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Bastian Klemke

Publications and source records attributed to Bastian Klemke.

12 recordsLinked to original sources

Emergent hidden order in ice: frustration and glassiness from slow hydrogen dynamics

Frustrated systems can host hidden order, in which weak interactions select correlated structure from a highly degenerate manifold. Water ice Ih is the canonical example of such a manifold, yet whether its hydrogen disorder conceals local structure beyond the Bernal-Fowler ice rules has remained controversial. Here, using high-resolution inelastic neutron scattering on single-crystal heavy ice, we identify strongly anisotropic librational phonons dispersing uniaxially along the crystallographic c axis - a spectroscopic signature inaccessible to bulk-averaging probes. A physics-guided analysis reveals that these excitations encode a hidden partial order: correlated polar armchair chains driven by a shallow stereochemical bias that creates an imperfectly flat energy landscape. This bias promotes nanoscale polar domains, yet frustrated topology prevents their straightforward coarsening into the ice XI ground state, trapping the system in a rugged configurational landscape that, within the experimentally constrained model, retains finite residual entropy even in the limit of infinitely slow cooling. These findings show that ice Ih is not a simple disordered solid, but a frustrated, partially ordered hydrogen network with glass-like arrest on a crystalline lattice, providing a microscopic framework that reconciles thermodynamic theory with spectroscopic observations.

cond-mat.mtrl-sci

An ultra-low field SQUID magnetometer for measuring antiferromagnetic and weakly remanent magnetic materials at low temperatures

A novel setup for the measurement of magnetic fields external to certain antiferromagnets and generally weakly remanent magnetic materials is presented. The setup features a highly sensitive Super Conducting Quantum Interference Device (SQUID) magnetometer with a magnetic field resolution of approx. 10 fT, non-electric thermalization of the sample space for a temperature range of 1.5 - 65 K with a non-electric sample movement drive and optical position encoding. To minimize magnetic susceptibility effects, the setup components are degaussed and realized with plastic materials in sample proximity. Running the setup in magnetically shielded rooms allows for a well-defined ultra low magnetic background field well below 150 nT in situ. The setup enables studies of inherently weak magnetic materials which cannot be measured with high field susceptibility setups, optical methods or neutron scattering techniques, giving new opportunities for the research on e.g. spin-spiral multiferroics, skyrmion materials and spin ices.

cond-mat.mtrl-sci

Structural magnetic glassiness in spin ice Dy$_2$Ti$_2$O$_7$

The spin ice compound Dy$_2$Ti$_2$O$_7$ is well-known to realise a three-dimensional Coulomb spin liquid with magnetically charged monopole excitations. Its fate at low temperatures, however, remains an intriguing open question. Based on a low-temperature analysis of the magnetic noise and diffuse neutron scattering under different cooling protocols, combined with extensive numerical modelling, we argue that upon cooling, the spins freeze into what may be termed a `structural magnetic glass', without an a priori need for chemical or structural disorder. Specifically, our model indicates the presence of frustration on two levels, first producing a near-degenerate constrained manifold inside which phase ordering kinetics is in turn frustrated. Our results suggest that spin ice Dy$_2$Ti$_2$O$_7$ provides one prototype of magnetic glass formation specifically, and a setting for the study of kinetically constrained systems more generally.

cond-mat.str-el

Tuning magnetoelectricity in a mixed-anisotropy antiferromagnet

Control of magnetization and electric polarization is attractive in relation to tailoring materials for data storage and devices such as sensors or antennae. In magnetoelectric materials, these degrees of freedom are closely coupled, allowing polarization to be controlled by a magnetic field, and magnetization by an electric field, but the magnitude of the effect remains a challenge in the case of single-phase magnetoelectrics for application. We demonstrate that the magnetoelectric properties of the mixed-anisotropy antiferromagnet LiNi$_{1-x}$Fe$_x$PO$_4$ are profoundly affected by replacing a fraction of the Ni$^{2+}$ ions with Fe$^{2+}$ on the transition metal site. This introduces random site-dependent single-ion anisotropy energies and causes a lowering of the magnetic symmetry of the system. In turn, magnetoelectric couplings that are symmetry-forbidden in the parent compounds, LiNiPO$_4$ and LiFePO$_4$, are unlocked and the dominant coupling is enhanced by two orders of magnitude. Our results demonstrate the potential of mixed-anisotropy magnets for tuning magnetoelectric properties.

cond-mat.str-el

Anomalous magnetic noise in imperfect flat bands in the topological magnet Dy2Ti2O7

