotypical determinants, i.e., sporulation and growth, the next and more comprehensive step to study the pathogen’s virulence is through genomic approaches. To this aim, I provided key data for future comparative genomic studies, i.e., highly complete genome assemblies based on Nanopore (3) and Illumina reads (11). These data can be exploited in several ways, from building a pangenome of the species to a genome-wide association study (GWAS), that can offer a much deeper understanding of A. astaci’s virulence and adaptability. In particular, the identification of the loci associated with virulence through a GWAS has the potential to be revolutionary for the management of A. astaci, as it can become the basis to create a genomic tool to quickly and accurately assess the virulence of newly introduced strains, directing management actions towards the more dangerous strains.
Burgardt, Sabrina ; Jäger, Simon Balthasar ; Feß, Julian ; Hiebel, Silvia ; Schneider, Imke ; Widera, Artur
We report the experimental implementation of dynamical decoupling on a small, non-interacting ensemble of up to 25 optically trapped, neutral Cs atoms. The qubit consists of the two magnetic-insensitive Cs clock states \(\vert F = 3, m_F = 0\rangle\) and \(\vert F = 4, m_F = 0\rangle\), which are coupled by microwave radiation. We observe a significant enhancement of the coherence time when employing Carr-Purcell-Meiboom-Gill (CPMG) dynamical decoupling. A CPMG sequence with ten refocusing pulses increases the coherence time of 16.2(9) ms by more than one order of magnitude to 178(2) ms. In addition, we make use of the filter function formalism and utilise the CPMG sequence to measure the background noise floor affecting the qubit coherence, finding a power-law noise spectrum \(1/\omega^\alpha\) with \(\mathit{\alpha} = 0.89(2)\). This finding is in very good agreement with an independent measurement of the noise in the intensity of the trapping laser. Moreover, the measured coherence evolutions also exhibit signatures of low-frequency noise originating at distinct frequencies. Our findings point toward noise spectroscopy of engineered atomic baths through single-atom dynamical decoupling in a system of individual Cs impurities immersed in an ultracold 87Rb bath.
Olive mill wastewater (OMW) is a by-product of olive oil extraction and its disposal on soil has been associated with significant environmental challenges, including toxic effects on soil organisms and quality of groundwater due to its high phenolic content. Recent studies focusing on the dynamics of OMW degradation in soil are handling the environmental conditions as main factors influencing the fate and transport of polyphenols in the soil-water system. The understanding of seasonal-dependent phenol leaching from OMW-treated soil remained elusive, as field studies are hindered by spatial variability and complex environmental dynamics. Therefore, controlled lysimeter experiments were conducted to investigate the leaching and transport mechanisms of OMW-derived phenolic compounds in soil.
This thesis presents the results of an 18-week lysimeter experiment conducted in a laboratory setting, aimed at monitoring and comprehending the distribution and leaching of OMW-derived phenolic compounds in soil after OMW application. The experiment spanned four seasonal simulation phases, including two winter, one spring, and one summer, under semi-arid climate Tunisian conditions. The effects of OMW on soil leachates properties, soil water repellency, and soil water retention capacity were assessed.
The soil leachates exhibited varying degrees of recovery across the different simulation phases. However, persistent salinity in the leachates and high soil water repellency at the top treated OMW-soils were recorded. The findings revealed also that OMW application changed the pore size distribution in treated OMW-soils. Most of the OMW-derived phenols were immobilized in the upper 5 cm of the soil. Notably, soluble phenolic compounds exhibited the formation of coarser pores for the sake of fine pores, suggesting that OMW- organic carbon played a crucial role in controlling the depth-dependent transport mechanisms of OMW within the soil matrix.
In conclusion, this study provides valuable insights into the fate and impact of OMW-derived phenolic compounds in soil. It emphasizes the significance of conducting OMW applications with careful irrigation practices and thorough phenol leaching surveys to minimize the risk of potential groundwater contamination. Additionally, more experiments are warranted to investigate the sorption capacity of the soil during and after OMW application and its influence on the stability of soluble phenolic compounds
in soils.
Thermo-optic interaction significantly differs from the usual particle-particle interactions in physics, as it is retarded in time. A prominent platform for realising this kind of interaction are photon Bose–Einstein condensates, which are created in dye-filled microcavities. The dye solution continually absorbs and re-emits these photons, causing the photon gas to thermalize and to form a Bose–Einstein condensate. Because of a non-ideal quantum efficiency, these cycles heat the dye solution, creating a medium that provides an effective thermo-optic photon–photon interaction. So far, only a mean-field description of this process exists. This paper goes beyond by working out a quantum mechanical description of the effective thermo-optic photon–photon interaction. To this end, the self-consistent modelling of the temperature diffusion builds the backbone of the modelling. Furthermore, the manyfold experimental timescales allow for deriving an approximate Hamiltonian. The resulting quantum theory is applied in the perturbative regime to both a harmonic and a box potential for investigating its prospect for precise measurements of the effective photon–photon interaction strength.
Although photon Bose–Einstein condensates have already been used for studying many interesting effects, the precise role of the photon–photon interaction is not fully clarified up to now. In view of this, it is advantageous that these systems allow measuring both the intensity of the light leaking out of the cavity and its spectrum at the same time. Therefore, the photon–photon interaction strength can be determined once via analysing the condensate broadening and once via examining the interaction-induced modifications of the cavity modes. As the former method depends crucially on the concrete shape of the trapping potential and the spatial resolution of the used camera, interferometric methods promise more precise measurements. To this end, the present paper works out the impact of the photon–photon interaction upon the cavity modes. A quantum mechanical description of the photon–photon interaction, including the thermal cloud, builds the theoretical backbone of the method. An exact diagonalisation approach introduced here exposes how the effective photon–photon interaction modifies both the spectrum and the width of the photon gas. A comparison with a variational approach based on the Gross–Pitaevskii equation quantifies the contribution of the thermal cloud in the respective applications.
Surface roughness plays a critical role and has effects in, e.g. fluid dynamics or contact mechanics. For example, to evaluate fluid behavior at different roughness properties, real-world or numerical experiments are performed. Numerical simulations of rough surfaces can speed up these studies because they can help collect more relevant information. However, it is hard to simulate rough surfaces with deterministic or structured components in current methods. In this work, we present a novel approach to simulate rough surfaces with a Gaussian process (GP) and a noise model because GPs can model structured and periodic elements. GPs generalize traditional methods and are not restricted to stationarity so they can simulate a wider range of rough surfaces. In this paper, we summarize the theoretical similarities of GPs with auto-regressive moving-average processes and introduce a linear process view of GPs. We also show examples of ground and honed surfaces simulated by a predefined model. The proposed method can also be used to fit a model to measurement data of a rough surface. In particular, we demonstrate this to model turned profiles and surfaces that are inherently periodic.
