arXiv subjects

J. Deisenhofer

Publications and source records attributed to J. Deisenhofer.

At least 19 recordsLinked to original sources

arXiv2026

Magnetic circular dichroism of THz modes and selection rules of Raman-active optical phonons in the polar altermagnet candidate \ce{Mn2Mo3O8}

We investigated the magnetic and vibrational excitations in the collinear altermagnet candidate \ce{Mn2Mo3O8} by temperature dependent Raman scattering and magneto-optical THz time-domain transmission spectroscopy. By comparison to \textit{ab initio} calculations accurately capturing the eigenfrequencies of the vibrational eigenmodes, we identify all optical phonons, including the lowest-lying Raman modes of $A_1$ and $E_2$ type, which had remained elusive in a previous Raman study. Moreover, we compare the selection rules for optically active phonons in the paramagnetic and the magnetically ordered phases of \ce{Mn2Mo3O8} and analyze the Raman selection rules with respect to pseudo-angular momentum conservation. No evidence of the expected splitting of the degenerate paramagnetic $E_2$ optical phonons into modes with circular polarization upon magnetic ordering could be resolved, likely due to weak spin-orbit coupling typical for Mn$^{2+}$. In contrast, we observe strong magnetic circular dichroism at a broad THz excitation band, emerging in the magnetically ordered state. This band, potentially originating from two-magnon excitations, is only electric-dipole active and features a field-dependent two-component fine structure. Its magnetic circular dichroism vanishes above the spin-flop transition at 4~T.

cond-mat.str-el↗

arXiv2025

Optical phonons as a testing ground for spin group symmetries

Lattice vibrations are highly sensitive to crystal symmetries and their changes across phase transitions. The latter can modify irreducible (co)representations and corresponding infrared and Raman selection rules of phonons. This concept is established for relativistic magnetic point groups, simultaneously transforming spatial and spin coordinates. However, in altermagnets described by non-relativistic spin groups with disjunct symmetry operations for both vector spaces, the phonon selection rules have remained unexplored. Here, we present a detailed study of the infrared- and Raman-active modes in the collinear antiferromagnet and altermagnet candidate Co$_2$Mo$_3$O$_8$. Comparing to ab initio calculations accurately capturing the eigenfrequencies, we identify all expected phonon modes at room temperature and deduce their selection rules using both symmetry approaches. Importantly, we observe the change of selection rules upon antiferromagnetic ordering, agreeing with the relativistic symmetry approach, while the spin group formalism predicts no changes. Therefore, optical phonons can reveal the appropriate symmetry treatment.

cond-mat.mtrl-sci↗

arXiv2024

Optical magnetoelectric effect in the polar honeycomb antiferromagnet Fe2Mo3O8

The lack of both time-reversal and spatial inversion symmetry in polar magnets is a prerequisite for the occurrence of optical magnetoelectric effects such as nonreciprocal directional dichroism with the potential for the realization of optical diodes. In particular, antiferromagnetic materials with magnetic excitations in the THz range such as Fe2Mo3O8 are promising candidates for next-generation spintronic applications. In a combined experimental and theoretical effort we investigated the THz excitations of the polar honeycomb antiferromagnet Fe2Mo3O8 in external magnetic fields and their nonreciprocal directional dichroism, together with the temperature dependence of the electronic transitions in the mid- and near-infrared frequency range. Using an advanced single-ion approach for the Fe ions, we are able to describe optical excitations from the THz to the near-infrared frequency range quantitatively and successfully model the observed nonreciprocal directional dichroism in the THz regime.

cond-mat.str-el↗

arXiv2023

Nodal line resonance generating the giant anomalous Hall effect of Co$_3$Sn$_2$S$_2$

Giant anomalous Hall effect (AHE) and magneto-optical activity can emerge in magnets with topologically non-trivial degeneracies. However, identifying the specific band structure features like Weyl points, nodal lines or planes which generate the anomalous response is a challenging issue. Since the low-energy interband transitions can govern the static AHE, we addressed this question in the prototypical magnetic Weyl semimetal Co$_3$Sn$_2$S$_2$ also hosting nodal lines by broadband polarized reflectivity and magneto-optical Kerr effect spectroscopy with a focus on the far-infrared range. In the linear dichroism spectrum we observe a strong resonance at 40\,meV, which also shows up in the optical Hall conductivity spectrum and primarily determines the static AHE, thus, confirms its intrinsic origin. Our material-specific theory reproduces the experimental data remarkably well and shows that strongly tilted nodal line segments around the Fermi energy generate the resonance. While the Weyl points only give vanishing contributions, these segments of the nodal lines gapped by the spin-orbit coupling dominate the low-energy optical response.

