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Poly(ethylene oxide) is an important polymer with many applications, e.g., as solid-state electrolyte in batteries. Its relaxation dynamics, characterizing its molecular and submolecular motions, which is relevant for many of these applications, was investigated numerous times, mostly employing dielectric spectroscopy. However, the various dynamic processes revealed by these studies were interpreted in conflicting ways and even their nomenclature in literature is highly inconsistent. Here we present the results of a detailed investigation of this polymer employing dielectric spectroscopy covering a relatively broad frequency and temperature range. We clearly detect four intrinsic relaxation processes. The slowest one most likely represents a so-called normal mode, reflecting global motions of the polymer chains, an interpretation that was not considered in previous works. The second process can be unequivocally identified with the segmental alpha relaxation, which governs glassy freezing and the glass transition. The third, only rarely detected process corresponds to the Johari-Goldstein relaxation of poly(ethylene oxide), widely overlooked in previous studies. The fourth and fastest process is unrelated to the supercooled and glassy state of this polymer and probably due to local, intramolecular motions., Comment: 11 pages, 3 figures

Recently, a universal relation between the thermal expansion coefficient of glasses $\alpha_g$, their glass-transition temperature Tg, and the so-called fragility index m of the corresponding supercooled liquid state was found to be valid for more than 200 glass formers, namely $\alpha_g/m\propto 1/T_g$ [P. Lunkenheimer et al., Nat. Phys. 19, 694 (2023)]. Here we show that this could also have far-reaching consequences for our understanding of crystal melting. Namely, when considering the empirically founded 2/3-rule, stating that the ratio of Tg and the melting temperature Tm is about 2/3 for almost all materials, for crystals a similar relation, $\alpha_c/m\propto 1/T_m$, should apply. Indeed, we find that the available experimental data are well consistent with such a relation. This implies that the melting of a crystal into an ordinary (non-supercooled) liquid is influenced by the fragility, a property quantifying the non-Arrhenius dynamics in the supercooled-liquid state of the material. We argue that this can be explained by a significant enhancement of the "ideal" (non-cooperative) melting temperature arising from the cooperativity of the particle motion in the liquid state above Tm. Therefore, a reassessment of the currently widely accepted microscopic understanding of crystal melting, still founded on the general ideas that lead to the time-honored Lindemann melting criterion, may be necessary., Comment: 9 pages, 3 figures + 6 pages Supplemental Material

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.

A detailed study of published experimental data for a variety of materials on the incremental variation of heat capacity, thermal expansion, and compressibility at glassy freezing reveals a striking dependence of the Prigogine-Defay ratio R on the fragility index m. At high m, R approaches values of ~1, the Ehrenfest expectation for 2nd order continuous phase transitions, while R reaches values > 20 for low fragilities. We explain this correlation by the degree of separation of the glassy freezing temperature from a hidden phase transition into an ideal low-temperature glass., Comment: Manuscript 11 pages, 2 figures and Supplemental Material 6 pages, 1 figure, 1 table

Deep eutectic solvents with admixed lithium salts are considered as electrolytes in electrochemical devices like batteries or supercapacitors. Compared to eutectic mixtures of hydrogen-bond donors and lithium salts, their raw-material costs are significantly lower. Not much is known about the glassy freezing and rotation-translation coupling of such systems. Here we investigate these phenomena by applying dielectric spectroscopy to the widely studied deep eutectic solvent glyceline, to which 1 and 5 mol% LiCl were added. Our studies cover a wide temperature range, including the deeply supercooled state. The temperature dependences of the detected dipolar reorientation dynamics and of the ionic dc conductivity reveal the signatures of glassy freezing. In comparison to pure glyceline, lithium admixture leads to a reduction of ionic conductivity, which is accompanied by a slowing down of the rotational dipolar motions. However, this reduction is much smaller than for DESs, where one main component is a lithium salt, which we trace back to the smaller glass-transition temperatures of the lithium-doped DESs. In contrast to pure glyceline, the ionic and dipolar dynamics become increasingly decoupled at low temperatures and obey a fractional Debye-Stokes-Einstein relation as previously found in other glass-forming liquids. The obtained results demonstrate the relevance of decoupling effects and of the glass transition for the enhancement of the technically relevant ionic conductivity in such lithium-doped DESs., Comment: 9 pages, 4 figures + Supporting Information

A promising mechanism for achieving colossal dielectric constants is to use insulating internal barrier layers, which typically form during synthesis and then remain in the material. It has recently been shown that insulating domain walls in ferroelectrics can act as such barriers. One advantage domain walls have, in comparison to stationary interfaces, is that they can be moved, offering the potential of post-synthesis control of the dielectric constant. However, to date, direct imaging of how changes in domain wall pattern cause a change in dielectric constant within a single sample has not been realized. In this work, we demonstrate that changing the domain wall density allows the engineering of the dielectric constant in hexagonal-ErMnO3 single crystals. The changes of the domain wall density are quantified via microscopy techniques, while the dielectric constant is determined via macroscopic dielectric spectroscopy measurements. The observed changes in the dielectric constant are quantitatively consistent with the observed variation in domain wall density, implying that the insulating domain walls behave as 'ideal' capacitors connected in series. Our approach to engineer the domain wall density can be readily extended to other control methods, e.g., electric fields or mechanical stresses, providing a novel degree of flexibility to in-situ tune the dielectric constant.

