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Alois Loidl

Publications and source records attributed to Alois Loidl.

At least 19 recordsLinked to original sources

The 2/3 Rule of Glass Physics Implies Universalities in Crystal Melting

Since more than 100 years, melting is thought to be governed by the Lindemann criterion. It assumes that a crystal melts when, upon heating, the growing atomic vibration amplitudes become sufficiently large to destabilize its crystalline lattice. However, it is unclear why the viscosities eta or the related relaxation times tau of the resulting liquids, measured directly at the melting point Tm, differ by up to nine decades, depending on the material. Based on the empirical rule that the ratio of the glass-transition temperature and Tm is about 2/3, here we show that this strong variation is due to differences in the liquid's fragilities, a property associated with pronounced non-Arrhenius behavior and often ascribed to cooperative motions. We propose that, without cooperativity, all crystals would melt into liquids with a universal viscosity value and relaxation time. Hence, the real melting point is only partly determined by the Lindemann criterion and strongly enhanced by the cooperativity of the resulting liquid. Our findings are corroborated by the determination of the idealized, fragility-free melting temperatures, and of the corresponding eta and tau values for various example materials.

cond-mat.soft

Broadband Dielectric and THz Spectroscopy on Bio-Related Matter: Water, Amino Acids, Proteins, and Blood

In the present work, we examine the relevance and proper interpretation of broadband-dielectric and THz-spectroscopy data for the investigation of various types of biological matter. We provide an overview of the rich variety of different dynamic processes that can be detected by these experimental methods. Several experimental examples are discussed in detail, helping to understand the information that can be drawn from such studies. This includes dielectric spectra, extending well into the GHz region, for pure water, which can be considered as a simple but highly important biological molecule. We also discuss results for a prototypical aqueous solution of a protein, belonging to one of the most important classes of biological macromolecules. Moreover, we examine broadband dielectric spectra on blood as an example of functional biological matter in organisms. To demonstrate the relevance of THz spectroscopy for the investigation of biological molecules, we finally treat such experiments applied to different amino acids.

cond-mat.soft

Exploring water's no-man's land

The investigation of water's glass transition and a possible liquid-liquid transition within its supercooled state is hampered by its inevitable crystallization in a temperature range, termed "no-man's land". Here we report dielectric-spectroscopy and calorimetry measurements of pure water and various aqueous LiCl solutions, part of the latter being quenched to avoid crystallization. By investigating solutions of relatively low salt content and by covering an exceptionally broad frequency range up to THz, we find strong hints at a crossover in water from a strong to a fragile liquid, characterized by different glass-transition temperatures and different non-Arrhenius temperature dependences of the molecular dynamics.

cond-mat.soft

Experimental observation of repulsively bound magnons

Stable composite objects, such as hadrons, nuclei, atoms, molecules and superconducting pairs, formed by attractive forces are ubiquitous in nature. By contrast, composite objects stabilized by means of repulsive forces were long thought to be theoretical constructions owing to their fragility in naturally occurring systems. Surprisingly, the formation of bound atom pairs by strong repulsive interactions has been demonstrated experimentally in optical lattices. Despite this success, repulsively bound particle pairs were believed to have no analogue in condensed matter owing to strong decay channels. Here we present spectroscopic signatures of repulsively bound three-magnon states and bound magnon pairs in the Ising-like chain antiferromagnet BaCo$_2$V$_2$O$_8$. In large transverse fields, below the quantum critical point, we identify repulsively bound magnon states by comparing terahertz spectroscopy measurements to theoretical results for the Heisenberg-Ising chain antiferromagnet, a paradigmatic quantum many-body model. Our experimental results show that these high-energy repulsively bound magnon states are well separated from continua, exhibit significant dynamical responses and, despite dissipation, are sufficiently long-lived to be identified. As the transport properties in spin chains can be altered by magnon bound states, we envision such states could serve as resources for magnonics based quantum information processing technologies.

cond-mat.str-el

Relaxation dynamics of poly(ethylene oxide)

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.

cond-mat.soft

Magnetism of CuCr$_2$X$_4$ (X= S and Se) spinels studied with muon spin rotation and relaxation ($μ$SR)

We present muon spin rotation and relaxation ($μ$SR) results for chalcogenide spinels CuCr$_2$X$_4$ with X= S and Se. Both compounds are known as ferromagnetic metals with high Curie temperatures. Our $μ$SR and magnetization data show clear signatures for additional magnetic transitions far below the respective Curie temperatures. They can be related to changes in the Cr valence system from the mixed valence between Cr$^{3+}$ and Cr$^{4+}$ at high temperatures with collinear ferromagnetism to a charge-ordered state at low temperatures with a different ferromagnetic structure. Our results demonstrate that the electronic systems and the related spin structures of both compounds are more complex than assumed so far.

