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K. Habicht

Publications and source records attributed to K. Habicht.

At least 19 recordsLinked to original sources

Kondo scaling of $4f$-electron states and the Kondo singlet breakdown in heavy fermions

The low-energy spin- and charge-sensitive thermodynamic properties of a broad range of strongly correlated 4f-electron systems follow Kondo scaling, with a characteristic Kondo temperature, $T_K$. While the theory is known for thermodynamic properties and high-energy spectroscopies of Kondo materials, the surface sensitivity of electron spectroscopy limits the extent to which Kondo scaling can be quantitatively verified. In this study, bulk-sensitive photon-in photon-out temperature-dependent resonant inelastic X-ray scattering (RIXS), in combination with single-impurity Anderson model (SIAM) calculations, is used to provide quantitative evidence of low- and high-energy Kondo scaling in CeSi$_2$. RIXS Ce M$_5$-edge spectra show a clear decrease in the occupancy of the $f^0$ state as temperature increases accompanied by an increase of the spectral weight of the $f^1\underline L^1$ state, in good agreement with the SIAM calculations. The results demonstrate the breakdown of the Kondo singlet state, coupled with thermal occupation of the low-lying first-excited magnetic states. The RIXS data reveal a temperature evolution of the $f^n$ spectral weights, which is in stark contrast to that extracted from photoemission and inverse photoemission spectroscopies. This study provides an accurate spectroscopic method to determine the Kondo energy $k_B$$T_K$ that is consistent with thermodynamic measurements, and highlights soft X-ray RIXS as a quantitative bulk probe of low- and high-energy-scale hybridization effects in strongly correlated materials.

cond-mat.str-el

Anomalous pressure dependence of the bulk modulus and Yb valence in cubic YbPd

We investigate the Yb valence instabilities in the strongly correlated YbPd compound using resonant X-ray emission spectroscopy as a function of pressure across the charge-order (CO) transition. At a low temperature (T = 30 K) in the CO phase, the Yb $4f$ valence remains nearly constant up to a pressure P$_L$ = 1.5 $\pm {0.2}$ GPa, and then increases gradually at higher pressures. In contrast, at room temperature in the normal phase, an anomalous decrease of the Yb $4f$ valence is observed, without any accompanying structural phase transition. This behavior is corroborated by a systematic pressure-dependent decrease of the unit-cell volume. Based on a Birch-Murnaghan analysis, the compressibility indicates hardening of the lattice with applied pressure up to a distinct kink seen at P$_K$ = 1.6 $\pm {0.2}$ GPa. In contrast, for P $>$ P$_K$, the Yb $4f$ valence saturates and the compressibility reveals a counterintuitive pressure-induced softening. The results show a minimum in the compressibility of YbPd (with $f^{0}$-$f^{1}$ hole-type mixed-valence), reminiscent of the maximum in compressibility seen in the $\gamma$-$\alpha$ first-order isostructural phase transition in cerium (with $f^{0}$-$f^{1}$ electron-type mixed-valence).

cond-mat.str-el

Evolution of plasmon excitations across the phase diagram of the cuprate superconductor La$_{2-x}$Sr$_{x}$CuO$_4$

We use resonant inelastic x-ray scattering (RIXS) at the O $K$- and Cu $K$-edges to investigate the doping- and temperature dependence of low-energy plasmon excitations in La$_{2-x}$Sr$_{x}$CuO$_4$. We observe a monotonic increase of the energy scale of the plasmons with increasing doping $x$ in the underdoped regime, whereas a saturation occurs above optimal doping $x \gtrsim 0.16$ and persists at least up to $x = 0.4$. Furthermore, we find that the plasmon excitations show only a marginal temperature dependence, and possible effects due to the superconducting transition and the onset of strange metal behavior are either absent or below the detection limit of our experiment. Taking into account the strongly correlated character of the cuprates, we show that layered $t$-$J$-$V$ model calculations accurately capture the increase of the plasmon energy in the underdoped regime. However, the computed plasmon energy continues to increase even for doping levels above $x \gtrsim 0.16$, which is distinct from the experimentally observed saturation, and reaches a broad maximum around $x = 0.55$. We discuss whether possible lattice disorder in overdoped samples, a renormalization of the electronic correlation strength at high dopings, or an increasing relevance of non-planar Cu and O orbitals could be responsible for the discrepancy between experiment and theory for doping levels above $x = 0.16$.