An important tool for the functional characterization of technical surfaces are envelope estimation techniques. This paper describes a new method for generating profile envelope lines based on a simplified beam-surface contact model with intuitive parameterization. The method is closely related to spline filters and shares some of their positive characteristics such as smoothness and robustness against isolated outliers. Unlike spline filters, the proposed method does not calculate mean lines, but envelope lines. Several examples of calculated profile envelopes of sintered surfaces are shown and a comparison with morphological methods, the state-of-the-art method for envelope estimation, is presented.
The Born–Fock theorem is one of the most fundamental theorems of quantum mechanics and forms the basis for reliable and efficient navigation in the Hilbert space of a quantum system with a time-dependent Hamiltonian by adiabatic evolution. In the absence of level crossings, i.e. without degeneracies, and under adiabatic time evolution all eigenstates of the Hamiltonian keep their energetic order, labeled by a conserved integer quantum number. Thus, controlling the eigenstates of the Hamiltonian and their energetic order in asymptotic limits allows one to engineer a perfect adiabatic transfer between a large number of initial and target states. The fidelity of the state transfer is only limited by adiabaticity and the selection of target states is controlled by the integer invariant labeling the order of eigenstates. We show here, for the example of a finite superlattice Wannier-Stark ladder, i.e. a one-dimensional lattice with alternating hopping amplitudes and constant potential gradient, that such an adiabatic control of eigenstates can be used to induce perfectly quantized single-particle transport across a pre-determined number of lattice sites. We dedicate this paper to the memory of our late friend and colleague Bruce Shore, who was an expert in adiabatic processes and taught us much about this field.
Dynamical change under slowly changing conditions: the quantum Kruskal–Neishtadt–Henrard theorem
(2022)
Adiabatic approximations break down classically when a constant-energy contour splits into separate contours, forcing the system to choose which daughter contour to follow; the choices often represent qualitatively different behavior, so that slowly changing conditions induce a sudden and drastic change in dynamics. The Kruskal–Neishtadt–Henrard (KNH) theorem relates the probability of each choice to the rates at which the phase space areas enclosed by the different contours are changing. This represents a connection within closed-system mechanics, and without dynamical chaos, between spontaneous change and increase in phase space measure, as required by the Second Law of Thermodynamics. Quantum mechanically, in contrast, dynamical tunneling allows adiabaticity to persist, for very slow parameter change, through a classical splitting of energy contours; the classical and adiabatic limits fail to commute. Here we show that a quantum form of the KNH theorem holds nonetheless, due to unitarity.
Experimental observation of a dissipative phase transition in a multi-mode many-body quantum system
(2022)
Dissipative phase transitions are a characteristic feature of open systems. One of the paradigmatic examples for a first order dissipative phase transition is the driven nonlinear single-mode optical resonator. In this work, we study a realization with an ultracold bosonic quantum gas, which generalizes the single-mode system to many modes and stronger interactions. We measure the effective Liouvillian gap of the system and find evidence for a first order dissipative phase transition. Due to the multi-mode nature of the system, the microscopic dynamics is much richer and allows us to identify a non-equilibrium condensation process.
Individual quantum emitters form a fundamental building block for emerging quantum technologies. Collective effects of emitters, such as superradiance, might improve the performance of applications even further. When scaling materials to larger sizes, however, the optical density of states is modified by the surrounding material, and the collective coupling in small domains might be covered by transitions to bulk properties due to the presence of multiple collectively emitting domains, which inhomogeneously add. Here, we probe the optical properties of nitrogen vacancy centers in agglomerates of nanodiamonds. We quantify the transition from individual emitters to bulk emission by fluorescence lifetime measurements, and find a transition to occur on a length scale of \(\sim \!3\) wavelengths around the emitter. While our lifetime measurements are consistent with superradiant decay, the second-order correlation function, which is a standard measure to reveal collective properties, fails to probe collective effects for our case of an ensemble of collectively contributing domains to the emission. Therefore, we propose and apply a new measure to trace collective effects based on the intensity fluctuations of the emitted light. Our work points toward systematically studying collective effects in a scalable solid-state quantum system, and using them for quantum optical applications in agglomerates of highly-doped nanodiamonds.
Within this paper, electro-mechanical long-term tests on a thrust bearing were presented. The effects of an additional electrical load on the bearing raceways and the used lubricant were investigated. Chemical investigations and viscosity measurements were presented, which show the changes in the lubricant. These investigations were compared with the electrical loads and the occurring raceway damage. In addition, a comparison was made with mechanical reference tests. This procedure makes it possible to classify the changes that occur due to the electrical load and to distinguish the effects from each other. The background to these investigations is the increased occurrence of parasitic currents in electric motors, which can lead to damage to machine elements. The phenomena that occur here are new challenges in the development of drive trains
Mousavion, Sina ; Yu, Ka Man ; Maniraj, Mahalingam ; Lyu, Lu ; Knippertz, Johannes ; Stadtmüller, Benjamin ; Aeschlimann, Martin
Surface alloys are a highly flexible 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 distinct binary rare-earth-noble metals (NM) surface alloys by employing scanning tunneling microscopy and low energy electron diffraction. Using Dysprosium as the guest element on fcc(111) NM substrates, we identify the formation of non-commensurate surface alloy superstructures, which lead to homogeneous moiré patterns for DyCu2/Cu(111) and DyAu2/Au(111), while an inhomogeneous one is found for DyAg2/Ag(111). The local structure was analyzed for these samples 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 DyAg2 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, which occur likely to relieve the in-plane strain within the DyAg2 surface alloy layer. Our findings clearly demonstrate that surface alloying is an intriguing tool to tailor the local atomic structure as well as the mesoscopic moiré structures of metallic heterostructures.
Spin transport and spin dynamics after femtosecond laser pulse irradiation of iron (Fe) are studied using a kinetic Monte Carlo model. This model simulates spin dependent dynamics by taking into account two interaction processes during nonequilibrium: elastic electron–lattice scattering, where only the direction of the excited electrons changes, and inelastic electron–electron scattering processes, where secondary electrons are generated. An analysis of the spin dependent particle kinetics inside the material shows that a smaller elastic scattering time leads to a larger spatial spread of electrons in the material, whereas generation of secondary electrons extends the time span for superdiffusive transport and increases the spin current density.
Since the advent of experiments with photon Bose–Einstein condensates (phBECs) in dye-filled microcavities in 2010, many investigations have focussed upon the emerging effective photon–photon interaction. Despite its smallness, it can be identified to stem from two physically distinct mechanisms. On the one hand, a Kerr nonlinearity of the dye medium yields a photon–photon contact interaction. On the other hand, a heating of the dye medium leads to an additional thermo-optic interaction, which is both delayed and non-local. The latter turns out to represent the leading contribution to the effective interaction for the current 2D experiments. Here we analyse theoretically how the effective photon–photon interaction increases when the system dimension is reduced from 2D to 1D. To this end, we consider an anisotropic harmonic trapping potential and determine via a variational approach how the properties of the phBEC in general, and both aforementioned interaction mechanisms in particular, change with increasing anisotropy. We find that the thermo-optic interaction strength increases at first linearly with the trap aspect ratio and later on saturates at a certain value of the trap aspect ratio. Furthermore, in the strong 1D limit the roles of both interactions get reversed as the thermo-optic interaction remains saturated and the contact Kerr interaction becomes the leading interaction mechanism. Finally, we discuss how the predicted effects can be measured experimentally.