We present a detailed study on the temperature-dependent THz spectra of the polycrystalline amino acids L-serine and L-cysteine for wave numbers from 20 to 120 cm-1 and temperatures from 4 to 300 K. Even though the structure of these two amino acids is very similar, with a sulfur atom in the side chain of cysteine instead of an oxygen atom in serine, the excitation spectra are drastically different. Obviously, the vibrational dynamics strongly depend on the ability of cysteine to form sulfur-hydrogen bonds. In addition, cysteine undergoes an order-disorder type phase transition close to 80 K, with accompanying anomalies in our THz results. On increasing temperatures, well-defined vibrational excitations, exhibit significant shifts in eigenfrequencies with concomitant line-broadening yielding partly overlapping modes. Interestingly, several modes completely lose all their dipolar strength and are unobservable at ambient conditions. Comparing the recent results with published work utilizing THz, Raman, and neutron-scattering techniques, as well as with ab-initio simulations, we aim at a consistent analysis of the results ascribing certain eigenfrequencies to distinct collective lattice modes. We document that THz spectra can be used to fine-tune parameters of model calculations and as a fingerprint property of certain amino acids. In addition, we analyzed the temperature-dependent heat capacity of both compounds and detected strong excess heat capacities at low temperatures compared to the canonical Debye behavior of crystalline solids, indicating soft excitations and a strongly enhanced phonon-density of states at low frequencies., Comment: 31 pages, 8 figures, 70 references

The glass formation and the dipolar reorientational motions in deep eutectic solvents (DESs) are frequently overlooked, despite their crucial role in defining the room-temperature physiochemical properties. To understand the effects of these dynamics on the ionic conductivity and their relation to the mechanical properties of the DES, we conducted broadband dielectric and rheological spectroscopy over a wide temperature range on three well-established carboxylic-acid-based natural DESs: oxaline, maline, and the eutectic mixture of choline chloride with phenylacetic acid (phenylaceline). In all three DESs, we observe signs of glassy freezing in the temperature dependence of their dipolar reorientational and structural dynamics, as well as varying degrees of motional decoupling between the different observed dynamics: Maline and oxaline display a breaking of the Walden rule near the glass-transition temperature, while the relation between the dc conductivity and dipolar relaxation time in both maline and phenylaceline is best described by a power law. The glass-forming properties of the investigated systems not only govern the orientational dipolar motions and rheological properties, which are of interest from a fundamental point of view, but they also affect the dc conductivity, even at room temperature, which is of high technical relevance., Comment: 11 pages, 6 figures + Supplemental Material (3 pages, 4 figures)

Glass formation and reorientational motions are widespread, but often-neglected features of deep eutectic solvents, although both can be relevant for the technically important ionic conductivity at room temperature. Here we investigate these properties for two mixtures of ethylene glycol and ZnCl2, which were recently considered as superior electrolyte materials for application in zinc-ion batteries. For this purpose, we employed dielectric spectroscopy performed in a broad temperature range, extending from the supercooled state at low temperatures up to the liquid phase around room temperature and beyond. We find evidence for a relaxation process arising from dipolar reorientation dynamics, which reveals the clear signatures of glassy freezing. This freezing also governs the temperature dependence of the ionic dc conductivity. We compare the obtained results with those for deep eutectic solvents that are formed by the same hydrogen-bond donor, ethylene glycol, but by two different salts, choline chloride and lithium triflate. The four materials reveal significantly different ionic and reorientational dynamics. Moreover, we find varying degrees of decoupling of rotational dipolar and translational ionic motions, which partly can be described by a fractional Debye-Stokes-Einstein relation. The typical glass-forming properties of these solvents strongly affect their room-temperature conductivity., Comment: 9 pages, 6 figures

Using a combination of resistance fluctuation (noise) and dielectric spectroscopy we investigate the nature of relaxor-type electronic ferroelectricity in the organic conductor $\kappa$-(BETS)$_2$Mn[N(CN)$_2$]$_3$, a system representative for a wider class of materials, where strong correlations of electrons on a lattice of dimerized molecules results in an insulating ground state. The two complementary spectroscopies reveal a distinct low-frequency dynamics. By dielectric spectroscopy we detect an intrinsic relaxation that is typical for relaxor ferroelectrics below the metal-to-insulator transition at $T_{\rm{MI}}\sim 25\,$K. Resistance noise spectroscopy reveals fluctuating two-level processes above $T_{\rm MI}$ which strongly couple to the applied electric field, a signature of fluctuating polar nanoregions (PNR), i.e. clusters of quantum electric dipoles fluctuating collectively. The PNR preform above the metal insulator transition. Upon cooling through $T_{\rm MI}$, a drastic increase of the low-frequency $1/f$-type fluctuations and slowing down of the charge carrier dynamics is accompanied by the onset of strong non-equilibrium dynamics indicating a glassy transition of interacting dipolar clusters, the scaling properties of which are consistent with a droplet model. The freezing of nano-scale polar clusters and non-equilibrium dynamics is suggested to be a common feature of organic relaxor-type electronic ferroelectrics and needs to be considered in theoretical models describing these materials.

