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Markus Grüninger

Publications and source records attributed to Markus Grüninger.

9 recordsLinked to original sources

Synthesis of epitaxial TaO$_2$ thin films on Al$_2$O$_3$ by suboxide molecular-beam epitaxy and thermal laser epitaxy

Tantalum dioxide (TaO2) is a metastable tantalum compound. Here, we report the epitaxial stabilization of TaO2 on Al2O3 (1-102) (r-plane sapphire) substrates using suboxide molecular-beam epitaxy (MBE) and thermal laser epitaxy (TLE), demonstrating single-oriented, monodomain growth of anisotropically strained thin films. Microstructural investigation is performed using synchrotron X-ray diffraction and scanning transmission electron microscopy. The tetravalent oxidation state of tantalum is confirmed using X-ray absorption and photoemission spectroscopy as well as electron energy-loss spectroscopy. Optical properties are investigated via spectroscopic ellipsometry and reveal a 0.3 eV Mott gap of the tantalum 5d electrons. Density-functional theory and group theoretical arguments are used to evaluate the limited stability of the rutile phase and reveal the potential to unlock a hidden metal-insulator transition concomitant with a structural phase transition to a distorted rutile phase, akin to NbO2. Our work expands the understanding of tantalum oxides and paves the way for their integration into next-generation electronic and photonic devices.

cond-mat.mtrl-sci

Magnetic-field-induced critical dynamics in magnetoelectric TbPO$_4$

We report on the magnetoelectric dynamics in the linear magnetoelectric antiferromagnet TbPO$_4$ studied by broadband dielectric spectroscopy. For the phase transition into the magnetoelectric antiferromagnetic phase at $T_{N} \approx 2.3$ K, a finite magnetic field $H$ induces critical behavior in the quasi-static permittivity $\varepsilon'$. Plotting the corresponding anomaly as function of $T/T_N(H)$, we observe the scaling behavior $Δ\varepsilon' \propto H^2$, a clear fingerprint of linear magnetoelectric antiferromagnets. Above the phase transition, we find a critical slowing down of the ferroic fluctuations in finite magnetic field. This behaviour can be understood via a magnetic-field-induced relaxational response that resembles the soft-mode behaviour in canonical ferroelectrics and multiferroics.

cond-mat.str-el

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

Magnetoelectric coupling in the mixed erythrosiderite [(NH$_4$)$_{1-x}$K$_x$]$_2$[FeCl$_5$(H$_2$O)]

We present a study of the dielectric, structural, and magnetic properties of the multiferroic or linear magnetoelectric substitution series [(NH$_4$)$_{1-x}$K$_x$]$_2$[FeCl$_5$(H$_2$O)]. Pyroelectric currents, magnetic susceptibilities, and thermodynamic properties were examined on large single crystals of the erythrosiderite compounds and detailed magnetic-field versus temperature phase diagrams are derived for three different substitution levels. With increasing potassium concentration the material is tuned from a multiferroic ($x \le 0.06$) to a linear magnetoelectric ($x \ge 0.15$) ground state. In contrast to the respective pure parent compounds with $x=0$ or 1, however, the ferroelectric or linear magnetoelectric polarization in none of the substituted samples is switchable by external electric fields, because these samples exhibit a significant electric polarization already above the magnetic ordering transition. The polarization arises at a higher-lying structural phase transition that is examined by THz spectroscopy and, on a deuterated pure single crystal, by comprehensive neutron-diffraction experiments. The structural phase transition is attributed to an ordering of NH$_4^+$ tetrahedra but does not break inversion symmetry in the pure material, while a finite K content causes pyroelectricity.

cond-mat.str-el

Large positive magneto-conductivity at microwave frequencies in the compensated topological insulator BiSbTeSe2