cond-mat.supr-con

Critical magnetic fluctuations in the layered ruthenates Ca$_2$RuO$_4$ and Ca$_3$Ru$_2$O$_7$

Materials realizing the XY model in two dimensions (2D) are sparse. Here we use neutron triple-axis spectroscopy to investigate the critical static and dynamical magnetic fluctuations in the square-lattice antiferromagnets Ca$_{2}$RuO$_{4}$ and Ca$_{3}$Ru$_2$O$_{7}$. We probe the temperature-dependence of the antiferromagnetic (AFM) Bragg-intensity, the $Q$-width, the amplitude, and the energy-width of the magnetic diffuse scattering in vicinity to the Néel temperature $T_N$ to determine the critical behavior of the magnetic order parameter $M$, correlation length $ξ$, susceptibility $χ$, and the characteristic energy $Γ$ with the corresponding critical exponents $β$, $ν$, $γ$, and $z$, respectively. We find that the critical behaviors of the single-layer compound Ca$_{2}$RuO$_{4}$ follow universal scaling laws that are compatible with predictions of the 2D-XY model. The bilayer compound Ca$_{3}$Ru$_2$O$_{7}$ is only partly consistent with the 2D-XY theory and best described by the three-dimensional Ising (3D-I) model, which is likely a consequence of the intra-bilayer exchange interactions in combination with an orthorhombic single-ion anisotropy. Hence, our results suggest that layered ruthenates are promising solid-state platforms for research on the 2D-XY model and the effects of 3D interactions and additional spin-space anisotropies on the magnetic fluctuations.

cond-mat.str-el

A Triplet Resonance in Superconducting FeSe0.4Te0.6

From heavy fermions to cuprates and iron pnictides, a spin resonance is a staple of nearly magnetic superconductors. Possible explanations include a two-particle bound state or loss of magnon damping in the superconductor. While both scenarios suggest a central role for magnetic fluctuations, distinguishing them is important to identify the right theoretical framework and to guide the search for higher temperature superconductors. Using inelastic neutron scattering technique, we show that the spin resonance in optimally doped Fe(Se,Te) splits into three peaks in a high magnetic field, a signature of a two-particle triplet bound state

cond-mat.supr-con

Time-dependent correlations in quantum magnets at finite temperature

In this article we investigate the time dependence of the gap mode of copper nitrate at various temperatures. We combine state-of-the-art theoretical calculations with high precision neutron resonance spin-echo measurements to understand the anomalous decoherence effects found previously in this material. It is shown that the time domain offers a complementary view on this phenomenon, which allows us to directly compare experimental data and theoretical predictions without the need of further intensive data analysis, such as (de)convolution.

cond-mat.str-el

Quantum phase transitions and decoupling of magnetic sublattices in the quasi-two-dimensional Ising magnet Co3V2O8 in a transverse magnetic field

The application of a magnetic field transverse to the easy axis, Ising direction in the quasi-two-dimensional Kagome staircase magnet, Co3V2O8, induces three quantum phase transitions at low temperatures, ultimately producing a novel high field polarized state, with two distinct sublattices. New time-of-flight neutron scattering techniques, accompanied by large angular access, high magnetic field infrastructure allow the mapping of a sequence of ferromagnetic and incommensurate phases and their accompanying spin excitations. At least one of the transitions to incommensurate phases at μ0Hc1~6.25 T and μ0Hc2~7 T is discontinuous, while the final quantum critical point at μ0Hc3~13 T is continuous.

cond-mat.str-el

Jahn-Teller versus quantum effects in the spin-orbital material LuVO3

We report on combined neutron and resonant x-ray scattering results, identifying the nature of the spin-orbital ground state and magnetic excitations in LuVO3 as driven by the orbital parameter. In particular, we distinguish between models based on orbital Peierls dimerization, taken as a signature of quantum effects in orbitals, and Jahn-Teller distortions, in favor of the latter. In order to solve this long-standing puzzle, polarized neutron beams were employed as a prerequisite in order to solve details of the magnetic structure, which allowed quantitative intensity-analysis of extended magnetic excitation data sets. The results of this detailed study enabled us to draw definite conclusions about classical vs quantum behavior of orbitals in this system and to discard the previous claims about quantum effects dominating the orbital physics of LuVO3 and similar systems.