We propose a new measurement of the ratio of positron-proton to electron-proton elastic scattering at DESY. The purpose is to determine the contributions beyond single-photon exchange, which are essential for the Quantum Electrodynamic (QED) description of the most fundamental process in hadronic physics. By utilizing a 20 cm long liquid hydrogen target in conjunction with the extracted beam from the DESY synchrotron, we can achieve an average luminosity of $2.12\times10^{35}$ cm$^{-2}\cdot$s$^{-1}\cdot$sr$^{-1}$ ($\approx200$ times the luminosity achieved by OLYMPUS). The proposed TPEX experiment entails a commissioning run at 2 GeV, followed by measurements at 3 GeV, thereby providing new data up to $Q^2=4.6$ (GeV/$c$)$^2$ (twice the range of current measurements). We present and discuss the proposed experimental setup, run plan, and expectations., Comment: 10 pages, 14 figures. arXiv admin note: substantial text overlap with arXiv:2301.04708

The MUSE experiment at the Paul Scherrer Institute is measuring elastic lepton-proton scattering cross sections in a four-momentum transfer range from $Q^2$ of approximately 0.002 to 0.08 GeV$^2$ using positively and negatively charged electrons and muons. The extraction of the Born cross sections from the experimental data requires radiative corrections. Estimates of the instrumental uncertainties in those corrections have been made using the ESEPP event generator. The results depend in particular on the minimum lepton momentum that contributes to the experimental cross section and the fraction of events with hard initial-state radiation that is detected in the MUSE calorimeter and is excluded from the data. These results show that the angular-dependent instrumental uncertainties in radiative corrections to the electron cross section are better than 0.4 % and are negligible for the muon cross section., Comment: Accepted version of the manuscript submitted to the EPJ A Topical Collection on radiative corrections

By using dielectric spectroscopy in a broad range of temperatures and frequencies, we have investigated dipolar relaxations, the dc conductivity, and the possible occurrence of polar order in AgCN. Conductivity contributions dominate the dielectric response at elevated temperatures and low frequencies, most likely arising from the mobility of the small silver ions. In addition, we observe dipolar relaxation dynamics of the dumbbell-shaped CN- ions, whose temperature dependence follows Arrhenius behavior with a hindering barrier of 0.59 eV. It correlates well with a systematic development of the relaxation dynamics with the cation radius, previously observed in various alkali cyanides. By comparison with the latter, we conclude that AgCN does not exhibit a plastic high-temperature phase with a free rotation of the cyanide ions. Instead, our results indicate that a phase with quadrupolar order, revealing dipolar head-to-tail disorder of the CN- ions, exists at elevated temperatures up to the decomposition temperature, which crosses over to long-range polar order of the CN dipole moments below about 475 K. Dipole ordering was also reported for NaCN and KCN and a comparison with these systems suggests a critical relaxation rate of 10^5 - 10^7 Hz marking the onset of dipolar order in the cyanides. The detected relaxation dynamics in this order-disorder type polar state points to glasslike freezing below about 195 K of a fraction of non-ordered CN dipoles., Comment: 14 pages, 4 figures

This White Paper presents the community inputs and scientific conclusions from the Hot and Cold QCD Town Meeting that took place September 23-25, 2022 at MIT, as part of the Nuclear Science Advisory Committee (NSAC) 2023 Long Range Planning process. A total of 424 physicists registered for the meeting. The meeting highlighted progress in Quantum Chromodynamics (QCD) nuclear physics since the 2015 LRP (LRP15) and identified key questions and plausible paths to obtaining answers to those questions, defining priorities for our research over the coming decade. In defining the priority of outstanding physics opportunities for the future, both prospects for the short (~ 5 years) and longer term (5-10 years and beyond) are identified together with the facilities, personnel and other resources needed to maximize the discovery potential and maintain United States leadership in QCD physics worldwide. This White Paper is organized as follows: In the Executive Summary, we detail the Recommendations and Initiatives that were presented and discussed at the Town Meeting, and their supporting rationales. Section 2 highlights major progress and accomplishments of the past seven years. It is followed, in Section 3, by an overview of the physics opportunities for the immediate future, and in relation with the next QCD frontier: the EIC. Section 4 provides an overview of the physics motivations and goals associated with the EIC. Section 5 is devoted to the workforce development and support of diversity, equity and inclusion. This is followed by a dedicated section on computing in Section 6. Section 7 describes the national need for nuclear data science and the relevance to QCD research., Comment: QCD Town Meeting White Paper, as submitted to 2023 NSAC LRP committee on Feb. 28, 2023

Melting is well understood in terms of the Lindemann criterion, essentially stating that crystalline materials melt when the thermal vibrations of their atoms become such vigorous that they shake themselves free of the binding forces. However, how about another common type of solids: glasses, where the nature of the solid-liquid crossover is highly controversial? The Lindemann criterion implies that the thermal expansion coefficients alpha of crystals are inversely proportional to their melting temperatures. Here we find that, unexpectedly, alpha of glasses decreases much stronger with increasing glass-transition temperature Tg marking the liquid-solid crossover in this material class. However, scaling alpha by the fragility m, a measure of particle cooperativity, restores the proportionality, i.e., alpha/m ~ 1/Tg. Obviously, for a glass to become liquid, it is not sufficient to simply overcome the interparticle binding energies. Instead, more energy has to be invested to break up the typical cooperative particle network which is considered a hallmark feature of glassy materials. Surprisingly, alpha of the liquid phase reveals similar anomalous behaviour and is universally enhanced by a constant factor of ~3. The found universalities allow estimating glass-transition temperatures from thermal expansion and vice versa., Comment: 6 pages, 2 figures + Supplementary Information (9 pages, 1 figure, 2 tables). First submitted version of manuscript