Photon Bose–Einstein condensates are characterised by a quite weak interaction, so they behave nearly as an ideal Bose gas. Moreover, since the current experiments are conducted in a microcavity, the longitudinal motion is frozen out and the photon gas represents effectively a two-dimensional trapped gas of massive bosons. In this paper we focus on a harmonically confined ideal Bose gas in two dimensions, where the anisotropy of the confinement allows for a dimensional crossover. If the confinement in one direction is strong enough so that this squeezed direction is frozen out, then only one degree of freedom survives and the system can be considered to be quasi-one dimensional. In view of an experimental set-up we work out analytically the thermodynamic properties for such a system with a finite number of photons. In particular, we focus on examining the dimensional information which is contained in the respective thermodynamic quantities.
Ohler, Simon ; Kiefer-Emmanouilidis, Maximilian ; Browaeys, Antoine ; Büchler, Hans Peter ; Fleischhauer, Michael
As shown in recent experiments (Lienhard et al 2020 Phys. Rev. X 10 021031), spin–orbit coupling in systems of Rydberg atoms can give rise to density-dependent Peierls phases in second-order hoppings of Rydberg spin excitations and nearest-neighbor repulsion. We here study theoretically a one-dimensional zig-zag ladder system of such spin–orbit coupled Rydberg atoms at half filling. The second-order hopping is shown to be associated with an effective gauge field, which in mean-field approximation is static and homogeneous. Beyond the mean-field level the gauge potential attains a transverse quantum component whose amplitude is dynamical and linked to density modulations. We here study the effects of this to the possible ground-state phases of the system. In a phase where strong repulsion leads to a density wave, we find that as a consequence of the induced quantum gauge field a regular pattern of current vortices is formed. However also in the absence of density–density interactions the quantum gauge field attains a non-vanishing amplitude. Above a certain critical strength of the second-order hopping the energy gain due to gauge-field induced transport overcomes the energy cost from the associated build-up of density modulations leading to a spontaneous generation of the quantum gauge field.
Fries, Daniela Veronika ; Klein, Matthias P. ; Straßner, Annika ; Huber, Maximilian ; Luczak, Maximilian ; Wiehn, Christopher ; Niedner-Schatteburg, Gereon
We investigate small tantalum clusters Tan+, n = 2–4, for their capability to cleave N2 adsorption spontaneously. We utilize infrared photon dissociation (IR-PD) spectroscopy of isolated and size selected clusters under cryogenic conditions within a buffer gas filled ion trap, and we augment our experiments by quantum chemical simulations (at DFT level). All Tan+ clusters, n = 2–4, seem to cleave N2 efficiently. We confirm and extend a previous study under ambient conditions on Ta2+ cluster [Geng et al., Proc. Natl. Acad. Sci. U. S. A. 115, 11680–11687 (2018)]. Our cryo studies and the concomitant DFT simulations of the tantalum trimer Ta3+ suggest cleavage of the first and activation of the second and third N2 molecule across surmountable barriers and along much-involved multidimensional reaction paths. We unravel the underlying reaction processes and the intermediates involved. The study of the N2 adsorbate complexes of Ta4+ presented here extends our earlier study and previously published spectra from (4,m), m = 1–5 [Fries et al., Phys. Chem. Chem. Phys. 23(19), 11345–11354 (2021)], up to m = 12. We confirm the priory published double activation and nitride formation, succeeded by single side-on N2 coordination. Significant red shifts of IR-PD bands from these side-on coordinated μ2-κN:κN,N N2 ligands correlate with the degree of tilting towards the second coordinating Ta center. All subsequently attaching N2 adsorbates onto Ta4+ coordinate in an end-on fashion, and we find clear evidence for co-existence of end-on coordination isomers. The study of stepwise N2 adsorption revealed adsorption limits m(max) of [Tan(N2)m]+ which increase with n, and kinetic fits revealed significant N2 desorption rates upon higher N2 loads. The enhanced absolute rate constants of the very first adsorbate steps kabs(n,0) of the small Ta3+ and Ta4+ clusters independently suggest dissociative N2 adsorption and likely N2 cleavage into Ta nitrides.
Fries, Daniela Veronika ; Klein, Matthias P. ; Straßner, Annika ; Huber, Maximilian ; Niedner-Schatteburg, Gereon
We present an IR-PD study of tantalum cluster adsorbate complexes [Tan(N2)m]+, abbreviated (n,m), n = 5–8. We utilize infrared spectroscopy of isolated and size selected clusters as prepared and characterized by a cryogenic tandem ion trap setup, and we augment our experiments with quantum chemical simulations at the level of density functional theory. The cluster adsorbate complexes (n,m) reveal vibrational bands above 2000 cm−1, which indicate end-on coordinated μ1-N2 oscillators, and bands below 2000 cm−1, which indicate side-on μ2-κN:κN,N coordinated ones. We observe a general increase in spectral complexity and an inhomogeneous broadening, mainly towards the red, at certain points of N2 loading m, which originates from an increasingly higher amount of double and triple N2 coordination at Ta sites, eventually at all of them. Other than the small tantalum clusters Tan+, n = 2–4, the IR-PD spectra of the initial N2 adsorbate species (n,1), n = 5–8, provide strong evidence for a lack of spontaneous N2 cleavage. Spontaneous N2 cleavage by Tan+, n = 5–8, seems suppressed. Therefore, the ability of a small Ta cluster to cleave dinitrogen disappears with one more tantalum core atom. The study of stepwise N2 adsorption on size selected Tan+, n = 5–8 clusters revealed adsorption limits m(max) of [Tan(N2)m]+ that are independent of cluster size within this size range. Cryo-adsorption kinetics at 26 K allowed for kinetic fits to consecutive N2 adsorption steps, and the fits revealed significant N2 desorption rates upon higher N2 loads, and the cluster adsorbate complexes eventually reached equilibrium. Some enhanced N2 desorption rates point towards likely adsorbate shell reorganization, and there is also some evidence for the coexistence of isomeric cluster adsorbate complexes.
Koujok, Abbas ; Riveros, Alejandro ; Rodrigues, Davi R. ; Finocchio, Giovanni ; Weiler, Mathias ; Hamadeh, Abbass ; Pirro, Philipp
Finding new energy-efficient methods for exciting magnetization dynamics is one of the key challenges in magnonics. In this work, we present an approach to excite the gyrotropic dynamics of magnetic vortices through the phenomenon of inverse magnetostriction, also known as the Villari effect. We develop an analytical model based on the Thiele formalism that describes the gyrotropic motion of the vortex core including the energy contributions due to inverse magnetostriction. Based on this model, we predict excitations of the vortex core resonances by surface acoustic waves whose frequency is resonant with the frequency of the vortex core. We verify the model's prediction using micromagnetic simulations and show the dependence of the vortex core's oscillation radius on the surface acoustic wave amplitude and the static bias field. Our study contributes to the advancement of energy-efficient magnetic excitations by relying on voltage-induced driven dynamics, which is an alternative to conventional current-induced excitations.