cond-mat.str-el

Prigogine-Defay ratio of glassy freezing scales with liquid fragility

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.

cond-mat.soft

THz spectroscopy on amino acids

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.

cond-mat.mtrl-sci

Chiral excitations and the intermediate-field spin-liquid regime in the Kitaev magnet $α$-RuCl$_3$

In the Kitaev magnet $α$-RuCl$_3$, the existence of a magnetic-field-induced quantum spin liquid phase and of anyonic excitations are discussed controversially. We address this elusive, exotic phase via helicity-dependent Raman scattering and analyze the Raman optical activity of excitations as a function of magnetic field and temperature. The hotly debated field regime between 7.5 T and 10.5 T is characterized by clear spectroscopic signatures such as a plateau of the Raman optical activity of the dominant, chiral spin-flip excitation. This provides direct evidence for the existence of a distinct intermediate field regime compatible with a quantum spin liquid phase.

cond-mat.str-el

Nonequilibrium dynamics of $α$-RuCl$_{3}$ -- a time-resolved magneto-optical spectroscopy study

We present time-resolved magneto-optical spectroscopy on the magnetic Mott-Hubbard-insulating Kitaev spin liquid candidate $α$-RuCl$_3$ to investigate the nonequilibrium dynamics of its antiferromagnetically ordered zigzag groundstate after photoexcitation. A systematic study of the transient magnetic linear dichroism under different experimental conditions (temperature, external magnetic field, photoexcitation density) gives direct access to the dynamical interplay of charge excitations with the zigzag ordered state on ultrashort time scales. We observe a rather slow initial demagnetization (few to 10s of ps) followed by a long-lived non-thermal antiferromagnetic spin-disordered state (100$-$1000s of ps), which can be understood in terms of holons and doublons disordering the antiferromagnetic background after photoexcitation. Varying temperature and fluence in the presence of an external magnetic field reveals two distinct photoinduced dynamics associated with the zigzag and quantum paramagnetic disordered phases. The photo-induced non-thermal spin-disordered state shows universal compressed-exponential recovery dynamics related to the growth and propagation of zigzag domains on nanosecond time scales, which is interpreted within the framework of the Fatuzzo-Labrune model for magnetization reversal. The study of nonequilibrium states in strongly correlated materials is a relatively unexplored topic, but our results are expected to be extendable to a large class of Mott-Hubbard insulator materials with strong spin-orbit coupling.

cond-mat.str-el

Magneto-optical study of metamagnetic transitions in the antiferromagnetic phase of $α$-RuCl$_3$

$α$-RuCl$_3$ is a promising candidate material to realize the so far elusive quantum spin liquid ground state. However, at low temperatures, the coexistence of different exchange interactions couple the effective pseudospins into an antiferromagnetically zigzag (ZZ) ordered state. The low-field evolution of spin structure is still a matter of debate and the magnetic anisotropy within the honeycomb planes is an open and challenging question. Here, we investigate the evolution of the ZZ order parameter by second-order magneto-optical effects, the magnetic linear dichroism and magnetic linear birefringence. Our results clarify the presence and nature of metamagnetic transitions in the ZZ phase of $α$-RuCl$_3$. Our experimental observations show the presence of initial magnetic domain repopulation followed by a spin-flop transition for small in-plane applied magnetic fields ($\approx$ 1.6 T) along specific crystallographic directions. In addition, using a magneto-optical approach, we detected the recently reported emergence of a field-induced intermediate phase before suppressing the ZZ order. Our results disclose the details of various angle-dependent in-plane metamagnetic transitions quantifying the bond-anisotropic interactions present in $α$-RuCl$_3$

cond-mat.str-el

Supercooled water confined in a metal-organic framework

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

cond-mat.soft

Universal correlations between the fragility and interparticle repulsion of glass-forming liquids

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.

cond-mat.dis-nn

Enhancement of magnetodielectric coupling in 6H-perovskites Ba3RRu2O9 for heavier rare earth cations (R=Ho,Tb)

The role of rare-earth (R) ions on the magnetodielectric (MD) coupling is always intriguing and markedly different for different systems. Although many reports are available concerning this aspect in frustrated 3d-transition metal oxides, no such reports exist on higher d (4d/5d)-orbital based systems due to the rare availability of highly insulating 4d/5d-systems. Here, we systematically investigated the magnetic, dielectric, ferroelectric and magnetodielectric behavior of the 6H-perovskites Ba3RRu2O9 for different R-ions, namely, R= Sm, Tb and Ho, which magnetically order at 12, 9.5 and 10.2 K respectively. For R=Tb and Ho, the temperature and magnetic-field dependent complex dielectric constant traces the magnetic features, which manifests MD coupling in this system. A weak magnetic-field (H) induced transition is observed for ~30 kOe, which is clearly captured in H-dependent dielectric measurements. No MD coupling is observed for Ba3SmRu2O9. The MD coupling is enhanced by a factor of 3 and 20 times for R=Tb and Ho, respectively, when compared to that of the Nd-counterpart. These results evidence the gradual enhancement of MD coupling with the introduction of heavier R-ions in this series, which is attributed to their larger moment values. A weak improper ferroelectricity is documented for Ho-member, which is absent for Nd. Our investigation establishes dominating 4d(Ru)-4f(R) magnetic correlation in this series for the heavier R-members.