In this paper, we describe an experiment measuring low-$Q^2$ elastic electron-proton scattering using a newly developed cryogenic supersonic gas jet target in the A1 three-spectrometer facility at the Mainz Microtron. We measured the proton electric form factor within the four-momentum transfer range of $0.01\le Q^2 \le 0.045(\text{GeV/c})^2$. The experiment showed consistent results with the existing measurements. The data we collected demonstrated the feasibility of the gas jet target and the potential of future scattering experiments using high-resolution spectrometers with this gas jet target., Comment: 10 pages, 8 figures

In many models in economics or business a dominantly self-interested homo economicus is assumed. Unfortunately (or fortunately), humans are in general not homines economici as e.g. the ultimatum game shows. This leads to the fact that all these models are at least doubtful. Moreover, economists started to set a quantitative value for the feeling of social justice, altruism, or envy and the like to execute utilitarian calculation. Besides being ethically doubtful, it delivers an explanation in hindsight with little predicting power. We use examples from game theory to show its arbitrariness. It is even possible that a stable Nash equilibrium can be calculated while it does not exist at all, due to the wide differences in human values. Finally, we show that assigned numbers for envy or altruism and the like do not build a field (in a mathematical sense). As there is no homomorphism to real numbers or a subset of it, any calculation is generally invalid or arbitrary. There is no (easy) way to fix the problem. One has to go back to ethical concepts like the categorical imperative or use at most semi quantitative approaches like considering knaves and knights. Mathematically one can only speculate whether e.g. surreal numbers can make ethics calculable.

We present dielectric, polarization, resistivity, specific heat, and magnetic susceptibility data on single crystals of the lacunar spinels GaNb4Se8 and GaTa4Se8, tetrahedral cluster-based materials with substantial spin-orbit coupling. We concentrate on the possible occurrence of antipolar order in these compounds, as previously reported for the isoelectronic GaNb4S8, where spin-orbit coupling plays a less important role. Our broadband dielectric-spectroscopy investigations reveal clear anomalies of the intrinsic dielectric constant at the magneto-structural transitions in both systems that are in accord with the expectations for antipolar transitions. A similar anomaly is also observed at the cubic-cubic transition of the Nb compound leading to an intermediate phase. Similar to other polar and antipolar lacunar spinels, we find indications for dipolar relaxation dynamics at low temperatures. Polarization measurements on GaNb4Se8 reveal weak ferroelectric ordering below the magneto-structural transition, either superimposed to antipolar order or emerging at structural domain walls. The temperature-dependent dc resistivity evidences essentially thermally-activated charge transport with different activation energies in the different phases. A huge step-like increase of the resistivity at the magneto-structural transition of the Ta compound points to a fundamental change in the electronic structure or the mechanism of the charge transport. At low temperatures, charge transport is governed by in-gap impurity states, as also invoked to explain the resistive switching in these compounds., Comment: 9 pages, 7 figures. Revised version as accepted for publication in Phys. Rev. B

Atomically sharp domain walls (DWs) in ferroelectrics are considered as an ideal platform to realize easy-to-reconfigure nanoelectronic building blocks, created, manipulated and erased by external fields. However, conductive DWs have been exclusively observed in oxides, where DW mobility and conductivity is largely influenced by stoichiometry and defects. In contrast, we here report on conductive DWs in the non-oxide ferroelectric GaV$_4$S$_8$, where charge carriers are provided intrinsically by multivalent V$_4$ molecular clusters. We show that this new mechanism gives rise to DWs composed of nanoscale stripes with alternating electron and hole conduction, unimaginable in oxides. By exerting magnetic control on these segments we promote the mobile and effectively 2D DWs into dominating the 3D conductance, triggering abrupt conductance changes as large as eight orders of magnitude. The flexible valency, as origin of these novel hybrid DWs with giant conductivity, demonstrates that non-oxide ferroelectrics can be the source of novel phenomena beyond the realm of oxide electronics., Comment: 8 pages, 4 figures

Lithium-salt-based deep eutectic solvents, where the only cation is Li+, are promising candidates as electrolytes in electrochemical energy-storage devices like batteries. We have performed broadband dielectric spectroscopy on three such systems, covering a broad temperature and dynamic range that extends from the low-viscosity liquid around room temperature down to the glassy state approaching the glass-transition temperature. We detect a relaxational process that can be ascribed to dipolar reorientational dynamics and exhibits the clear signatures of glassy freezing. We find that the temperature dependence of the ionic dc conductivity and its room-temperature value also are governed by the glassy dynamics of these systems, depending, e.g., on the glass-transition temperature and fragility. Compared to the previously investigated corresponding systems, containing choline chloride instead of a lithium salt, both the reorientational and ionic dynamics are significantly reduced due to variations of the glass-transition temperature and the higher ionic potential of the lithium ions. These lithium-based deep eutectic solvents partly exhibit significant decoupling of the dipolar reorientational and the ionic translational dynamics and approximately follow a fractional Debye-Stokes-Einstein relation, leading to an enhancement of the dc conductivity, especially at low temperatures. The presented results clearly reveal the importance of decoupling effects and of the typical glass-forming properties of these systems for the technically relevant room-temperature conductivity., Comment: 12 pages, 8 figures. Revised version as accepted for publication in J. Chem. Phys