The bulk electronic properties of compensated topological insulators are strongly affected by the self-organized formation of charge puddles at low temperature, but their response in the microwave frequency range is little studied. We employed broadband impedance spectroscopy up to 5 GHz to address the ac transport properties of well-compensated BiSbTeSe2, where charge puddles are known to form as metallic entities embedded in an insulating host. It turns out that the average puddle size sets the characteristic frequency cut-off in the GHz range, across which the insulating dc behavior is separated from a metal-like high-frequency response of delocalized carriers within the puddles. The cut-off frequency is found to be controlled by a magnetic field, giving rise to a large positive magneto-conductivity observable only in the GHz range. This curious phenomenon is driven by the Zeeman energy which affects the local band filling in the disordered potential landscape to enhance the puddle size.

cond-mat.str-el

Phase separation in the non-equilibrium Verwey transition in magnetite

We present equilibrium and out-of-equilibrium studies of the Verwey transition in magnetite. In the equilibrium optical conductivity, we find a step-like change at the phase transition for photon energies below about 2 eV. The possibility of triggering a non-equilibrium transient metallic state in insulating magnetite by photo excitation was recently demonstrated by an x-ray study. Here we report a full characterization of the optical properties in the visible frequency range across the non-equilibrium phase transition. Our analysis of the spectral features is based on a detailed description of the equilibrium properties. The out-of-equilibrium optical data bear the initial electronic response associated to localized photo-excitation, the occurrence of phase separation, and the transition to a transient metallic phase for excitation density larger than a critical value. This allows us to identify the electronic nature of the transient state, to unveil the phase transition dynamics, and to study the consequences of phase separation on the reflectivity, suggesting a spectroscopic feature that may be generally linked to out-of-equilibrium phase separation.

cond-mat.str-el

Witnessing the formation and relaxation of massive quasi-particles in a strongly correlated electron system

The non-equilibrium semiconductors physics is based on the paradigm that different degrees of freedom interact on different timescales. In this context the photo-excitation is often treated as an impulsive injection of electronic energy that is transferred to other degrees of freedom only at later times. Here, by studying the ultrafast particles dynamics in a archetypal strongly correlated charge-transfer insulator (La2CuO4), we show that the interaction between electrons and bosons manifest itself directly in the photo-excitation processes of a correlated material. With the aid of a general theoretical framework (Hubbard Holstein Hamiltonian), we reveal that sub-gap excitation pilots the formation of itinerant quasi-particles which are suddently dressed (<100 fs) by an ultrafast reaction of the bosonic field.

cond-mat.str-el

Hubbard exciton revealed by time-domain optical spectroscopy

We use broadband ultra-fast pump-probe spectroscopy in the visible range to study the lowest excitations across the Mott-Hubbard gap in the orbitally ordered insulator YVO3. Separating thermal and non-thermal contributions to the optical transients, we show that the total spectral weight of the two lowest peaks is conserved, demonstrating that both excitations correspond to the same multiplet. The pump-induced transfer of spectral weight between the two peaks reveals that the low-energy one is a Hubbard exciton, i.e. a resonance or bound state between a doublon and a holon. Finally, we speculate that the pump-driven spin-disorder can be used to quantify the kinetic energy gain of the excitons in the ferromagnetic phase.

cond-mat.str-el

Cyclic Spin Exchange in Cuprate Spin Ladders

We investigate the influence of a cyclic spin exchange J_{cyc} on the one- and two-triplet excitations of an undoped two-leg S=1/2 ladder, using the density matrix renormalization group (DMRG). The dispersion of the S=0 two-triplet bound state is dramatically reduced by J_{cyc} due to a repulsion between triplets on neighboring rungs. In (La,Ca)_{14}Cu_{24}O_{41} a consistent description of both the spin gap and the S=0 bound state requires $J_{cyc}/J_\perp \approx 0.20-0.27$ and $J/J_{\perp} \approx 1.25-1.35$. With these coupling ratios the recently developed dynamical DMRG yields an excellent description of the entire S=0 excitation spectrum observed in the optical conductivity, including the continuum contribution.

cond-mat.str-el