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Jens Müller

Publications and source records attributed to Jens Müller.

At least 19 recordsLinked to original sources

Epitaxial growth and magnetic phase transitions in non-centrosymmetric EuPdSi$_3$ thin films

Non-centrosymmetric magnetic materials are a promising platform for stabilizing chiral spin textures, such as skyrmions and cycloidal magnetic states. This is particularly true in epitaxial thin film geometries, where strain and interface effects offer additional control. Herein, we report on the first epitaxial thin films of EuPdSi$_3$ grown by molecular beam epitaxy on MgO(001). X-ray diffraction confirms an epitaxial relationship of tetragonal EuPdSi$_3$ in the BaNiSn$_3$ structure with out-of-plane c-axis orientation and parallel in-plane a-axes. Hard x-ray photoelectron spectroscopy reveals a stable Eu valence of 2.0, yielding a large magnetic moment of approximately 7 $μ_B$ per Eu atom in accordance with Hund's rule. Owing to the non-centrosymmetric crystal structure, non-collinear magnetic states such as Néel-type skyrmions and cycloidal phases are allowed by symmetry. Electronic transport measurements reveal two magnetic phase transitions at 19 K and 15 K in zero applied field. Under magnetic fields applied along the crystallographic [100] and [001] directions, distinct temperature dependent magnetic phases emerge, demonstrating the sensitivity of the magnetic ground state to field orientation in epitaxial EuPdSi$_3$ thin films.

cond-mat.mtrl-sci

Towards Context-Aware Domain Generalization: Understanding the Benefits and Limits of Marginal Transfer Learning

In this work, we analyze the conditions under which information about the context of an input $X$ can improve the predictions of deep learning models in new domains. Following work in marginal transfer learning in Domain Generalization (DG), we formalize the notion of context as a permutation-invariant representation of a set of data points that originate from the same domain as the input itself. We offer a theoretical analysis of the conditions under which this approach can, in principle, yield benefits, and formulate two necessary criteria that can be easily verified in practice. Additionally, we contribute insights into the kind of distribution shifts for which the marginal transfer learning approach promises robustness. Empirical analysis shows that our criteria are effective in discerning both favorable and unfavorable scenarios. Finally, we demonstrate that we can reliably detect scenarios where a model is tasked with unwarranted extrapolation in out-of-distribution (OOD) domains, identifying potential failure cases. Consequently, we showcase a method to select between the most predictive and the most robust model, circumventing the well-known trade-off between predictive performance and robustness.

cs.LG

Robust Magnetic Polaron Percolation in the Antiferromagnetic CMR System EuCd$_2$P$_2$

Antiferromagnetic EuCd$_2$P$_2$ has attracted considerable attention due to its unconventional (magneto)transport properties. At a temperature $T_{\rm peak}$ significantly above the magnetic ordering temperature $T_\textrm{N} = 11\,$K a large peak in resistivity is observed which gets strongly suppressed in magnetic field, resulting in a colossal magnetoresistance (CMR), for which magnetic fluctuations and the formation of ferromagnetic clusters have been proposed as underlying mechanisms. Employing a selection of sensitive probes including fluctuation spectroscopy and third-harmonic resistance, Hall effect, AC susceptibility and $μ$SR measurements, allows for a direct comparison of electronic and magnetic properties on multiple time scales. We find compelling evidence for the formation and percolation of magnetic polarons, which explains the CMR of the system. Large peaks in the weakly-nonlinear transport and the resistance noise power spectral density at zero magnetic field signify an inhomogeneous, percolating electronic system below $T^\ast \approx 2\,T_\textrm{N}$ with a percolation threshold at $T_{\rm peak}$. In magnetic fields, the onset of large negative MR in the paramagnetic regime occurs at a universal critical magnetization similar to ferromagnetic CMR materials. The size of the magnetic polarons at the percolation threshold is estimated to $\sim 1 - 2\,$nm. The mechanism of magntic cluster formation and percolation in EuCd$_2$P$_2$ appears to be rather robust despite large variations in carrier concentration and likely is relevant for other Eu-based antiferromagnetic CMR systems.