cond-mat.str-el

Gains from the upgrade of the cold neutron triple-axis spectrometer FLEXX at the BER-II reactor

The upgrade of the cold neutron triple-axis spectrometer FLEXX is described. We discuss the characterisation of the gains from the new primary spectrometer, including a larger guide and double focussing monochromator, and present measurements of the energy and momentum resolution and of the neutron flux of the instrument. We found an order of magnitude gain in intensity (at the cost of coarser momentum resolution), and that the incoherent elastic energy widths are measurably narrower than before the upgrade. The much improved count rate should allow the use of smaller single crystals samples and thus enable the upgraded FLEXX spectrometer to continue making leading edge measurements.

physics.ins-det

Quantum criticality in an Ising chain: experimental evidence for emergent E8 symmetry

Quantum phase transitions take place between distinct phases of matter at zero temperature. Near the transition point, exotic quantum symmetries can emerge that govern the excitation spectrum of the system. A symmetry described by the E8 Lie group with a spectrum of 8 particles was long predicted to appear near the critical point of an Ising chain. We realize this system experimentally by tuning the quasi-one-dimensional Ising ferromagnet CoNb2O6 through its critical point using strong transverse magnetic fields. The spin excitations are observed to change character from pairs of kinks in the ordered phase to spin-flips in the paramagnetic phase. Just below the critical field, the spin dynamics shows a fine structure with two sharp modes at low energies, in a ratio that approaches the golden mean as predicted for the first two meson particles of the E8 spectrum. Our results demonstrate the power of symmetry to describe complex quantum behaviours.

cond-mat.str-el

Excitations from a chiral magnetized state of a frustrated quantum spin liquid

We study excitations in weakly interacting pairs of quantum spin ladders coupled through geometrically frustrated bonds. The ground state is a disordered spin liquid, that at high fields is replaced by an ordered chiral helimagnetic phase. The spectra observed by high-field inelastic neutron scattering experiments on the prototype compound Sul-Cu2Cl4 are qualitatively different from those in the previously studied frustration-free spin liquids. Beyond the critical field Hc=3.7 T, the soft mode that drives the quantum phase transition spawns two separate excitations: a gapless Goldstone mode and a massive magnon. Additional massive quasiparticles are clearly visible below Hc, but are destroyed in the ordered phase. In their place one observes a sharply bound excitation continuum.

cond-mat.str-el

Dimensional crossover in a spin liquid to helimagnet quantum phase transition

Neutron scattering is used to study magnetic field induced ordering in the quasi-1D quantum spin-tube compound Sul--Cu$_2$Cl$_4$ that in zero field has a non-magnetic spin-liquid ground state. The experiments reveal an incommensurate chiral high-field phase stabilized by a geometric frustration of the magnetic interactions. The measured critical exponents $β\approx0.235$ and $ν\approx0.34$ at $H_c\approx3.7$ T point to an unusual sub-critical scaling regime and may reflect the chiral nature of the quantum critical point.

cond-mat.str-el

Direct Observation of Magnon Fractionalization in the Quantum Spin Ladder

We measure by inelastic neutron scattering the spin excitation spectra as a function of applied magnetic field in the quantum spin-ladder material (C5H12N)2CuBr4. Discrete magnon modes at low fields in the quantum disordered phase and at high fields in the saturated phase contrast sharply with a spinon continuum at intermediate fields characteristic of the Luttinger-liquid phase. By tuning the magnetic field, we drive the fractionalization of magnons into spinons and, in this deconfined regime, observe both commensurate and incommensurate continua.