Wolff, Alexander ; Franke, Lars ; Klingel, Steffen ; Krieger, Janis ; Müller, Lukas ; Stemler, Ralf ; Rahm, Marco
Varactor diodes have been proposed as active tuning elements of reconfigurable metasurfaces in the Ka-band. However, their experimental realization in this frequency range has not been demonstrated yet. We report the implementation of such a reconfigurable intelligent surface (RIS) made of 20 × 20 unit cells. By active tuning of the bias voltage of the varactors, the phase of the backward diffracted wave can be continuously tuned between 0 ° and 180 °. Thus, the phase tuning can be independently controlled for each unit cell. The frequency working range of the RIS is 1.1 GHz (from 30.6 to 31.7 GHz). As an illustration of the practical use, we demonstrate continuous beam steering of microwave radiation at 31 GHz in a defined propagation plane.
Rapid-prototyping of microscopic thermal landscapes in Brillouin light scattering spectroscopy
(2023)
Schweizer, Matthias R. ; Kühn, Franziska ; Koster, Malte ; Freymann, Georg von ; Hillebrands, Burkard ; Serga, Alexander A.
Since temperature and its spatial, and temporal variations affect a wide range of physical properties of material systems, they can be used to create reconfigurable spatial structures of various types in physical and biological objects. This paper presents an experimental optical setup for creating tunable two-dimensional temperature patterns on a micrometer scale. As an example of its practical application, we have produced temperature-induced magnetization landscapes in ferrimagnetic yttrium iron garnet films and investigated them using micro-focused Brillouin light scattering spectroscopy. It is shown that, due to the temperature dependence of the magnon spectrum, spatial temperature distributions can be visualized even for microscale thermal patterns.
The concept of building logically functional networks employing spintronics or magnetic heterostructures is becoming more and more popular today. Incorporating logical segments into a circuit needs physical bonds between the magnetic molecules or clusters involved. In this framework, we systematically study ultrafast laser-induced spin-manipulation scenarios on a closed system of three carbon chains to which three Ni atoms are attached. After the inclusion of spin–orbit coupling and an external magnetic field, different ultrafast spin dynamics scenarios involving spin-flip and long-distance spin-transfer processes are achieved by various appropriately well-tailored time-resolved laser pulses within subpicosecond timescales. We additionally study the various effects of an external magnetic field on spin-flip and spin-transfer processes. Moreover, we obtain spin-dynamics processes induced by a double laser pulse, rather than a single one. We suggest enhancing the spatial addressability of spin-flip and spin-transfer processes. The findings presented in this article will improve our knowledge of the magnetic properties of carbon-based magnetic molecular structures. They also support the relevant experimental realization of spin dynamics and their potential applications in future molecular spintronics devices.
Mass transfer through fluid interfaces is an important phenomenon in industrial applications as well as in naturally occurring processes. In this work, we investigate the mass transfer across vapor–liquid interfaces in binary mixtures using molecular dynamics simulations. We investigate the influence of interfacial properties on mass transfer by studying three binary azeotropic mixtures known to have different interfacial behaviors. Emphasis is placed on the effect of the intermolecular interactions by choosing mixtures with the same pure components but different cross-interactions such that different azeotropic behaviors are obtained. The molar flux is created by utilizing a non-stationary molecular dynamics simulation approach, where particles of one component are inserted into the vapor phase over a short period of time before the system’s response to this insertion is monitored. From a direct comparison of the density profiles and the flux profiles in close proximity to the interface, we analyze the particles’ tendency to accumulate in the interfacial region throughout the different stages of the simulation. We find that for mixtures with strong attractive cross-interactions, the inserted particles are efficiently transported into the liquid phase. For systems with weak attractive cross-interactions, the inserted particles show a tendency to accumulate in the interfacial region, and the flux through the system is lower. The results from this work indicate that the accumulation of particles at the interface can act as a hindrance to mass transfer, which has practical relevance in technical processes.
Briones, Johan ; Weber, Marius ; Stadtmüller, Benjamin ; Schneider, Hans Christian ; Rethfeld, Bärbel
This paper is concerned with a theoretical analysis of the behavior of optically excited spin currents in bilayer and multilayer systems of ferromagnetic and normal metals. As the propagation, control, and manipulation of the spin currents created in ferromagnets by femtosecond optical pulses is of particular interest, we examine the influence of different thicknesses of the constituent layers for the case of electrons excited several electronvolts above the Fermi level. Using a Monte-Carlo simulation framework for such highly excited electrons, we first examine the spatiotemporal characteristics of the spin current density driven in a Fe layer, where the absorption profile of the light pulse plays an important role. Further, we examine how the combination of light absorption profile, spin-dependent transmission probabilities, and iron layer thickness affects spin current density in a Fe/Au bilayer system. For high-energy electrons studied here, the interface and secondary electron generation have a small influence on spin transport in the bilayer system. However, we find that spin injection from one layer to another is most effective within a certain range of iron layer thicknesses.
Colloidal nanorods based on CdS or CdSe, functionalized with metal particles, have proven to be efficient catalysts for light-driven hydrogen evolution. Seeded CdSe@CdS nanorods have shown increasing performance with increasing rod length. This observation was rationalized by the increasing lifetime of the separated charges, as a large distance between holes localized in the CdSe seed and electrons localized at the metal tip decreases their recombination rate. However, the impact of nanorod length on the electron-to-tip localization efficiency or pathway remained an open question. Therefore, we investigated the photo-induced electron transfer to the metal in a series of Ni-tipped CdSe@CdS nanorods with varying length. We find that the transfer processes occurring from the region close to the semiconductor–metal interface, the rod region, and the CdSe seed region depend in different ways on the rods’ length. The rate of the fastest process from excitonic states generated directly at the interface is independent of the rod length, but the relative amplitude decreases with increasing rod length, as the weight of the interface region is decreasing. The transfer of electrons to the metal tip from excitons generated in the CdS rod region depends strongly on the length of the nanorods, which indicates an electron transport-limited process, i.e., electron diffusion toward the interface region, followed by fast interface crossing. The transfer originating from the CdSe excitonic states again shows no significant length dependence in its time constant, as it is probably limited by the rate of overcoming the shallow confinement in the CdSe seed.