A cryogenic supersonic gas jet target was developed for the MAGIX experiment at the high-intensity electron accelerator MESA. It will be operated as an internal, windowless target in the energy-recovering recirculation arc of the accelerator with different target gases, e.g., hydrogen, deuterium, helium, oxygen, argon, or xenon. Detailed studies have been carried out at the existing A1 multi-spectrometer facility at the electron accelerator MAMI. This paper focuses on the developed handling procedures and diagnostic tools, and on the performance of the gas jet target under beam conditions. Considering the special features of this type of target, it proves to be well suited for a new generation of high-precision electron scattering experiments at high-intensity electron accelerators.

Lacunar spinels with a chemical formula of $AM_4X_8$ form a populous family of narrow-gap semiconductors, which offer a fertile ground to explore correlation and quantum phenomena, including transition between Mott and spin-orbit insulator states, ferro/antiferroelectricity driven by cluster Jahn-Teller effect, and magnetoelectric response of magnetic skyrmions with polar dressing. The electronic and magnetic properties of lacunar spinels are determined to a large extent by their molecular-crystal-like structure. The interplay of electronic correlations with spin-orbit and vibronic couplings leads to a complex electronic structure already on the single-cluster level, which -- together with weaker inter-cluster interactions -- gives rise to a plethora of unconventional correlated states. This review primarily focuses on recent progresses in the field of optical, dielectric, and magnetoelectric properties on lacunar spinels. After introducing the main structural aspects, lattice dynamics and electronic structure of these compounds are discussed on the basis of optical spectroscopy measurements. Dielectric and polarization studies reveal the main characteristics of their low-temperature ferro- or antiferroelectric phases as well as orbital fluctuations in their high-temperature cubic state. Strong couplings between spin, lattice, and orbital degrees of freedom are manifested in singlet formation upon magnetostructural transitions, the emergence of various multiferroic phases, and exotic domain-wall functionalities.

This review summarizes more than 100 years of research on spinel compounds, mainly focusing on the progress in understanding their magnetic, electronic, and polar properties during the last two decades. Many spinel compounds are magnetic insulators or semiconductors; however, a number of spinel-type metals exists including superconductors and some rare examples of d-derived heavy-fermion compounds. In the early days, they gained importance as ferrimagnetic or even ferromagnetic insulators with relatively high saturation magnetization and high ordering temperatures, with magnetite being the first magnetic mineral known to mankind. However, spinels played an outstanding role in the development of concepts of magnetism, in testing and verifying the fundamentals of magnetic exchange, in understanding orbital-ordering and charge-ordering phenomena. In addition, the A- site as well as the B-site cations in the spinel structure form lattices prone to strong frustration effects resulting in exotic ground-state properties. In case the A-site cation is Jahn-Teller active, additional entanglements of spin and orbital degrees of freedom appear, which can give rise to a spin-orbital liquid or an orbital glass state. The B-site cations form a pyrochlore lattice, one of the strongest contenders of frustration in three dimensions. In addition, in spinels with both cation lattices carrying magnetic moments, competing magnetic exchange interactions become important, yielding ground states like the time-honoured triangular Yafet-Kittel structure. Finally, yet importantly, there exists a long-standing dispute about the possibility of a polar ground state in spinels, despite their reported overall cubic symmetry. Indeed, over the years number of multiferroic spinels were identified., Comment: 118 pages, 60 figures

We present an extension and revision of the spectroscopic and structural data of the mixed stack charge transfer (CT) crystal 3,3$^\prime$,5,5$^\prime$-tetramethylbenzidine--tetrafluoro-tetracyanoquinodimethane (TMB-TCNQF4), associated with new electric and dielectric measurements. Refinement of syncrotron structural data at low temperature has led to revise the previously reported [Phys. Rev. Mat. 2, 024602 (2018)] $C2/m$ structure. The revised structure is $P2_1/m$, with two dimerized stacks per unit cell, and is consistent with the vibrational data. However, polarized Raman data in the low-frequency region also indicate that by increasing temperature above 200 K the structure presents an increasing degree of disorder mainly along the stack axis. X-ray diffraction data at room temperature have confirmed that the correct structure is $P2_1/m$ -- no phase transitions -- but did not allow to definitely substantiate the presence of disorder. On the other hand, dielectric measurement have evidenced a typical relaxor ferroelectric behavior already at room temperature, with a peak in real part of dielectric constant $\epsilon'(T,\nu)$ around 200 K and 0.1 Hz. The relaxor behavior is explained in terms of the presence of spin solitons separating domains of opposite polarity that yield to ferroelectric nanodomains. TMB-TCNQF4 is confirmed to be a narrow gap band semiconductor ($E_a \sim 0.3$ eV) with room temperature conductivity of $\sim 10^{-4}~ \Omega^{-1}$ cm$^{-1}$., Comment: 21 pages, including the Supporting Information in the same file. Version 3 updates the x-ray structural data at room temperature