cond-mat.str-el↗

arXiv2022

Magneto-optical detection of topological contributions to the anomalous Hall effect in a kagome ferromagnet

A single ferromagnetic kagome layer is predicted to realize a Chern insulator with quantized Hall conductance, which upon stacking can become a Weyl-semimetal with large anomalous Hall effect (AHE) and magneto-optical activity. Indeed, in the kagome bilayer material Fe$_3$Sn$_2$, a large AHE was detected, however, it still awaits the direct probing of the responsible band structure features by bulk sensitive methods. We measure the optical, both diagonal and Hall, conductivity spectra over a broad spectral range and identify the origin of the intrinsic AHE with the help of momentum- and band-decomposed first-principles calculations. We find that low-energy transitions, tracing "helical volumes" in momentum space reminiscent of the formerly predicted helical nodal lines, substantially contribute to the AHE, which is further increased by contributions from multiple higher-energy interband transitions. Our study also reveals that local Coulomb interactions lead to band reconstructions near the Fermi level.

cond-mat.str-el↗

arXiv2021

Confirming the trilinear form of the optical magnetoelectric effect in the polar honeycomb antiferromagnet Co$_{2}$Mo$_3$O$_8$

Magnetoelectric phenomena are intimately linked to relativistic effects and also require the material to break spatial inversion symmetry and time reversal invariance. Magnetoelectric coupling can substantially affect light-matter interaction and lead to non-reciprocal light propagation. Here, we confirm on a fully experimental basis, without invoking either symmetry-based or material-specific assumptions, that the optical magnetoelectric effect in materials with non-parallel magnetization ($\boldsymbol{M}$) and electric polarization ($\boldsymbol{P}$) generates a trilinear term in the refractive index, $δn\propto\boldsymbol{k}\cdot(\boldsymbol{P}\times\boldsymbol{M})$, where $\boldsymbol{k}$ is the propagation vector of light. Its sharp magnetoelectric resonances, that are simultaneously electric and magnetic dipole active excitations, make Co$_{2}$Mo$_3$O$_8$ an ideal compound to demonstrate this fundamental relation via independent variation of $\boldsymbol{M}$, $\boldsymbol{P}$ and $\boldsymbol{k}$. Remarkably, the material shows almost perfect one-way transparency in moderate magnetic fields at some of the magnetoelectric resonances.

cond-mat.str-el↗

arXiv2021

On the complexity of spinels: Magnetic, electronic, and polar ground states

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.

cond-mat.str-el↗

arXiv2020

Magnetic and vibronic THz excitations in Zn doped Fe$_{2}$Mo$_3$O$_8$

We report on optical excitations in the magnetically ordered phases of multiferroic Fe$_{1.86}$Zn$_{0.14}$Mo$_3$O$_8$ in the frequency range from 10-130 cm$^{-1}$ (0.3-3.9 THz). In the collinear easy-axis antiferromagnetic phase below $T_N=50$~K eleven optically active modes have been observed in finite magnetic fields, assuming that the lowest-lying mode is doubly degenerate. The large number of modes reflects either a more complex magnetic structure than in pure Fe$_{2}$Mo$_3$O$_8$ or that spin stretching modes become active in addition to the usual spin precessional modes. Their magnetic field dependence, for fields applied along the easy axis, reflects the irreversible magnetic-field driven phase transition from the antiferromagnetic ground state to a ferrimagnetic state, while the number of modes remains unchanged in the covered frequency region. We determined selection rules for some of the AFM modes by investigating all polarization configurations and identified magnetic- and electric-dipole active modes as well. In addition to these sharp resonances, a broad electric-dipole active excitation band, which is not influenced by the external magnetic field, occurs below $T_N$ with an onset at 12 cm$^{-1}$. We are able to model this absorption band as a vibronic excitation related to the lowest-lying Fe$^{2+}$ electronic states in tetrahedral environment.