A set of molecular models for the alkali nitrates (LiNO3, NaNO3, KNO3, RbNO3, and CsNO3) in aqueous solutions is presented and used for predicting the thermophysical properties of these solutions with molecular dynamics simulations. The set of models is obtained from a combination of a model for the nitrate anion from the literature with a set of models for the alkali cations developed in previous works of our group. The water model is SPC/E and the Lorentz–Berthelot combining rules are used for describing the unlike interactions. This combination is shown to yield fair predictions of thermophysical and structural properties of the studied aqueous solutions, namely the density, the water activity and the mean ionic activity coefficient, the self-diffusion coefficients of the ions, and radial distribution functions, which were studied at 298 K and 1 bar; except for the density of the solutions of all five nitrates and the activity properties of solutions of NaNO3, which were also studied at 333 K. For calculating the water the activity and the mean ionic activity coefficient, the OPAS (osmotic pressure for the activity of selvents) method was applied. The new models extend an ion model family for the alkali halides developed in previous works of our group in a consistent way.
Hamadeh, Abbass ; Breitbach, David ; Ender, Milan ; Mohseni, Morteza ; Kohl, Felix ; Maskill, Jan ; Bechberger, Moritz ; Pirro, Philipp
We propose a hybrid magnonic-oscillator system based on the combination of a spin transfer auto-oscillator and a magnonic waveguide to open new perspectives for spin-wave based circuits. The system is composed of a spin transfer oscillator based on a vortex state which is dipolarly coupled to a nanoscale spin-wave waveguide with longitudinal magnetization. In its auto-oscillating regime, the oscillator emits coherent spin waves with tunable and controllable frequencies, directions, and amplitudes into the waveguide. We demonstrate the principle of this method using micromagnetic simulations and show that reconfiguration of the system is possible by changing the chirality and polarity of the magnetic vortex. Spin waves are emitted into the waveguide with high non-reciprocity and the preferred direction depends on the core polarity of the vortex. In contrast, different vortex chiralities lead to different amplitudes of the emitted waves. Our findings open up a novel way to design an agile spintronic device for the coherent and tunable generation of propagating spin waves.
Confinement of Bose–Einstein magnon condensates in adjustable complex magnetization landscapes
(2022)
Schweizer, Matthias R. ; Kreil, Alexander J. E. ; Freymann, Georg von ; Hillebrands, Burkard ; Serga, Alexander A.
Coherent wave states such as Bose–Einstein condensates (BECs), which spontaneously form in an overpopulated magnon gas even at room temperature, have considerable potential for wave-based computing and information processing at microwave frequencies. The ability to control the transport properties of magnon BECs plays an essential role in their practical use. Here, we demonstrate the spatiotemporal control of the BEC density distribution through the excitation of magnon supercurrents in an inhomogeneously magnetized yttrium iron garnet film. The BEC is created by microwave parametric pumping and probed by Brillouin light scattering spectroscopy. The desired magnetization profile is prepared by heating the film with optical patterns projected onto its surface using a phase-based wavefront modulation technique. Specifically, we observe a pronounced spatially localized magnon accumulation caused by magnon supercurrents flowing toward each other originating in two heated regions. This accumulation effect increases the BEC lifetime due to the constant influx of condensed magnons into the confinement region. The shown approach to manipulate coherent waves provides an opportunity to extend the lifetime of freely evolving magnon BECs, create dynamic magnon textures, and study the interaction of magnon condensates formed in different regions of the sample.
We present a robust, fiber-based endoscope with a silver direct-laser-written structure for radio frequency (RF) emission next to the optical fiber facet. Thereby, we are able to excite and probe a sample, such as nitrogen-vacancy (NV) centers in diamond, with RF and optical signals simultaneously and specifically measure the fluorescence of the sample fully through the fiber. At our targeted frequency range of around 2.9 GHz, the facet of the fiber core is in the near-field of the RF-guiding silver structure, which comes with the advantage of an optimal RF intensity decreasing rapidly with the distance. By creating a silver structure on the cladding of the optical fiber, we achieve the minimal possible distance between an optically excited and detected sample and an antenna structure without affecting the optical performance of the fiber. This allows us to realize a high RF amplitude at the sample’s position when considering an endoscope solution with integrated optical and RF access. The capabilities of the endoscope are quantified by optically detected magnetic resonance (ODMR) measurements of an NV-doped microdiamond that we probe as a practical use case. We demonstrate a magnetic sensitivity of our device of 17.8 nT/Hz when measuring the ODMR exclusively through our fiber and compare the sensitivity to a measurement using a confocal microscope. Moreover, the application of our device is not limited to NV centers in diamonds. Similar endoscope-like devices combining optical excitation and detection with radio frequency or microwave antenna could be used as a powerful tool for measuring a variety of fluorescent particles that have so far only been investigated with bulky and large optical setups. Furthermore, our endoscope points toward precise distance measurements based on Rabi oscillations.
Schlafschwierigkeiten und Insomnie stellen ein gesellschaftlich zunehmendes Phänomen dar. Studierende sind hiervon überdurchschnittlich häufig betroffen, mehr als ein Drittel beklagt eine niedrige Schlafqualität. In diesem Kontext erwiesen sich vor allem achtsamkeitsbasierte Interventionen als hilfreich. Wirksame, neuere Forschungsansätze widmen sich der Untersuchung mobiler Gesundheitsanwendungen. Daran anknüpfend setzt sich die Studie zum Ziel, die Effektivität einer achtsamkeitsbasierten Intervention mittels Meditations-App („7Mind“) in Bezug auf Schlafschwierigkeiten zu evaluieren. Studierende wurden randomisiert der Treatment- oder Wartelisten-Kontrollgruppe zugeordnet. Baseline-Messung, Post-Messung (2 Wochen) und Follow-up-Messung (4 Wochen) wurden mit Selbstberichtfragebogen zu den Variablen Schlafqualität, Insomnie-Schweregrad, Achtsamkeit, Tagesmüdigkeit, Stress und Lebensqualität untersucht. Die Intervention sollte 14 Tage 20 Minuten täglich absolviert werden. Von 53 Studierenden mit Baseline-Messung füllten 35 die Post-Messung und 28 alle Messzeitpunkte aus. Im Anschluss an das Training zeigten sich zwischen den Gruppen signifikante Unterschiede bezüglich der Schlafparameter (p < .001), wohingegen die Achtsamkeit unverändert blieb. Dafür wies letztere eine signifikante Zeit x Gruppe Interaktion auf (p = .018). In Bezug auf den Schlaf ergaben sich hohe Effektstärken, welche auch zum Follow-up-Zeitpunkt persistierten (d= 2.36). Die Variablen Tagesmüdigkeit,
Stress und Lebensqualität waren hochsignifikant mit der Schlafqualität korreliert (p < .001).
Mobile achtsamkeitsbasierte Interventionen stellen eine ökonomische Alternative dar, um Studierende mit Schlafschwierigkeiten zu unterstützen. Zukünftige Schritte inkludieren die Überprüfung über einen längeren Zeitraum und mit einer größeren Reichweite.