Geometrical frustration among interacting spins combined with strong quantum fluctuations destabilize long-range magnetic order in favour of more exotic states such as spin liquids. By following this guiding principle, a number of spin liquid candidate systems were identified in quasi-two-dimensional (quasi-2D) systems. For 3D, however, the situation is less favourable as quantum fluctuations are reduced and competing states become more relevant. Here we report a comprehensive study of thermodynamic, magnetic and dielectric properties on single crystalline and pressed-powder samples of PbCuTe$_2$O$_6$, a candidate material for a 3D frustrated quantum spin liquid featuring a hyperkagome lattice. Whereas the low-temperature properties of the powder samples are consistent with the recently proposed quantum spin liquid state, an even more exotic behaviour is revealed for the single crystals. These crystals show ferroelectric order at $T_{\text{FE}} \approx 1\,\text{K}$, accompanied by strong lattice distortions, and a modified magnetic response -- still consistent with a quantum spin liquid -- but with clear indications for quantum critical behaviour., Comment: 59 pages, 15 figures, This version of the article has been accepted for publication, after peer review but is not the Version of Record and does not reflect post-acceptance improvements, or any corrections. The Version of Record is available online

We performed rheological measurements of the typical deep eutectic solvents (DESs) glyceline, ethaline, and reline in a very broad temperature and dynamic range, extending from the low-viscosity to the high-viscosity supercooled-liquid regime. We find that the mechanical compliance spectra can be well described by the random free-energy barrier hopping model, while the dielectric spectra on the same materials involve significant contributions arising from reorientational dynamics. The temperature-dependent viscosity and structural relaxation time, revealing non-Arrhenius behavior typical for glassy freezing, are compared to the ionic dc conductivity and relaxation times determined by broadband dielectric spectroscopy. For glyceline and ethaline we find essentially identical temperature dependences for all dynamic quantities. These findings point to a close coupling of the ionic and molecular translational and reorientational motions in these systems. However, for reline the ionic charge transport appears decoupled from the structural and reorientational dynamics, following a fractional Walden rule. Especially, at low temperatures the ionic conductivity in this DES is enhanced by about one decade compared to expectations based on the temperature dependence of the viscosity. The results for all three DESs can be understood without invoking a revolving-door mechanism previously considered as a possible charge-transport mechanism in DESs., Comment: final accepted version of the manuscript

The light collection of several fiber configurations embedded in a box-shaped plastic scintillating counter was studied by scanning with minimum ionizing electrons. The light was read out by silicon photomultipliers at both ends. The light yield produced by the 855-MeV beam of the Mainz Microtron showed a strong dependence on the transverse distance from the beam position to the fibers. The observations were modeled by attributing the collection of indirect light inside of the counter and of direct light reaching a fiber to the total light yield. The light collection with fibers was compared to that of a scintillating counter without fibers. These studies were carried out within the development of plastic scintillating detectors as an active veto system for the DarkMESA electron beam-dump experiment that will search for light dark matter particles in the MeV mass range., Comment: 13 pages, 7 figures, 2 tables

Local-probe imaging of the ferroelectric domain structure and auxiliary bulk pyroelectric measurements were conducted at low temperatures with the aim to clarify the essential aspects of the orbitally driven phase transition in GaMo4S8, a lacunar spinel crystal that can be viewed as a spin-hole analogue of its GaV4S8 counterpart. We employed multiple scanning probe techniques combined with symmetry and mechanical compatibility analysis to uncover the hierarchical domain structures, developing on the 10-100 nm scale. The identified domain architecture involves a plethora of ferroelectric domain boundaries and junctions, including primary and secondary domain walls in both electrically neutral and charged configurations, and topological line defects transforming neutral secondary walls into two oppositely charged ones., Comment: This is the Accepted Manuscript version of an article accepted for publication in Journal of Physics: Condensed Matter. IOP Publishing Ltd is not responsible for any errors or omissions in this version of the manuscript or any version derived from it. The Version of Record is available online at https://doi.org/10.1088/1361-648X/aae448

A recently published analytical model, describing and predicting elasticity, viscosity, and fragility of metallic melts, is applied for the analysis of about 30 nonmetallic glassy systems, ranging from oxide network glasses to alcohols, low-molecular-weight liquids, polymers, plastic crystals, and even ionic glass formers. The model is based on the power-law exponent lambda representing the steepness parameter of the repulsive part of the inter-atomic or -molecular potential and the thermal-expansion parameter alpha_T determined by the attractive anharmonic part of the effective interaction. It allows fitting the typical super-Arrhenius temperature variation of the viscosity or dielectric relaxation time for various classes of glass-forming matter, over many decades. We discuss the relation of the model parameters found for all these different glass-forming systems to the fragility parameter m and detect a correlation of lambda and m for the non-metallic glass formers, in accord with the model predictions. Within the framework of this model, thus the fragility of glass formers can be traced back to microscopic model parameters characterizing the intermolecular interactions., Comment: 11 pages, 4 figures + Supplemental Material (9 pages, 11 figures). This article has been accepted by J. Chem. Phys. After it is published, it will be found at https://doi.org/10.1063/5.0014457