cond-mat.str-el↗

arXiv2020

Structure, phonons, and orbital degrees of freedom in Fe$_2$Mo$_3$O$_8$

We report on the structural and spectroscopic characterization of the multiferroic Fe$_2$Mo$_3$O$_8$. Synchrotron x-ray and neutron diffraction, as well as thermal expansion measurements reveal a lattice anomaly at $T_{\mathrm{N}}\simeq 60\,$K but do not show any symmetry lowering in the magnetically ordered state. The lattice parameter $c$ exhibits a non-monotonic behavior with a pronounced minimum around $200\,$K, which is also reflected in an anomalous behavior of some of the observed infrared-active optical excitations and parallels the onset of short-range magnetic order. The infrared reflectivity spectra measured between 5 and 300$\,$K in the frequency range of $100-8000\,$cm$^{-1}$ reveal most of the expected phonon modes in comparison with the eigenfrequencies obtained by density-functional calculations. The $A_1$ phonons show an overall hardening upon cooling, whereas a non-monotonic behavior is observed for some of the $E_1$ modes. These modes also show a strongly increased phonon lifetime below $T_\mathrm{N}$, which we associate with the quenched direction of the orbital moment in the magnetically ordered state. A similar increase is observed in the lifetime of the higher-lying $d$-$d$ excitations of the tetrahedral Fe$^{2+}$ site, which become clearly visible below $T_\mathrm{N}$ only.

cond-mat.str-el↗

arXiv2020

Magneto-electric properties and low-energy excitations of multiferroic FeCr2S4

We report on the low-frequency optical excitations in the multiferroic ground state of polycrystalline FeCr2S4 in the frequency range 0.3-3~THz and their changes upon applying external magnetic fields up to 7~T. In the ground state below the orbital-ordering temperature T_OO=9K we observe the appearance of several new modes. By applying the external magnetic field parallel and perpendicular to the propagation direction of the THz radiation, we can identify the strongest absorptions to be of predominantly electric-dipole origin. We discuss these modes as the low-energy electronic excitations of the Fe^{2+} ions (3d^6, S=2) in an tetrahedral environment. The eigenfrequencies and relative intensities of these absorption lines are satisfactorily reproduced by our calculation assuming an effective exchange field of 12.8 cm-1 at the Fe^{2+}-ions sites. The direction of the exchange field is found to be slightly tilted out of the ab-plane. With our approach we can also describe previously reported results from Mössbauer studies and the order of magnitude of the electric polarisation induced by orbital and non-collinear spin ordering.

cond-mat.str-el↗

arXiv2020

Lattice dynamics and electronic excitations in a large family of lacunar spinels with a breathing pyrochlore lattice structure

Reproducing the electronic structure of AM$_4$X$_8$ lacunar spinels with a breathing pyrochlore lattice is a great theoretical challenge due to the interplay of various factors. The character of the M$_4$X$_4$ cluster orbitals is critically influenced by the Jahn-Teller instability, the spin-orbit interaction, and also by the magnetic state of the clusters. Consequently, to reproduce the narrow-gap semiconducting nature of these moderately correlated materials requires advanced approaches, since the strength of the inter-cluster hopping is strongly affected by the character of the cluster orbitals. In order to provide a solid experimental basis for theoretical studies, we performed broadband optical spectroscopy on a large set of lacunar spinels, with systematically changing ions at the A and M sites as well as the ligand (A=Ga, Ge, Al; M=V, Mo, Nb, Ta; X=S, Se). Our study covers the range of phonon excitations and also electronic transitions near the gap edge. In the phonon excitation spectrum a limited subset of the symmetry allowed modes is observed in the cubic state, with a few additional modes emerging upon the symmetry-lowering structural transition. All the infrared active modes are assigned to vibrations of the ligands and ions at the A sites, with no obvious contribution from the M-site ions. Concerning the electronic states, we found that all compounds are narrow-gap semiconductors ($E_\mathrm{g} = 130 - 350\,$meV) already in their room-temperature cubic state and their structural transitions induce weak, if any, changes in the band gap. The gap value is decreased when substituting S with Se and also when replacing $3d$ ions by $4d$ or $5d$ ions at the M sites.

cond-mat.str-el↗

arXiv2019

Spin-lattice coupling in a ferrimagnetic spinel: The exotic $H$-$T$ phase diagram of MnCr$_2$S$_4$ up to 110 T