Interfacial properties of binary azeotropic mixtures of Lennard-Jones truncated and shifted fluids were studied by molecular dynamics (MD) simulation and density gradient theory (DGT) in combination with an equation of state. Three binary mixtures were investigated, which differ in the energetic cross interaction parameter that yields different types of azeotropic behavior. This study covers a wide temperature and composition range. Mixture A exhibits a heteroazeotrope at low temperatures, which changes to a low-boiling azeotrope at high temperatures, mixture B exhibits a low-boiling azeotrope, and mixture C exhibits a high-boiling azeotrope. The phase behavior and fluid interfacial properties as well as their relation were studied. Vapor–liquid, liquid–liquid, and vapor–liquid–liquid equilibria and interfaces were considered. Density profiles, the surface tension, the interfacial thickness, as well as the relative adsorption and enrichment of the components at the interface were studied. The results obtained from the two independent methods (MD and DGT) are overall in good agreement. The results provide insights into the relation of the phase behavior, particularly the azeotropic behavior, of simple fluid mixtures and the corresponding interfacial properties. Strong enrichment was found for the mixture with a heteroazeotrope in the vicinity of the three-phase equilibrium, which is related to a wetting transition.
Geilen, Moritz ; Nicoloiu, Alexandra ; Narducci, Daniele ; Mohseni, Morteza ; Bechberger, Moritz ; Ender, Milan ; Ciubotaru, Florin ; Hillebrands, Burkard ; Müller, Alexandru ; Adelmann, Christoph ; Pirro, Philipp
We report on the resonant excitation of spin waves in micro-structured magnetic thin films by short-wavelength surface acoustic waves (SAWs). The spin waves as well as the acoustic waves are studied by micro-focused Brillouin light scattering spectroscopy. At low magnetic bias fields, a resonant phonon–magnon conversion is possible, which results in the excitation of short-wavelength spin waves. Using micromagnetic simulations, we verify that during this excitation both energy and linear momentum are conserved and fully transferred from the SAW to the spin wave. This conversion can already be detected after an interaction length of a few micrometers. Thus, our findings pave the way for miniaturized magneto-elastic spin-wave emitters for magnon computing.
We study the influence of transport effects on time- and space-resolved magnetization dynamics in a laser-excited thick nickel film. We explicitly include diffusive heat transport and spin-resolved charge transport as well as Seebeck and Peltier effects and calculate the dynamics of spin-dependent electronic temperatures, chemical potentials, lattice temperatures, and magnetization. We find that transport has an influence on the magnetization dynamics closer to the excited surface as well as in regions deeper than the penetration depth of the laser. We reveal that, for higher absorbed fluences and in the presence of transport, thick magnetic films show a quenching time nearly independent of depth, though the magnitude of quenching is depth-dependent.
We investigate ultrafast spin dynamics due to exchange, electron–phonon and Elliott–Yafet spin-flip scattering in a model with a simple band structure and ferromagnetically coupled electronic sublattices (or more generally, subsystems). We show that this incoherent model of electronic dynamics leads to sublattice magnetization changes in opposite directions after ultrashort-pulse excitation. This prominent feature on an ultrafast timescale is related to a transfer of energy and angular momentum between the subsystems due to exchange scattering. Our calculations illustrate a possible incoherent mechanism that works in addition to the coherent optically induced spin transfer mechanism.
Böttcher, Tobias ; Ruhwedel, Moritz ; Levchenko, Khrystyna O. ; Wang, Qi ; Chumak, Hryhorii Leonidovych ; Popov, Maksym A. ; Zavislyak, Igor V. ; Dubs, Carsten ; Surzhenko, Oleksii ; Hillebrands, Burkard ; Chumak, Andrii V. ; Pirro, Philipp
Spin waves in yttrium iron garnet (YIG) nano-structures attract increasing attention from the perspective of novel magnon-based data processing applications. For short wavelengths needed in small-scale devices, the group velocity is directly proportional to the spin-wave exchange stiffness constant λex. Using wave vector resolved Brillouin light scattering spectroscopy, we directly measure λex in Ga-substituted YIG thin films and show that it is about three times larger than for pure YIG. Consequently, the spin-wave group velocity overcomes the one in pure YIG for wavenumbers k > 4 rad/μm, and the ratio between the velocities reaches a constant value of around 3.4 for all k > 20 rad/μm. As revealed by vibrating-sample magnetometry and ferromagnetic resonance spectroscopy, Ga:YIG films with thicknesses down to 59 nm have a low Gilbert damping (α<10−3), a decreased saturation magnetization μ0MS≈20 mT, and a pronounced out-of-plane uniaxial anisotropy of about μ0Hu1≈95 mT, which leads to an out-of-plane easy axis. Thus, Ga:YIG opens access to fast and isotropic spin-wave transport for all wavelengths in nano-scale systems independently of dipolar effects.
In this work, we present a method to microscopically investigate the liquid–vapor interfaces on the bottom side of droplets, which were placed on superhydrophobic structures, so that wetting in the Cassie–Baxter (CB) state occurred. These interfaces are hard to access optically, especially when an opaque substrate material is used, which is usually the case for technical applications. In that case, the menisci have to be observed through the droplet, which substantially deteriorates the imaging quality. Other methods that circumvent these distortions, such as optical coherence tomography, are restricted to a resolution of several micrometers. Confocal or fluorescence microscopy additionally requires a transparent substrate. To measure the liquid–vapor interfaces formed in the Cassie–Baxter state with high accuracy liquid droplets of a monomer solution that chemically reacts to form the elastomer, polydimethylsiloxane was placed on structured surfaces. Because double reentrant structures were used, wetting occurred in the Cassie–Baxter state despite the low surface tension of the monomer solution. After curing, it was possible to remove the solid droplets from the surface and investigate them using confocal microscopy, which provides an excellent height resolution of 10 nm. Test structures such as arrays of stripes and holes with variable spacing or diameter were used to investigate the impact of their geometry on the liquid–vapor interfaces formed in the CB state. Although the maximum height of the menisci on the droplet's bottom side is in the region of several 10 μm, the 10 nm resolution is required to adequately compare their topography with simplified theoretical models.
Stiehl, Martin ; Weber, Marius ; Seibel, Christopher ; Hoefer, Jonas ; Weber, Sebastian T. ; Nenno, Dennis M. ; Schneider, Hans Christian ; Rethfeld, Baerbel ; Stadtmüller, Benjamin ; Aeschlimann, Martin
The magnetic response of a ferromagnet after an ultrafast optical excitation can be connected to the underlying electronic dynamics either via primary excitation processes during the laser pulse or via secondary collision processes. In the latter case, the information on the details of the excitation is lost and, therefore, the electron dynamics can be described using quasi-equilibrium concepts. In this work, we study the effect of the pump photon energy on the ultrafast demagnetization dynamics in ferromagnetic nickel. We find that the magnetization dynamics for similar absorbed energies for a range of pump photon energies are almost identical and depend only on the absorbed energy. This is in stark contrast to characteristic differences in the optically excited electronic distributions, as calculated from the band structure. In addition, the measured fluence-dependent dynamics can be reproduced with a model based on local temperatures. These findings indicate that it is mainly secondary processes that are responsible for the observed demagnetization dynamics.