Within the so-called "no-man's land" between about 150 and 235 K, crystallization of bulk water is inevitable. The glasslike freezing and a liquid-to-liquid transition of water, predicted to occur in this region, can be investigated by confining water in nanometer-sized pores. Here we report the molecular dynamics of water within the pores of a metal-organic framework using dielectric spectroscopy. The detected temperature-dependent dynamics of supercooled water matches that of bulk water as reported outside the borders of the no-man's land. In confinement, a different type of water is formed, nevertheless still undergoing a glass transition with considerable molecular cooperativity. Two different length scales seem to exist in water: A smaller one, of the order of 2 nm, being the cooperativity length scale governing glassy freezing, and a larger one (> 2 nm), characterizing the minimum size of the hydrogen-bonded network needed to create "real" water with its unique dynamic properties, Comment: This is a pre-print of an article published in "Communication Physics". The final authenticated version is available online at: https://doi.org/10.1038/s42005-020-0363-x"

We report the observation of an antipolar phase in cubic GaNb$_4$S$_8$ driven by an unconventional microscopic mechanism, the cooperative Jahn-Teller effect of Nb$_4$S$_4$ molecular clusters. The assignment of the antipolar nature is based on sudden changes in the crystal structure and a strong drop of the dielectric constant at $T_\mathrm{JT}=31$\,K, also indicating the first-order nature of the transition. In addition, we found that local symmetry lowering precedes long-range orbital ordering, implying the presence of a dynamic Jahn-Teller effect in the cubic phase above $T_\mathrm{JT}$. Based on the variety of structural polymorphs reported in lacunar spinels, also including ferroelectric phases, we argue that GaNb$_4$S$_8$ may be transformable to a ferroelectric state, which would further classify the observed antipolar phase as antiferrolectric.

We investigated the mixed-stack charge-transfer crystal, N,N'-dimethylphenazine-TCNQ (M$_2$P-TCNQ), which is polar at room temperature and just at the neutral-to-ionic interface (ionicity $\rho \approx 0.5$). We detect the typical dielectric signature of a relaxor ferroelectric and an asymmetric positive-up-negative-down behavior. While relaxor ferroelectricity is usually ascribed to disorder in the crystal, we find no evidence for structural disorder in the investigated crystals. To elucidate the origin of M$_2$P-TCNQ's dielectric properties we perform parallel structural and spectroscopic measurements, associated with theoretical modeling and quantum-mechanical calculations. Our combined effort points to a highly polarizable electronic system that is strongly coupled to lattice vibrations. The found indications for polarization reversal imply flipping of the bent conformation of the M$_2$P molecule with an associated energy barrier of a few tens of an eV, broadly consistent with an Arrhenius fit of the dielectric relaxation times. While the polarization is mostly of electronic origin, its possible reversal implies slow collective motions that are affected by solid-state intermolecular interactions., Comment: 13 pages, 12 figures

We have performed a dielectric investigation of the ionic charge transport and the relaxation dynamics in plastic-crystalline 1-cyano-adamantane (CNA) and in two mixtures of CNA with the related plastic crystals adamantane or 2-adamantanon. Ionic charge carriers were provided by adding 1% of Li salt. The molecules of these compounds have nearly globular shape and, thus, the so-called revolving-door mechanism assumed to promote ionic charge transport via molecular reorientations in other PC electrolytes, should not be active here. Indeed, a comparison of the dc resistivity and the reorientational alpha-relaxation times in the investigated PCs, reveals complete decoupling of both dynamics. Similar to other PCs, we find a significant mixing-induced enhancement of the ionic conductivity. Finally, these solid-state electrolytes reveal a second relaxation process, slower than the alpha-relaxation, which is related to ionic hopping. Due to the mentioned decoupling, it can be unequivocally detected and is not superimposed by the reorientational contributions as found for most other ionic conductors., Comment: 9 pages, 7 figures

We report on a new measurement of the beam-normal single spin asymmetry $A_{\mathrm{n}}$ in the elastic scattering of 570 MeV transversely polarized electrons off $^{28}$Si and $^{90}$Zr at $Q^{2}=0.04\, \mathrm{GeV}^2/c^2$. The studied kinematics allow for a comprehensive comparison with former results on $^{12}$C. No significant mass dependence of the beam-normal single spin asymmetry is observed in the mass regime from $^{12}$C to $^{90}$Zr., Comment: Submitted for publication to Physics Letters B

H3LiIr2O6 is the first honeycomb-lattice system without any signs of long-range magnetic order down to the lowest temperatures, raising the hope for the realization of an ideal Kitaev quantum spin liquid. Its honeycomb layers are coupled by interlayer hydrogen bonds. Static or dynamic disorder of these hydrogen bonds was proposed to strongly affect the magnetic exchange and to make Kitaev-type interactions dominant. Using dielectric spectroscopy, here we provide experimental evidence for dipolar relaxations in H3LiIr2O6 and deuterated D3LiIr2O6, which mirror the dynamics of protons and deuterons within the double-well potentials of the hydrogen bonds. The detected hydrogen dynamics reveals glassy freezing, characterized by a strong slowing down under cooling, with a crossover from thermally-activated hopping to quantum-mechanical tunneling towards low temperatures. Thus, besides being Kitaev quantum-spin-liquid candidates, these materials also are quantum paraelectrics. However, the small relaxation rates in the mHz range, found at low temperatures, practically realize quasi-static hydrogen disorder, as assumed in recent theoretical works to explain the quantum-spin-liquid ground state of both compounds., Comment: 10 pages, 8 figures