cond-mat.str-el

Manipulating surface magnetic order in iron telluride

Control of emergent magnetic orders in correlated electron materials promises new opportunities for applications in spintronics. For their technological exploitation, it is important to understand the role of surfaces and interfaces to other materials and their impact on the emergent magnetic orders. Here, we demonstrate for iron telluride, the nonsuperconducting parent compound of the iron chalcogenide superconductors, determination and manipulation of the surface magnetic structure by low-temperature spin-polarized scanning tunneling microscopy. Iron telluride exhibits a complex structural and magnetic phase diagram as a function of interstitial iron concentration. Several theories have been put forward to explain the different magnetic orders observed in the phase diagram, which ascribe a dominant role either to interactions mediated by itinerant electrons or to local moment interactions. Through the controlled removal of surface excess iron, we can separate the influence of the excess iron from that of the change in the lattice structure.

cond-mat.str-el

Chirality-driven ferroelectricity in LiCuVO$_4$

Chirality or the handedness of objects is of prime importance in life science, biology, chemistry and physics. It is also a major symmetry ingredient in frustrated magnets revealing spin-spiral ground states. Vector chiral phases, with the twist (either clock- or counter clock-wise) between neighbouring spins being ordered, but with disorder with respect to the angles between adjacent spins, have been predicted almost five decades ago. Experimental proofs, however, are rare and controversial. Here, we provide experimental evidence for such a phase in LiCuVO$_4$, a one-dimensional quantum magnet with competing ferromagnetic and antiferromagnetic interactions. The vector chiral state is identified via a finite ferroelectric polarization arising at temperatures well above the multiferroic phase exhibiting long-range three-dimensional spin-spiral and polar order. On increasing temperatures, spin order becomes suppressed at TN, while chiral long-range order still exist, leaving a temperature window with chirality-driven ferroelectricity in the presence of an external magnetic field.

cond-mat.str-el

Multiferroic spin-superfluid and spin-supersolid phases in MnCr2S4

Spin supersolids and spin superfluids reveal complex canted spin structures with independent order of longitudinal and transverse spin components. This work addresses the question whether these exotic phases can exhibit spin-driven ferroelectricity. Here we report the results of dielectric and pyrocurrent measurements of MnCr2S4 as function of temperature and magnetic field up to 60 T. This sulfide chromium spinel exhibits a Yafet-Kittel type canted spin structure at low temperatures. As function of external magnetic field, the manganese spins undergo a sequence of ordering patterns of the transverse and longitudinal spin components, which can be mapped onto phases as predicted by lattice-gas models including solid, liquid, super-fluid, and supersolid phases. By detailed dielectric and pyrocurrent measurements, we document a zoo of multiferroic phases with sizable ferroelectric polarization strongly varying from phase to phase. Using lattice-gas terminology, the title compound reveals multiferroic spin-superfluid and spin-supersolid phases, while the antiferromagnetic solid is paraelectric.

cond-mat.str-el

High-resolution neutron depolarization microscopy of the ferromagnetic transitions in Ni$_3$Al and HgCr$_2$Se$_4$ under pressure

We performed neutron imaging of ferromagnetic transitions in Ni$_3$Al and HgCr$_2$Se$_4$ crystals. These neutron depolarization measurements revealed bulk magnetic inhomogeneities in the ferromagnetic transition temperature with spatial resolution of about 100~$μ$m. To obtain such spatial resolution, we employed a novel neutron microscope equipped with Wolter mirrors as a neutron image-forming lens and a focusing neutron guide as a neutron condenser lens. The images of Ni$_3$Al show that the sample does not homogeneously go through the ferromagnetic transition; the improved resolution allowed us to identify a distribution of small grains with slightly off-stoichiometric composition. Additionally, neutron depolarization imaging experiments on the chrome spinel, HgCr$_2$Se$_4$, under pressures up to 15~kbar highlight the advantages of the new technique especially for small samples or sample environments with restricted sample space. The improved spatial resolution enables one to observe domain formation in the sample while decreasing the acquisition time despite having a bulky pressure cell in the beam.

cond-mat.str-el