cond-mat.str-el

Magnetic Ordering and Negative Thermal Expansion in PrFeAsO

We report the structure and magnetism of PrOFeAs, one of the parent phases of the newly discovered Fe-As superconductors, as measured by neutron powder diffraction. In common with other REOFeAs materials, a tetragonal-orthorhombic phase transition is found on cooling below 136 K and striped Fe magnetism with $k =$(1,0,1) is detected below $\sim$ 85 K. Our magnetic order parameter measurements show that the ordered Fe moment along the a axis reaches a maximum at $\sim$ 40 K, below which an anomalous expansion of the c axis sets in, which results in a negative thermal volume expansion of 0.015 % at 2 K. We propose that this effect, which is suppressed in superconducting samples, is driven by a delicate interplay between Fe and Pr ordered moments.

cond-mat.supr-con

External magnetic field effects on a distorted kagome antiferromagnet

We report bulk magnetization, and elastic and inelastic neutron scattering measurements under an external magnetic field, $H$, on the weakly coupled distorted kagome system, Cu_{2}(OD)_3Cl. Our results show that the ordered state below 6.7 K is a canted antiferromagnet and consists of large antiferromagnetic $ac$-components and smaller ferromagnetic $b$-components. By first-principle calculations and linear spin wave analysis, we present a simple spin hamiltonian with non-uniform nearest neighbor exchange interactions resulting in a system of coupled spin trimers with a single-ion anisotropy that can qualitatively reproduce the spin dynamics of Cu_{2}(OD)_3Cl.

cond-mat.str-el

Melting of magnetic correlations in charge-orbital ordered La(0.5)Sr(1.5)MnO(4) : competition of ferro and antiferromagnetic states

The magnetic correlations in the charge- and orbital-ordered manganite La(0.5)Sr(1.5)MnO(4) have been studied by elastic and inelastic neutron scattering techniques. Out of the well-defined CE-type magnetic structure with the corresponding magnons a competition between CE-type and ferromagnetic fluctuations develops. Whereas ferromagnetic correlations are fully suppressed by the static CE-type order at low temperature, elastic and inelastic CE-type correlations disappear with the melting of the charge-orbital order at high temperature. In its charge-orbital disordered phase, La(0.5)Sr(1.5)MnO(4) exhibits a dispersion of ferromagnetic correlations which remarkably resembles the magnon dispersion in ferromagnetically ordered metallic perovskite manganites.

cond-mat.str-el

Gap excitations in a four-leg Heisenberg spin tube antiferromagnet

Inelastic neutron scattering is used to investigate magnetic excitations in the quasi-one-dimensional quantum spin-liquid system Cu2Cl4 D8C4SO2. Contrary to previously conjectured models that relied on bond-alternating nearest neighbor interactions in the spin chains, the dominant interactions are actually next-nearest-neighbor in-chain antiferromagnetic couplings. The appropriate Heisenberg Hamiltonian is equivalent to that of a S = 1/2 4-leg spin-tube with almost perfect one dimensionality and no bond alternation. A partial geometric frustration of rung interactions induces a small incommensurability of short-range spin correlations.

cond-mat.str-el

Quantum spin liquid states in the two dimensional kagome antiferromagnets, ZnxCu4-x(OD)6Cl2

A three-dimensional system of interacting spins typically develops static long-range order when it is cooled. If the spins are quantum (S = 1/2), however, novel quantum paramagnetic states may appear. The most highly sought state among them is the resonating valence bond (RVB) state in which every pair of neighboring quantum spins form entangled spin singlets (valence bonds) and the singlets are quantum mechanically resonating amongst all the possible highly degenerate pairing states. Here we provide experimental evidence for such quantum paramagnetic states existing in frustrated antiferromagnets, ZnxCu4-x(OD)6Cl2, where the S = 1/2 magnetic Cu2+ moments form layers of a two-dimensional kagome lattice. We find that in Cu4(OD)6Cl2, where distorted kagome planes are weakly coupled to each other, a dispersionless excitation mode appears in the magnetic excitation spectrum below ~ 20 K, whose characteristics resemble those of quantum spin singlets in a solid state, known as a valence bond solid (VBS), that breaks translational symmetry. Doping nonmagnetic Zn2+ ions reduces the distortion of the kagome lattice, and weakens the interplane coupling but also dilutes the magnetic occupancy of the kagome lattice. The VBS state is suppressed and for ZnCu3(OD)6Cl2 where the kagome planes are undistorted and 90% occupied by the Cu2+ ions, the low energy spin fluctuations in the spin liquid phase become featureless.

cond-mat.str-el