In antiferromagnets, the interplay of spin frustration and spin-lattice coupling has been extensively studied as the source of complex spin patterns and exotic magnetism. Here, we demonstrate that, although neglected in the past, the spin-lattice coupling is essential to ferrimagnetic spinels as well. We performed ultrahigh-field magnetization measurements up to 110 T on a Yafet-Kittel ferrimagnetic spinel, MnCr$_2$S$_4$, which was complemented by measurements of magnetostriction and sound velocities up to 60 T. Classical Monte Carlo calculations were performed to identify the complex high-field spin structures. Our minimal model incorporating spin-lattice coupling accounts for the experimental results and corroborates the complete phase diagram, including two new high-field phase transitions at 75 and 85 T. Magnetoelastic coupling induces striking effects: An extremely robust magnetization plateau is embedded between two unconventional spin-asymmetric phases. Ferrimagnetic spinels provide a new platform to study asymmetric and multiferroic phases stabilized by spin-lattice coupling.

cond-mat.str-el↗

arXiv2019

Structure, superconductivity, and magnetism in Rb1-xFe1.6Se2-zSz

The single-crystal growth, stoichiometry, and structure of Rb1-xFe2-ySe2-zSz crystals with substitution of Se by S are reported. The variation of the magnetic and thermodynamic parameters of samples was studied by differential-scanning calorimetry, magnetic susceptibility, conductivity, and specific heat. The experimental results are discussed within a T-z phase diagram, which includes vacancy-ordered and vacancy-disordered antiferromagnetic (AFM), superconducting (SC), and non-superconducting phases. The structural study revealed change in the local environment of the Fe tetrahedrons depending on substitution: a reduction of the Fe-Fe and Fe-Ch(chalcogen) bond lengths and a tendency for the six out of eight bond angles to approach values for a regular tetrahedron suggesting a reduction of structural distortions with substitution. With increasing substitution, a lowering of the superconducting transition temperature Tc was observed; the percolation threshold for the SC state is located at the substitution z = 1.2. The SC state was found to coexist with the AFM state that persists in all samples independent of substitution. The temperature of the transition into the AFM state TN shows a monotonous decrease indicating a weakening of the AFM interactions with increasing substitution. The AFM phase exhibits an iron-vacancy-ordered structure below the structural transition at Ts. The temperature Ts shows a non-monotonous variation: a decrease with increasing z up to 1.3, followed by an increase for further increasing z. The suppression of the superconductivity with substitution is accompanied by a significant reduction of the density of states at the Fermi energy and a weakening of the electronic correlations in the studied system.

cond-mat.supr-con↗

arXiv2018

Intrinsic charge dynamics in high-Tc AFeAs(O,F) superconductors

We report the first determination of the in-plane complex optical conductivity of 1111 high-Tc superconducting iron oxypnictide single crystals PrFeAsO0.6F0.35 and thin films SmFeAsO1-xFx by means of bulk-sensitive conventional and micro-focused infrared spectroscopy, ellipsometry, and time-domain THz transmission spectroscopy. A strong itinerant contribution is found to exhibit a dramatic difference in coherence between the crystal and the film. Using extensive temperature-dependent measurements of THz transmission we identify a previously undetected 2.5-meV collective mode in the optical conductivity of SmFeAs(O,F), which is strongly suppressed at Tc and experiences an anomalous T-linear softening and narrowing below T*=110K>>Tc. The suppression of the infrared absorption in the superconducting state reveals a large optical superconducting gap with a similar gap ratio 2D=kBTc=7 in both materials, indicating strong pairing.

cond-mat.supr-con↗

arXiv2017

High-pressure versus isoelectronic doping effect on the honeycomb iridate Na$_2$IrO$_3$

We study the effect of isoelectronic doping and external pressure in tuning the ground state of the honeycomb iridate Na$_2$IrO$_3$ by combining optical spectroscopy with synchrotron x-ray diffraction measurements on single crystals. The obtained optical conductivity of Na$_2$IrO$_3$ is discussed in terms of a Mott insulating picture versus the formation of quasimolecular orbitals and in terms of Kitaev-interactions. With increasing Li content $x$, (Na$_{1-x}$Li$_x$)$_2$IrO$_3$ moves deeper into the Mott insulating regime and there are indications that up to a doping level of 24\% the compound comes closer to the Kitaev-limit. The optical conductivity spectrum of single crystalline $α$-Li$_2$IrO$_3$ does not follow the trends observed for the series up to $x=0.24$. There are strong indications that $α$-Li$_2$IrO$_3$ is less close to the Kitaev-limit compared to Na$_2$IrO$_3$ and closer to the quasimolecular orbital picture. Except for the pressure-induced hardening of the phonon modes, the optical properties of Na$_2$IrO$_3$ seem to be robust against external pressure. Possible explanations of the unexpected evolution of the optical conductivity with isolectronic doping and the drastic change between $x=0.24$ and $x=1$ are given by comparing the pressure-induced changes of lattice parameters and the optical conductivity with the corresponding changes induced by doping.