cond-mat.str-el

Deciphering the Definition of Adversarial Robustness for post-hoc OOD Detectors

Detecting out-of-distribution (OOD) inputs is critical for safely deploying deep learning models in real-world scenarios. In recent years, many OOD detectors have been developed, and even the benchmarking has been standardized, i.e. OpenOOD. The number of post-hoc detectors is growing fast. They are showing an option to protect a pre-trained classifier against natural distribution shifts and claim to be ready for real-world scenarios. However, its effectiveness in dealing with adversarial examples (AdEx) has been neglected in most studies. In cases where an OOD detector includes AdEx in its experiments, the lack of uniform parameters for AdEx makes it difficult to accurately evaluate the performance of the OOD detector. This paper investigates the adversarial robustness of 16 post-hoc detectors against various evasion attacks. It also discusses a roadmap for adversarial defense in OOD detectors that would help adversarial robustness. We believe that level 1 (AdEx on a unified dataset) should be added to any OOD detector to see the limitations. The last level in the roadmap (defense against adaptive attacks) we added for integrity from an adversarial machine learning (AML) point of view, which we do not believe is the ultimate goal for OOD detectors.

cs.CR

Magnetic frustration and weak Mn magnetic ordering in EuMn$_2$P$_2$

We report on the electron spin resonance (ESR), heat capacity, magnetization, nuclear magnetic resonance (NMR), magnetic circular and linear dichroism (XMCD, XMLD), as well as the electrical resistivity of EuMn$_{2}$P$_{2}$ single crystals. Antiferromagnetic order of Eu was observed in several quantities at $T^{\rm Eu}_{\rm N}\,=\,18\,\rm K$. The temperature dependencies of ESR linewidth and resonance shift show, when approaching the Eu-ordered state, a divergence towards $T^{\rm Eu}_{\rm N}$, indicating the growing importance of magnetic correlations and the build-up of internal magnetic fields. An additional temperature scale of $\approx 47\,\rm K$ has considerable impact on linewidth, resonance field and intensity. This points to the presence of weak Mn-based ordering. The observed ESR line is interpreted as an Eu$^{2+}$ resonance, which probes the weak magnetic background of the Mn subsystem. Such picture is suggested by the lineshape which keeps to be Lorentzian across the $47\,\rm K$ scale and by the ESR intensity which can be described by the same Curie-Weiss temperature above and below $47\,\rm K$. In the same temperature range anomalies were observed at $48.5\,\rm K$ and $51\,\rm K$ in the heat capacity data as well as a pronounced broadening of the NMR signal of the EuMn$_{2}$P$_{2}$ samples. In XMCD and XMLD measurements, this weak magnetic order could not be detected in the same temperature range which might be due to the small magnetic moment, with a potential $c$-component or frustration.

cond-mat.str-el

Ferroelectric and Multiferroic Properties of Quasi-2D Organic Charge-Transfer Salts

In conventional ferroelectrics the electric dipoles are generated by off-center displacements of ions. In recent years, a new type of so-called electronic ferroelectrics has attracted great attention, where the polarization is driven by electronic degrees of freedom. Of particular interest are materials with strong electronic correlations, featuring a variety of intriguing phenomena and instabilities, which may interact with or even induce electronic ferroelectricity. In this review, we will focus on the class of strongly correlated charge-transfer salts, where electronic ferroelectricity was suggested by theory and has been confirmed by numerous experiments. The paper summarizes some basic physical properties of various relevant quasi-two dimensional salts and gives some background on the experimental tools applied to establish ferroelectricity. We discuss the key experimental observations, including the exciting discovery of multiferroicity, and provide some theoretical considerations on the magnetoelectric couplings that are of relevance here.

cond-mat.str-el

Magnetism, heat capacity and electronic structure of EuCd$_2$P$_2$ in view of its colossal magnetoresistance

The mechanism of the peculiar transport properties around the magnetic ordering temperature of semiconducting antiferromagnetic EuCd$_2$P$_2$ is not yet understood. With a huge peak in the resistivity observed above the Néel temperature, $T_{\rm N}=10.6\,\rm K$, it exhibits a colossal magnetoresistance effect. Recent reports on observations of ferromagnetic contributions above $T_{\rm N}$ as well as metallic behavior below this temperature have motivated us to perform a comprehensive characterization of this material, including its resistivity, heat capacity, magnetic properties and electronic structure. Our transport measurements revealed quite different temperature dependence of resistivity with the maximum at $14\,\rm K$ instead of previously reported $18\,\rm K$. Low-field susceptibility data support the presence of static ferromagnetism above $T_{\rm N}$ and show a complex behavior of the material at small applied magnetic fields. Namely, signatures of reorientation of magnetic domains are observed up to $T=16\,\rm K$. Our magnetization measurements indicate a magnetocrystalline anisotropy which also leads to a preferred alignment of the magnetic clusters above $T_{\rm N}$. The momentum-resolved photoemission experiments at temperatures from $24\,\rm K$ down to $2.5\,\rm K$ indicate the permanent presence of a fundamental band gap without change of the electronic structure when going through $T_N$ that is in contradiction with previous results. We performed \textit{ab initio} band structure calculations which are in good agreement with the measured photoemission data when assuming an antiferromagnetic ground state. Calculations for the ferromagnetic phase show a much smaller bandgap, indicating the importance of possible ferromagnetic contributions for the explanation of the colossal magnetoresistance effect in the related EuZn$_2$P$_2$.