The spin ice compound Dy_2Ti_2O_7 stands out as the first topological magnet in three dimensions, with its tell-tale emergent fractionalized magnetic monopole excitations. Its real-time dynamical properties have been an enigma from the very beginning. Using ultrasensitive, non-invasive SQUID measurements, we show that Dy_2Ti_2O_7 exhibits a highly anomalous noise spectrum, in three qualitatively different regimes: equilibrium spin ice, a `frozen' regime extending to ultra-low temperatures, as well as a high-temperature `anomalous' paramagnet. We show that in the simplest model of spin ice, the dynamics is not anomalous, and we present several distinct mechanisms which give rise to a coloured noise spectrum. In addition, we identify the structure of the single-ion dynamics as a crucial ingredient for any modelling. Thus, the dynamics of spin ice Dy_2Ti_2O_7 reflects the interplay of local dynamics with emergent topological degrees of freedom and a frustration-generated imperfectly flat energy landscape, and as such should be relevant for a broad class of magnetic materials.

cond-mat.str-el

Dispersions of Many-Body Bethe strings

Complex bound states of magnetic excitations, known as Bethe string, were predicted almost a century ago to exist in one-dimensional quantum magnets 1. The dispersions of the string states have so far remained the subject of intensive theoretical studies 2-7. By performing neutron scattering experiments on the one-dimensional Heisenberg-Ising antiferromagnet SrCo2V2O8 in high longitudinal magnetic fields, we reveal in detail the dispersion relations of the string states over the full Brillouin zone, as well as their magnetic field dependences. Furthermore the characteristic energy, the scattering intensity and linewidth of the observed string states exhibit excellent agreement with our precise Bethe Ansatz calculations. Our results establish the important role of string states in the quantum spin dynamics of one-dimensional systems, and will invoke studies of their dynamical properties in more general many-body systems.

cond-mat.str-el

Magnetocaloric properties and critical behavior of Co$_2$Cr$_{1-x}$Mn$_x$Al Heusler alloys

We study the magnetocaloric effect and critical behavior of Co$_2$Cr$_{1-x}$Mn$_x$Al ($x=$ 0.25, 0.5, 0.75) Heusler alloys across the ferromagnetic (FM) transition (T$_{\rm C}$). The Rietveld refinement of x-ray diffraction patterns exhibit single phase cubic structure for all the samples. The temperature dependent magnetic susceptibility $χ$(T) data show a systematic enhancement in the Curie temperature and effective magnetic moment with Mn concentration, which is consistent with the Slater-Pauling behavior. The M(H) isotherms also exhibit the FM ordering and the analysis of $χ$(T) data indicates the nature of the phase transition to be a second order, which is further supported by scaling of the entropy curves and Arrott plot. Interestingly, the Mn substitution causes an increase in the magnetic entropy change and hence large relative cooling power for multi-stage magnetic refrigerator applications. In order to understand the nature of the magnetic phase transition we examine the critical exponents $β$, $γ$, $δ$ for the $x=$ 0.75 sample by the modified Arrott plot and the critical isotherm analysis, which is further confirmed by Kouvel-Fisher method and Widom scaling relation, respectively. The estimated values of $β=$ 0.507, $γ=$ 1.056, $δ=$ 3.084 are found to be close to the mean field theoretical values. The renormalized isotherms (m vs h) corresponding to these exponent values collapse into two branches, above and below T$_{\rm C}$ that validates our analysis. Our results suggest for the existence of long-range FM interactions, which decays slower than power law as $J(r)\sim r^{-4.5}$ for a 3 dimensional mean field theory.

cond-mat.mtrl-sci

Incommensurate atomic and magnetic modulations in the spin-frustrated β-NaMnO2 triangular lattice

The layered β-NaMnO2, a promising Na-ion energy-storage material has been investigated for its triangular lattice capability to promote complex magnetic configurations that may release symmetry restrictions for the coexistence of ferroelectric and magnetic orders. The complexity of the neutron powder diffraction patterns underlines that the routinely adopted commensurate structural models are inadequate. Instead, a single-phase superspace symmetry description is necessary, demonstrating that the material crystallizes in a compositionally modulated q= (0.077(1), 0, 0) structure. Here, Mn3+ Jahn-Teller distorted MnO6 octahedra form corrugated layer stacking sequences of the β-NaMnO2 type, which are interrupted by flat sheets of the α-like oxygen topology. Spontaneous long-range collinear antiferromagnetic order, defined by the propagation vector k= (1/2, 1/2, 1/2), appears below TN1= 200 K. Moreover, a second transition into a spatially modulated proper-screw magnetic state (k+-q) is established at TN2= 95 K, with an antiferromagnetic order parameter resembling that of a two-dimensional (2D) system. The evolution of 23Na NMR spin-lattice relaxation identifies a magnetically inhomogene-ous state in the intermediate T-region (TN2 <T< TN1), while its strong suppression below TN2 indicates that a spin-gap opens in the excitation spectrum. High-resolution neutron inelastic scattering confirms that the magnetic dynamics are indeed gapped (Δ~5 meV) in the low-temperature magnetic phase, while simulations on the basis of the single-mode approximation suggest that Mn-spins residing on ad-jacent antiferromagnetic chains, establish sizable 2D correlations. Our analysis points that novel struc-tural degrees of freedom promote, cooperative magnetism and emerging dielectric properties in this non-perovskite-type of manganite.