Straßner, Annika ; Klein, Matthias P. ; Fries, Daniela V. ; Wiehn, Christopher ; Huber, Maximilian E. ; Mohrbach, Jennifer ; Dillinger, Sebastian ; Spelsberg, Dirk ; Armentrout, Peter B. ; Niedner-Schatteburg, Gereon
We present a study of stepwise cryogenic N2 adsorption on size-selected Fen+ (n = 8–20) clusters within a hexapole collision cell held at T = 21–28 K. The stoichiometries of the observed adsorption limits and the kinetic fits of stepwise N2 uptake reveal cluster size-dependent variations that characterize four structural regions. Exploratory density functional theory studies support tentative structural assignment in terms of icosahedral, hexagonal antiprismatic, and closely packed structural motifs. There are three particularly noteworthy cases, Fe13+ with a peculiar metastable adsorption limit, Fe17+ with unprecedented nitrogen phobia (inefficient N2 adsorption), and Fe18+ with an isomeric mixture that undergoes relaxation upon considerable N2 uptake.
Cryo infrared spectroscopy of N2 adsorption onto bimetallic rhodium–iron clusters in isolation
(2021)
Klein, Matthias P. ; Erhard, Amelie A. ; Huber, Maximilian E. ; Straßner, Annika ; Fries, Daniela V. ; Dillinger, Sebastian ; Mohrbach, Jennifer ; Niedner-Schatteburg, Gereon
We investigated the N2 adsorption behavior of bimetallic rhodium–iron cluster cations [RhiFej(N2)m]+ by means of InfraRed MultiplePhotoDissociation (IR-MPD) spectroscopy in comparison with density functional theory (DFT) modeling. This approach allows us to refine our kinetic results [Ehrhard et al., J. Chem. Phys. (in press)] to enhance our conclusions. We focus on a selection of cluster adsorbate complexes within the ranges of i = j = 3–8 and m = 1–10. For i = j = 3, 4, DFT suggests alloy structures in the case of i = j = 4 of high (D2d) symmetry: Rh–Fe bonds are preferred instead of Fe–Fe bonds or Rh–Rh bonds. N2 adsorption and IR-MPD studies reveal strong evidence for preferential adsorption to Rh sites and mere secondary adsorption to Fe. In some cases, we observe adsorption isomers. With the help of modeling the cluster adsorbate complex [Rh3Fe3(N2)7]+, we find clear evidence that the position of IR bands allows for an element specific assignment of an adsorption site. We transfer these findings to the [Rh4Fe4(N2)m]+ cluster adsorbate complex where the first four N2 molecules are exclusively adsorbed to the Rh atoms. The spectra of the larger adsorbates reveal N2 adsorption onto the Fe atoms. Thus, the spectroscopic findings are well interpreted for the smaller clusters in terms of computed structures, and both compare well to those of our accompanying kinetic study [Ehrhard et al., J. Chem. Phys. (in press)]. In contrast to our previous studies of bare rhodium clusters, the present investigations do not provide any indication for a spin quench in [RhiFej(N2)m]+ upon stepwise N2 adsorption.
Many amphibians and insects have a biphasic life cycle, linking aquatic and terrestrial ecosystems. In temperate wetlands, insect communities are largely dominated by midges, such as non-biting chironomids and mosquitoes. Particularly chironomids and their aquatic larvae play a key role for both aquatic and terrestrial predators, e.g., dragonflies and damselflies (Odonata), birds, riparian spiders and amphibians. Therefore, adverse effects on chironomid larvae induced by pesticides or biocides can have implications on food webs across ecosystem boundaries.
In floodplains of the Upper Rhine Valley in southwest Germany, the biocide Bacillus thuringiensis var. israelensis (Bti) has been applied for over 40 years to reduce nuisance by mass emergence of mosquitoes. Due to its specific mode of action, Bti is presumed to be a more environmentally friendly alternative to non-selective, highly toxic pesticides used in the past. However, research on indirect effects of Bti on non-target organisms inhabiting these wetlands is still relatively scarce. The aim of this thesis was the investigation of direct and indirect effects of Bti on non-target organisms and, consequently, bottom-up effects on aquatic food webs and propagation to the terrestrial ecosystem. Effects were examined in outdoor floodplain pond mesocosms (FPMs) with natural flora and fauna communities.
Benthic macroinvertebrate communities were significantly altered in Bti-treated FPMs, largely due to the reduction of chironomid density by over 40% compared to untreated FPMs. Sampling of exuviae indicated that the emergence of Libellulidae (Odonata) was reduced by Bti, while larger Aeshnidae were not affected. This finding suggested increased intraguild predation (predation of competing predators) in Bti-treated FPMs as a result of decreased prey availability, i.e. chironomid larvae. This conclusion was partly confirmed in food web analyses using stable isotopes of C and N and fatty acids, with Aeshnidae experiencing a slight diet shift towards larger prey (i.e., newts, Aeshnidae) in Bti-treated FPMs. In contrast, the diet proportions of newt larvae were not affected by Bti treatment, but showed a marginal trend in lower omega-6 fatty acid content. Analyses of oxidative stress biomarkers did not reveal any direct effects of Bti on common frog tadpoles under natural climatic conditions.
This thesis emphasizes that adverse effects of Bti on the base of aquatic-terrestrial food webs, i.e., reduction of larval chironomids, can have implications for higher trophic levels and cascade to terrestrial ecosystems. Affected organisms also include species of concern, such as protected Odonata species. In view of the global insect and amphibian decline, the large-scale use of Bti in (partially protected) wetlands should be carefully considered.
Erhard, Amelie A. ; Klein, Matthias P. ; Mohrbach, Jennifer ; Dillinger, Sebastian ; Niedner-Schatteburg, Gereon
We report the N2 cryo adsorption kinetics of selected gas phase mixed rhodium–iron clusters [RhiFej]+ in the range of i = 3–8 and j = 3–8 in 26 K He buffer gas by the use of a cryo tandem RF-hexapole trap–Fourier transform ion cyclotron resonance mass spectrometer. From kinetic data and fits, we extract relative rate constants for each N2 adsorption step and possible desorption steps. We find significant trends in adsorption behavior, which reveal adsorption limits, intermittent adsorption limits, and equilibrium reactions. For those steps, which are in equilibrium, we determine the Gibbs free energies. We conclude on likely ligand shell reorganization and some weakly bound N2 ligands for clusters where multiple N2 adsorbates are in equilibrium. The relative rate constants are transferred to absolute rate constants, which are slightly smaller than the collision rate constants calculated by the average dipole orientation (Langevin) theory. The calculated sticking probabilities increase, in general, with the size of the clusters and decrease with the level of N2 adsorption, in particular, when reaching an adsorption/desorption equilibrium. We receive further evidence on cluster size dependent properties, such as cluster geometries and metal atom distributions within the clusters through the accompanying spectroscopic and computational study on the equiatomic i = j clusters [Klein et al., J. Chem. Phys. 156, 014302 (2022)].