cond-mat.str-el

Origin of magnetic switching cascades in tetrahedral CoFe nanostructures

We present a comprehensive study of small-scale three-dimensional (3D) tetrahedral CoFe nanostructure arrays prepared by focused electron beam-induced deposition (FEBID) and placed in two distinct orientations with respect to the direction of an external magnetic field. Using ultra-sensitive micro-Hall magnetometry we obtain angular-dependent magnetic stray field hysteresis loops that show characteristic cascading magnetic switching close to zero magnetic field. By employing micromagnetic simulations we could reproduce the hysteresis loops and identify characteristic field dependent magnetic configurations including a vortex-type groundstate. From this we derive a coarse-graining macrospin model and show that the complex switching behavior can be explained by the reorientation dynamics of non-interacting uniaxial anisotropic magnetic grains modeled as a superposition of Stoner-Wohlfarth particles.

cond-mat.mes-hall

Combined experimental and theoretical studies on glasslike transitions in the frustrated molecular conductors $θ$-(BEDT-TTF)$_2MM'$(SCN)$_4$

We present results of the coefficient of thermal expansion for the frustrated quasi-two-dimensional molecular conductor $θ$-(BEDT-TTF)$_2$RbZn(SCN)$_4$ for temperatures 1.5 K $\leq T \leq$ 290 K. A pronounced first-order phase transition anomaly is observed at the combined charge-order/structural transition at 215 K. Furthermore, clear evidence is found for two separate glasslike transitions at $T_{\mathrm{g}}$ = 90-100 K and $T_{\mathrm{g}}^\dagger$ = 120-130 K, similar to previous findings for $θ$-(BEDT-TTF)$_2$CsZn(SCN)$_4$ and $θ$-(BEDT-TTF)$_2$CsCo(SCN)$_4$, reported in T. Thomas et al., Phys. Rev. B 105, L041114 (2022), both of which lack the charge-order/structural transition. Our findings indicate that these glasslike transitions are common features for the $θ$-(BEDT-TTF)$_2MM^\prime$(SCN)$_4$ family with $M$ = (Rb, Cs) and $M^\prime$ = (Co, Zn), irrespective of the presence or absence of charge order. These results are consistent with our model calculations on the glasslike dynamics associated with the flexible ethylene endgroups of the BEDT-TTF molecules for various $θ$-(BEDT-TTF)$_2MM^\prime$(SCN)$_4$ salts, predicting two different conformational glass transitions. Moreover, calculations of the hopping integrals show a substantial degree of dependence on the endgroups' conformation, suggesting a significant coupling to the electronic degrees of freedom. Our findings support the possibility that the glassy freezing of the ethylene endgroups could drive or enhance glassy charge dynamics.

cond-mat.str-el

Colossal magnetoresistance in EuZn$_2$P$_2$ and its electronic and magnetic structure

We investigate single crystals of the trigonal antiferromagnet EuZn$_2$P$_2$ ($P\overline{3}m1$) by means of electrical transport, magnetization measurements, X-ray magnetic scattering, optical reflectivity, angle-resolved photoemission spectroscopy (ARPES) and ab-initio band structure calculations (DFT+U). We find that the electrical resistivity of EuZn$_2$P$_2$ increases strongly upon cooling and can be suppressed in magnetic fields by several orders of magnitude (CMR effect). Resonant magnetic scattering reveals a magnetic ordering vector of $q = (0\, 0\, \frac{1}{2})$, corresponding to an $A$-type antiferromagnetic (AFM) order, below $T_{\rm N} = 23.7\,\rm K$. We find that the moments are canted out of the $a-a$ plane by an angle of about $40^{\circ}\pm 10^{\circ}$ degrees and aligned along the [100] in the $a-a$ plane. We observe nearly isotropic magnetization behavior for low fields and low temperatures which is consistent with the magnetic scattering results. The magnetization measurements show a deviation from the Curie-Weiss behavior below $\approx 150\,\rm K$, the temperature below which also the field dependence of the material's resistivity starts to increase. An analysis of the infrared reflectivity spectrum at $T=295\,\rm K$ allows us to resolve the main phonon bands and intra-/interband transitions, and estimate indirect and direct band gaps of $E_i^{\mathrm{opt}}=0.09\,\rm{eV}$ and $E_d^{\mathrm{opt}}=0.33\,\rm{eV}$, respectively, which are in good agreement with the theoretically predicted ones. The experimental band structure obtained by ARPES is nearly $T$-independent above and below $T_{\rm N}$. The comparison of the theoretical and experimental data shows a weak intermixing of the Eu 4$f$ states close to the $Γ$ point with the bands formed by the phosphorous 3$p$ orbitals leading to an induction of a small magnetic moment at the P sites.