cond-mat.mtrl-sci

Direct observation of the Higgs amplitude mode in a two-dimensional quantum antiferromagnet near the quantum critical point

Spontaneous symmetry-breaking quantum phase transitions play an essential role in condensed matter physics. The collective excitations in the broken-symmetry phase near the quantum critical point can be characterized by fluctuations of phase and amplitude of the order parameter. The phase oscillations correspond to the massless Nambu$-$Goldstone modes whereas the massive amplitude mode, analogous to the Higgs boson in particle physics, is prone to decay into a pair of low-energy Nambu$-$Goldstone modes in low dimensions. Especially, observation of a Higgs amplitude mode in two dimensions is an outstanding experimental challenge. Here, using the inelastic neutron scattering and applying the bond-operator theory, we directly and unambiguously identify the Higgs amplitude mode in a two-dimensional S=1/2 quantum antiferromagnet C$_9$H$_{18}$N$_2$CuBr$_4$ near a quantum critical point in two dimensions. Owing to an anisotropic energy gap, it kinematically prevents such decay and the Higgs amplitude mode acquires an infinite lifetime.

cond-mat.str-el

Magnetic phase diagram of CePt3B1-xSix

We present a study of the main bulk properties (susceptibility, magnetization, resistivity and specific heat) of CePt_3B_(1-x)Si-x, an alloying system that crystallizes in a noncentrosymmetric lattice, and derive the magnetic phase diagram. The materials at the end point of the alloying series have previously been studied, with CePt_3B established as a material with two different magnetic phases at low temperatures (antiferromagnetic below T_N = 7.8 K, weakly ferromagnetic below T_C ~ 5 K), while CePt3Si is a heavy fermion superconductor (T_c = 0.75 K) coexisting with antiferromagnetism (T_N = 2.2 K). From our experiments we conclude that the magnetic phase diagram is divided into two regions. In the region of low Si content (up to x ~ 0.7) the material properties resemble those of CePt3B. Upon increasing the Si concentration further the magnetic ground state continuously transforms into that of CePt3Si. In essence, we argue that CePt_3B can be understood as a low pressure variant of CePt3Si.

cond-mat.str-el

Solitonic lattice and Yukawa forces in the rare earth orthoferrite TbFeO3

The control of domains in ferroic devices lies at the heart of their potential for technological applications. Multiferroic materials offer another level of complexity as domains can be either or both of a ferroelectric and magnetic nature. Here we report the discovery of a novel magnetic state in the orthoferrite TbFeO3 using neutron diffraction under an applied magnetic field. This state has a very long incommensurate period ranging from 340 Angstrom at 3K to 2700 Angstrom at the lowest temperatures and exhibits an anomalously large number of higher-order harmonics, allowing us to identify it with the periodic array of sharp domain walls of Tb spins separated by many lattice constants. The Tb domain walls interact by exchanging spin waves propagating through the Fe magnetic sublattice. The resulting Yukawa-like force, familiar from particle physics, has a finite range that determines the period of the incommensurate state.

cond-mat.str-el

Magnetic Structure and Interactions in the Quasi-1D Antiferromagnet CaV$_2$O$_4$

CaV$_2$O$_4$ is a spin-1 antiferromagnet, where the magnetic vanadium ions are arranged on quasi-one-dimensional (1D) zig-zag chains with potentially frustrated antiferromagnetic exchange interactions. High temperature susceptibility and single-crystal neutron diffraction measurements are used to deduce the non-collinear magnetic structure, dominant exchange interactions and orbital configurations. The results suggest that at high temperatures CaV$_2$O$_4$ behaves as a Haldane chain, but at low temperatures, orbital ordering lifts the frustration and it becomes a spin-1 ladder.

cond-mat.str-el