Straßner, Annika ; Wiehn, Christopher ; Klein, Matthias P. ; Fries, Daniela V. ; Dillinger, Sebastian ; Mohrbach, Jennifer ; Prosenc, Marc H. ; Armentrout, Peter B. ; Niedner-Schatteburg, Gereon
Infrared photodissociation (IR-PD) spectra of iron cluster dinitrogen adsorbate complexes [Fen(N2)m]+ for n = 8–20 reveal slightly redshifted IR active bands in the region of 2200–2340 cm−1. These bands mostly relate to stretching vibrations of end-on coordinated N2 chromophores, a μ1,end end-on binding motif. Density Functional Theory (DFT) modeling and detailed analysis of n = 13 complexes are consistent with an icosahedral Fe13+ core structure. The first adsorbate shell closure at (n,m) = (13,12)—as recognized by the accompanying paper on the kinetics of N2 uptake by cationic iron clusters—comes with extensive IR-PD band broadening resulting from enhanced couplings among adjacent N2 adsorbates. DFT modeling predicts spin quenching by N2 adsorption as evidenced by the shift of the computed spin minima among possible spin states (spin valleys). The IR-PD spectrum of (17,1) surprisingly reveals an absence of any structure but efficient non-resonant fragmentation, which might indicate some weakly bound (roaming) N2 adsorbate. The multiple and broad bands of (17,m) for all other cases than (17,1) and (17,7) indicate a high degree of variation in N2 binding motifs and couplings. In contrast, the (17,7) spectrum of six sharp bands suggests pairwise equivalent N2 adsorbates. The IR-PD spectra of (18,m) reveal additional features in the 2120–2200 cm−1 region, which we associate with a μ1,side side-on motif. Some additional features in the (18,m) spectra at high N2 loads indicate a μ1,tilt tilted end-on adsorption motif.
We discuss the realization of a magnonic version of the STImulated-Raman-Adiabatic-Passage (m-STIRAP) mechanism using micromagnetic simulations. We consider the propagation of magnons in curved magnonic directional couplers. Our results demonstrate that quantum-classical analogy phenomena are accessible in magnonics. Specifically, the inherent advantages of the STIRAP mechanism, associated with dark states, can now be utilized in magnonics. Applications of this effect for future magnonic device functionalities and designs are discussed.
Sombrio, Guilherme ; Oliveira, Emerson ; Strassner, Johannes ; Doering, Christoph ; Fouckhardt, Henning
Semiconductor multilayer and device fabrication is a complex task in electronics and opto-electronics. Layer dry etching is one of the process steps to achieve a specific lateral device design. In situ and real-time monitoring of etch depth will be necessary if high precision in etch depth is required. Nondestructive optical techniques are the methods of choice. Reflectance anisotropy spectroscopy equipment has been used to monitor the accurate etch depth during reactive ion etching of III/V semiconductor samples in situ and real time. For this purpose, temporal Fabry–Perot oscillations due to the etch-related shrinking thickness of the uppermost layer have been exploited. Earlier, we have already reported an etch-depth resolution of ±16.0 nm. By the use of a quadruple-Vernier-scale measurement and an evaluation protocol, now we even improve the in situ real-time etch-depth resolution by a factor of 20, i.e., nominally down to ±0.8 nm.
Heinz, Björn ; Wang, Qi ; Schneider, Michael ; Weiß, Elisabeth ; Lentfert, Akira ; Lägel, Bert ; Brächer, Thomas ; Dubs, Carsten ; Dobrovolskiy, Oleksandr V. ; Pirro, Philipp ; Chumak, Andrii V.
Magnonics attracts increasing attention in the view of low-energy computation technologies based on spin waves. Recently, spin-wave propagation in longitudinally magnetized nano-scaled spin-wave conduits was demonstrated, proving the fundamental feasibility of magnonics at the sub-100 nm scale. Transversely magnetized nano-conduits, which are of great interest in this regard as they offer a large group velocity and a potentially chirality-based protected transport of energy, have not yet been investigated due to their complex internal magnetic field distribution. Here, we present a study of propagating spin waves in a transversely magnetized nanoscopic yttrium iron garnet conduit of 50 nm width. Space and time-resolved microfocused Brillouin-light-scattering spectroscopy is employed to measure the spin-wave group velocity and decay length. A long-range spin-wave propagation is observed with a decay length of up to (8.0 ± 1.5) μm and a large spin-wave lifetime of up to (44.7 ± 9.1) ns. The results are supported with micromagnetic simulations, revealing a broad single-mode frequency range and the absence of a mode localized to the edges. Furthermore, a frequency nonreciprocity for counter-propagating spin waves is observed in the simulations and the experiment, caused by the trapezoidal cross section of the structure. The revealed long-distance spin-wave propagation on the nano-scale is particularly interesting for an application in spin-wave devices, allowing for long-distance transport of information in magnonic circuits and low-energy device architectures.
Examination of laminar Couette flow with obstacles by a low-cost particle image velocimetry setup
(2021)
For many technical applications, a detailed analysis of the fluid mechanical properties is necessary, for which computational fluid dynamics (CFD) simulations are used. However, even though flow simulations are becoming faster and more accurate, validation through experimentation is essential. One way of validation is to use Particle Image Velocimetry (PIV), an imaging technique that can visualize the flow field and measure flow velocities. Since the measuring equipment of commercial systems is very expensive, we propose a low-cost PIV setup that is also affordable for small scientific institutions. In addition to the quality of the acquired images, the reliability and comparability between experiment and simulation are also important issues. Therefore, in this work, we compare the image acquisition quality of the proposed low-cost PIV system with two- and three-dimensional CFD simulations for a laminar Couette flow and a laminar flow around square and hexagonal obstacles with very good agreement. In addition, we analyzed the transferability of 2D and 3D CFD simulations with experiments by measuring the velocity field and found that experimentally determined flow velocities often cannot be used to validate idealized (2D) simulations due to the spatial flow that occurs. However, if the non-ideal conditions of the experiment are considered in the (3D) simulation, a good comparability is given and an experimental validation is possible, for which the presented low-cost PIV system is well suitable.
In situ condition monitoring of rotary shaft seals could significantly improve the reliability of future seals in numerous applications. A superficial application of strain gauges capturing the state of deformation could offer a cost-effective retrofit solution for indirect measurements of central operational parameters. Within a simulative investigation of the sealing system, possible sensor positions for determination of the preload as well as the friction torque prevailing in the sealing contact are therefore identified as two parameters directly related to the operating condition. Further investigations of the potential sensor signal with focus on its time-dependent behavior prove the theoretical feasibility of the measurement concepts developed and provide promising prospects for an initial technical implementation.