cond-mat.str-el

On the Convergence Rate of Gaussianization with Random Rotations

Gaussianization is a simple generative model that can be trained without backpropagation. It has shown compelling performance on low dimensional data. As the dimension increases, however, it has been observed that the convergence speed slows down. We show analytically that the number of required layers scales linearly with the dimension for Gaussian input. We argue that this is because the model is unable to capture dependencies between dimensions. Empirically, we find the same linear increase in cost for arbitrary input $p(x)$, but observe favorable scaling for some distributions. We explore potential speed-ups and formulate challenges for further research.

cs.LG

Finding Competence Regions in Domain Generalization

We investigate a "learning to reject" framework to address the problem of silent failures in Domain Generalization (DG), where the test distribution differs from the training distribution. Assuming a mild distribution shift, we wish to accept out-of-distribution (OOD) data from a new domain whenever a model's estimated competence foresees trustworthy responses, instead of rejecting OOD data outright. Trustworthiness is then predicted via a proxy incompetence score that is tightly linked to the performance of a classifier. We present a comprehensive experimental evaluation of existing proxy scores as incompetence scores for classification and highlight the resulting trade-offs between rejection rate and accuracy gain. For comparability with prior work, we focus on standard DG benchmarks and consider the effect of measuring incompetence via different learned representations in a closed versus an open world setting. Our results suggest that increasing incompetence scores are indeed predictive of reduced accuracy, leading to significant improvements of the average accuracy below a suitable incompetence threshold. However, the scores are not yet good enough to allow for a favorable accuracy/rejection trade-off in all tested domains. Surprisingly, our results also indicate that classifiers optimized for DG robustness do not outperform a naive Empirical Risk Minimization (ERM) baseline in the competence region, that is, where test samples elicit low incompetence scores.

cs.LG

Convolutional Neural Networks for Epileptic Seizure Prediction

Epilepsy is the most common neurological disorder and an accurate forecast of seizures would help to overcome the patient's uncertainty and helplessness. In this contribution, we present and discuss a novel methodology for the classification of intracranial electroencephalography (iEEG) for seizure prediction. Contrary to previous approaches, we categorically refrain from an extraction of hand-crafted features and use a convolutional neural network (CNN) topology instead for both the determination of suitable signal characteristics and the binary classification of preictal and interictal segments. Three different models have been evaluated on public datasets with long-term recordings from four dogs and three patients. Overall, our findings demonstrate the general applicability. In this work we discuss the strengths and limitations of our methodology.

cs.LG

Microstructuring YbRh2Si2 for resistance and noise measurements down to ultra-low temperatures

The discovery of superconductivity in the quantum critical Kondo-lattice system YbRh2Si2 at an extremely low temperature of 2 mK has inspired efforts to perform high-resolution electrical resistivity measurements down to this temperature range in highly conductive materials. Here we show that control over the sample geometry by microstructuring using focused-ion-beam (FIB) techniques allows to reach ultra-low temperatures and increase signal-to-noise ratios (SNR) tenfold, without adverse effects to sample quality. In five experiments we show four-terminal sensing resistance and magnetoresistance measurements which exhibit sharp phase transitions at the Néel temperature, and Shubnikov-de-Haas (SdH) oscillations between 13 T and 18 T where we identified a new SdH frequency of 0.39 kT. The increased SNR allowed resistance fluctuation (noise) spectroscopy that would not be possible for bulk crystals, and confirmed intrinsic 1/f-type fluctuations. Under controlled strain, two thin microstructured samples exhibited a large increase of T_N from 67 mK up to 188 mK while still showing clear signatures of the phase transition and SdH oscillations. SQUID-based thermal noise spectroscopy measurements in a nuclear demagnetisation refrigerator down to 0.95 mK, show a sharp superconducting transition at T_c = 1.2 mK. These experiments demonstrate microstructuring as a powerful tool to investigate the resistance and the noise spectrum of highly conductive correlated metals over wide temperature ranges.