cond-mat.str-el↗

arXiv2017

Structure, magnetic susceptibility and specific heat of the spin-orbital-liquid candidate FeSc2S4 : Influence of fe off-stoichiometry

We report structural, susceptibility and specific heat studies of stoichiometric and off-stoichiometric poly- and single crystals of the A-site spinel compound FeSc2S4. In stoichiometric samples no long-range magnetic order is found down to 1.8 K. The magnetic susceptibility of these samples is field independent in the temperature range 10 - 400 K and does not show irreversible effects at low temperatures. In contrast, the magnetic susceptibility of samples with iron excess shows substantial field dependence at high temperatures and manifests a pronounced magnetic irreversibility at low temperatures with a difference between ZFC and FC susceptibilities and a maximum at 10 K reminiscent of a magnetic transition. Single crystal x-ray diffraction of the stoichiometric samples revealed a single phase spinel structure without site inversion. In single crystalline samples with Fe excess besides the main spinel phase a second ordered single-crystal phase was detected with the diffraction pattern of a vacancy-ordered superstructure of iron sulfide, close to the 5C polytype Fe9S10. Specific heat studies reveal a broad anomaly, which evolves below 20 K in both stoichiometric and off-stoichiometric crystals. We show that the low-temperature specific heat can be well described by considering the low-lying spin-orbital electronic levels of Fe2+ ions. Our results demonstrate significant influence of excess Fe ions on intrinsic magnetic behavior of FeSc2S4 and provide support for the spin-orbital liquid scenario proposed in earlier studies for the stoichiometric compound.

cond-mat.mtrl-sci↗

arXiv2016

Singlet-triplet excitations and long range entanglement in the spin-orbital liquid candidate FeSc2S4

Theoretical models of the spin-orbital liquid (SOL) FeSc$_2$S$_4$ have predicted it to be in close proximity to a quantum critical point separating a spin-orbital liquid phase from a long-range ordered magnetic phase. Here, we examine the magnetic excitations of FeSc$_2$S$_4$ through time-domain terahertz spectroscopy under an applied magnetic field. At low temperatures an excitation emerges that we attribute to a singlet-triplet excitation from the SOL ground state. A three-fold splitting of this excitation is observed as a function of applied magnetic field. As singlet-triplet excitations are forbidden in inversion symmetric pure spin systems, our results demonstrate the non-trivial character of the entangled spin-orbital singlet ground state. Using experimentally obtained parameters we compare to existing theoretical models to determine FeSc$_2$S$_4$'s proximity to the quantum critical point. In the context of these models, we estimate that the characteristic length of the singlet correlations to be $ξ/ (\textbf{a}/2) \approx 8.2$ (where $\textbf{a}/2$ is the nearest neighbor lattice constant) which establishes FeSc$_2$S$_4$ as a SOL with long-range entanglement.

cond-mat.str-el↗

arXiv2016

Tuning orbital-selective correlation effects in superconducting Rb$_{0.75}$Fe$_{1.6}$Se$_{2-z}$S$_z$

We report on terahertz time-domain spectroscopy on superconducting and metallic iron chalcogenides Rb$_{0.75}$Fe$_{1.6}$Se$_{2-z}$S$_z$. The superconducting transition is reduced from $T_c=$ 32 K ($z=0$) to 22 K ($z=1.0$), and finally suppressed ($z=1.4$) by isoelectronic substitution of Se with S. Dielectric constant and optical conductivity exhibit a metal-to-insulator transition associated with an orbital-selective Mott phase. This orbital-selective Mott transition appears at higher temperature $T_{met}$ with increasing sulfur content, identifying sulfur substitution as an efficient parameter to tune orbital-dependent correlation effects in iron-chalcogenide superconductors. The reduced correlations of the $d_{xy}$ charge carriers can account for the suppression of the superconductivity and the pseudogap-like feature between $T_c$ and $T_{met}$ that was observed for $z=0$.

cond-mat.supr-con↗