We report a magnetic state in GaV$_4$Se$_8$ which emerges exclusively in samples with mesoscale polar domains and not in polar mono-domain crystals. Its onset is accompanied with a sharp anomaly in the magnetic susceptibility and the magnetic torque, distinct from other anomalies observed also in polar mono-domain samples upon transitions between the cycloidal, the N\'eel-type skyrmion lattice and the ferromagnetic states. We ascribe this additional transition to the formation of magnetic textures localized at structural domain walls, where the magnetic interactions change stepwise and spin textures with different spiral planes, hosted by neighbouring domains, need to be matched. A clear anomaly in the magneto-current indicates that the domain-wall-confined magnetic states also have strong contributions to the magnetoelectric response. We expect polar domain walls to commonly host such confined magnetic edge states, especially in materials with long wavelength magnetic order.

Broad-band dielectric spectroscopy, heat capacity measurements and molecular dynamic simulations are applied to study excitations of interacting electric dipoles spatially arranged in a network with an inter-dipole distance of 5-10 A. The dipoles with magnitude of 1.85 Debye are represented by single H2O molecules located in voids (0.5 nm size) formed by ions of the crystal lattice of cordierite. We discover emergence of nontrivial disordered paraelectric phase of dipolar system with signs of phase transition below 3 K., Comment: 3 pages, 4 figures

We investigate the dielectric response in the glass-electret state of two dipolar glass-forming materials. This unusual polar glassy state of matter is produced when a dipolar liquid is supercooled under the influence of a high electric dc field, which leads to partial orientational order of the molecules carrying a dipole moment. Investigation of the prepared glass-electrets by using low-field dielectric spectroscopy reveals a clear modification of their dielectric response in the regime of the Johari-Goldstein beta-relaxation, pointing to a small but significant increase of its relaxation strength compared to the normal glass. We discuss the implications of this finding for the still controversial microscopic interpretation of the Johari-Goldstein relaxation, an inherent property of glassy matter., Comment: 5 pages, 4 figures + Supplemental Material (3 pages, 5 figures); revised version as accepted for publication in Phys. Rev. Materials

MAGIX is a planned experiment that will be implemented at the upcoming accelerator MESA in Mainz. Due to its location in the energy-recovering lane of the accelerator beam-currents up to 1mA with a maximum energy of 105 MeV will be available for precision experiments. MAGIX itself consists of a jet-target and two magnetic spectrometers. Inside the spectrometers GEM-based detectors will be used in the focal plane for track reconstruction. The design goals for the detector modules are a spatial resolution of 50 um, a size of 1.20 m x 0.3 m and a minimal material budget. To accomplish these goals we started developing several GEM-prototypes to study different behaviors and techniques to optimize the final detector design. The GEM foils used are provided by CERN and are trained, stretched and framed in our laboratory. The readout is done with an SRS based system. In this contribution the requirements, achievements and the ongoing developments are presented., Comment: Prepared for submission to JINST

Many plastic crystals, molecular solids with long-range, center-of-mass crystalline order but dynamic disorder of the molecular orientations, are known to exhibit exceptionally high ionic conductivity. This makes them promising candidates for applications as solid-state electrolytes, e.g., in batteries. Interestingly, it was found that the mixing of two different plastic-crystalline materials can considerably enhance the ionic dc conductivity, an important benchmark quantity for electrochemical applications. An example is the admixture of different nitriles to succinonitrile, the latter being one of the most prominent plastic-crystalline ionic conductors. However, until now only few such mixtures were studied. In the present work, we investigate succinonitrile mixed with malononitrile, adiponitrile, and pimelonitrile, to which 1 mol% of Li ions were added. Using differential scanning calorimetry and dielectric spectroscopy, we examine the phase behavior and the dipolar and ionic dynamics of these systems. We especially address the mixing-induced enhancement of the ionic conductivity and the coupling of the translational ionic mobility to the molecular reorientational dynamics, probably arising via a "revolving-door" mechanism., Comment: 9 pages, 7 figures; revised version as accepted for publication in J. Chem. Phys

Spin liquids may host emergent quasiparticles, collective excitations of the spin degrees of freedom with characteristic features of Majorana fermions, which experimentally are detectable by broad excitation continua due to spin fractionalization. The latter is predicted for the Kitaev spin liquid, an exactly solvable model with bond-dependent interactions on a two-dimensional honeycomb lattice. Here we report on detailed THz experiments in {\alpha}-RuCl3, identifying these characteristic fingerprints of Majorana fermions. The continuum intensity decreases and finally vanishes on increasing temperature. It partly overlaps with phonon modes representing characteristic sliding and compression modes of the van der Waals bonded molecular layers., Comment: 6 pages, 4 figures