cond-mat.str-el

Phonon renormalization effects accompanying the 6 K anomaly in the Quantum Spin Liquid Candidate $κ$-(BEDT-TTF)$_{2}$Cu$_{2}$(CN)$_{3}$

The low-temperature state of the quantum spin liquid candidate $κ$-(BEDT-TTF)$_{2}$Cu$_{2}$(CN)$_{3}$ emerges via an anomaly at $T^{*}\sim6$ K. Although signatures of this anomaly have been revealed in various quantities, its origin has remained unclear. Here we report inelastic neutron scattering measurements on single crystals of $κ$-(BEDT-TTF)$_{2}$Cu$_{2}$(CN)$_{3}$, aiming at studying phonon renormalization effects at $T^{*}$. A drastic change was observed in the phonon damping across $T^{*}$ for a breathing mode of BEDT-TTF dimers at $E=4.7$ meV. The abrupt change in the phonon damping is attributed to a phase transition into a valence bond solid state based on an effective model describing the spin-charge coupling in this dimer-Mott system.

cond-mat.str-el

Comparison of the charge-crystal and charge-glass state in geometrically frustrated organic conductors studied by fluctuation spectroscopy

We present a systematic investigation of the low-frequency charge carrier dynamics in different charge states of the organic conductors $θ$-(BEDT-TTF)$_2$$M$Zn(SCN)$_4$ with $M$=Rb,Tl, which result from quenching or relaxing the charge degrees of freedom on a geometrically frustrated triangular lattice. Due to strong electronic correlations these materials exhibit a charge-ordering transition, which can be kinetically avoided by rapid cooling resulting in a so-called charge-glass state without long-range order. The combination of fluctuation spectroscopy and a heat pulse method allows us to study and compare the resistance fluctuations in the low-resistive quenched and the high-resistive charge-ordered state, revealing striking differences in the respective noise magnitudes. For both compounds, we find strongly enhanced resistance fluctuations right at the metal-insulator transition and a broad noise maximum in the slowly cooled charge-crystal state with partly dominating two-level processes revealing characteristic activation energies.

cond-mat.str-el

Seizure prediction with long-term iEEG recordings: What can we learn from data nonstationarity?

Repeated epileptic seizures impair around 65 million people worldwide and a successful prediction of seizures could significantly help patients suffering from refractory epilepsy. For two dogs with yearlong intracranial electroencephalography (iEEG) recordings, we studied the influence of time series nonstationarity on the performance of seizure prediction using in-house developed machine learning algorithms. We observed a long-term evolution on the scale of weeks or months in iEEG time series that may be represented as switching between certain meta-states. To better predict impending seizures, retraining of prediction algorithms is therefore necessary and the retraining schedule should be adjusted to the change in meta-states. There is evidence that the nature of seizure-free interictal clips also changes with the transition between meta-states, accwhich has been shown relevant for seizure prediction.

q-bio.NC

Probing the magnetic polaron state in the ferromagnetic semiconductor HgCr$_2$Se$_4$ with resistance fluctuation and muon-spin spectroscopy measurements

Combined resistance noise and muon-spin relaxation ($μ$SR) measurements of the ferromagnetic semiconductor HgCr$_2$Se$_4$ suggest a degree of magnetoelectric coupling and provide evidence for the existence of isolated magnetic polarons. These form at elevated temperatures and undergo a percolation transition with a drastic enhancement of the low-frequency 1/$f$-type charge fluctuations at the insulator-to-metal transition at $\sim 95 - 98$ K in the vicinity of the magnetic ordering temperature $T_C \sim 105 - 107$ K. Upon approaching the percolation threshold from above, the strikingly unusual dynamics of a distinct two-level fluctuator superimposed on the $1/f$ noise can be described by a slowing down of the dynamics of a nanoscale magnetic cluster, a magnetic polaron, when taking into account an effective radius of the polaron depending on the spin correlation length. Coinciding temperature scales found in $μ$SR and noise measurements suggest changes in the magnetic dynamics over a wide range of frequencies and are consistent with the existence of large polarized and domain-wall-like regions at low temperatures, that result from the freezing of spin dynamics at the magnetic polaron percolation transition.

cond-mat.str-el