Christian Pfleiderer

Topology of Correlated Systems

Technical University of Munich

TUM School of Natural Sciences

James-Franck-Str. 1

85748 Garching

christian.pfleiderer[at]tum.de

Research Website

Description

Research focus: quantum phase transitions, electronic order, topology of correlated systems

The systematic search for quantum order in bulk materials, comprising the synthesis of high-purity single crystals, the experimental exploration of their thermodynamic and transport properties under extreme conditions, as well as microscopic studies using advance neutron and x-ray scattering form the basis for harvesting quantum phenomena in real materials.


phase-plot
Quantum phase transitions

The notion of particle-like elementary excitations represents a cornerstone of present day condensed matter physics. The putative breakdown of this concept in the vicinity of so-called quantum phase transitions, driven by quantum rather than thermal fluctuations, has been attracting tremendous interest for many decades. In turn the materials properties in the vicinity of quantum phase transitions offer an important starting point for an understanding of a wide range of materials with anomalous normal state properties, as well as emergent novel electronic phases such as magnetically mediated superconductivity or partial spin and charge order.


Selected publications

- Formation of a Topological Non-Fermi Liquid in MnSi; Nature, 497, 231 (2013)

- Spin Dynamics and Spin Freezing at Ferromagnetic Quantum Phase Transitions, European Journal of Physics: Special Topics, 224, 1041 (2015)


fermi-surfaces
Complex forms of electronic order

Complex forms of electronic order are intimately connected with the electronic structure and the topological character of the Fermi surface as well as their modification in the presence of strong quantum correlations. The experimental investigation of the electronic structure of materials with complex forms of electronic order permits to track the effects of many body quantum effects and their relationship with thermodynamic and transport properties close to and far from equilibrium.

Selected publications

- Spin-resolved Fermi surface of the localized ferromagnetic Heusler compound Cu2MnAl measured with spin-polarized positron annihilation, Phys. Rev. Lett., 115, 206404 (2015)

- Parasitic small-moment-antiferromagnetism and non-linear coupling of hidden order and antiferromagnetism in URu2Si2 observed by Larmor diffraction, Phys. Rev. Lett., 104, 106406 (2010)

- Superconducting phases of f-electron compounds, Rev. Mod. Phys., 81, 1551 (2009)


topsquirm
Topological phenomena

The notions of symmetry breaking and generalized rigidities have let to a remarkably comprehensive account of complex forms of magnetic order in condensed matter systems. In recent years a new facet of magnetism research receives increasing attention that concerns the topological character of magnetically ordered systems, notably those properties that remain unchanged under elastic deformations. Important examples include skyrmions, vortices and monopoles in chiral or frustrated magnets. These topological aspects of magnetic order are not only appealing from an esthetical and conceptual point of view, but offer strikingly simple explanations for materials properties that may seem to be surprising and hideously complicated at first sight.

Selected publications

- Universal Helimagnon and Skyrmion Excitations in Metallic, Semiconducting, and Insulating Chiral Magnets, Nature Materials 14, 478 (2015)

- Unwinding of a Skyrmion Lattice by Magnetic Monopoles, Science 340, 1076 (2013)

- First Order Metamagnetic Transition in Ho2Ti2O7 observed by Vibrating Coil Magnetometery at Milli- Kelvin Temperatures, Phys. Rev. Lett. 108, 257204 (2012)

- Spin Transfer Torques in MnSi at Ultra-low Current Densities, Science 330, 1648 (2010)

- Skyrmion Lattice in a Chiral Magnet, Science 323, 915 (2009)

Publications

Influence of the magnetovolume effect on the transient reflectivity of MnSi

J. Kalin, S. Sievers, H. W. Schumacher, H. Füser, M. Bieler, A. Bauer, C. Pfleiderer

Physical Review B 110 (1), 14415 (2024).

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The magnetovolume effect is a well established yet frequently overlooked phenomenon in magnetic materials that may affect a wide range of physical properties. Our study explores the influence of the magnetovolume effect on the transient reflectivity of MnSi, a well-known chiral magnet with strong magnetoelastic coupling. We observe a unipolar reflectivity transient in the paramagnetic phase, contrasting with a bipolar response in phases with magnetic long-range order. Comparing our findings with thermal expansion from literature, we establish that the bipolar response originates in the magnetovolume effect which dominates the thermal expansion and influences the optical reflectivity. Our results highlight not only that the magnetovolume effect must be considered when discussing transient reflectivity measurements of magnetic materials but also that such measurements permit to study the characteristic time scales of the magnetovolume effect itself, contributing to a deeper understanding of this often-neglected phenomenon.

DOI: 10.1103/PhysRevB.110.014415

Long-range magnetic order in CePdAl 3 enabled by orthorhombic deformation

M. Stekiel, P. Cermák, C. Franz, M. Meven, D. Legut, W. Simeth, U. B. Hansen, B. Fak, S. Weber, R. Schönmann, V. Kumar, K. Nemkovski, H. Deng, A. Bauer, C. Pfleiderer, A. Schneidewind

Physical Review Research 6 (2), 23117 (2024).

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We investigate the effect of structural deformation on the magnetic properties of orthorhombic CePdAl 3 in relation to its tetragonal polymorph. Utilizing x-ray and neutron diffraction, we establish that the crystal structure has the Cmcm space -group symmetry and exhibits pseudotetragonal twinning. According to density functional calculations, the tetragonal -orthorhombic deformation mechanism has its grounds in the relatively small free enthalpy difference between the polymorphs, allowing either phase to be quenched, and fully accounts for the twinned microstructure of the orthorhombic phase. Neutron diffraction measurements show that orthorhombic CePdAl 3 establishes long-range magnetic order below T N = 5 . 29 (5) K characterized by a collinear, antiferromagnetic arrangement of magnetic moments. Magnetic anisotropies of orthorhombic CePdAl 3 arise from strong spin -orbit coupling as evidenced by the crystal -field splitting of the 4 f multiplet, fully characterised with neutron spectroscopy. We discuss the potential mechanism of frustration posed by antiferromagnetic interactions between nearest neighbors in the tetragonal phase, which hinders the formation of long-range magnetic order in tetragonal CePdAl 3 . We propose that orthorhombic deformation releases the frustration and allows for long-range magnetic order.

DOI: 10.1103/PhysRevResearch.6.023117

Electron-phonon coupling in Mn1-xFexSi

N. Khan, O. D. Pena-Seaman, R. Heid, D. Voneshen, A. H. Said, A. Bauer, T. Konrad, M. Merz, T. Wolf, C. Pfleiderer, F. Weber

Physical Review B 109 (18), 184306 (2024).

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We present a study of the lattice dynamical properties of Mn1-xFexSi with 0 x 0.22. Employing timeof-flight neutron spectroscopy and inelastic x-ray scattering, we investigate the doping dependence of phonon energies, Eph, and linewidths, rph. We find anomalous softening and broadening of a phonon mode propagating along the [111] direction. Ab initio lattice dynamical calculations link this softening to an enhanced electronphonon coupling due to the doping-dependent changes of the Fermi surface. We discuss an interplay of increased electron-phonon coupling and reduced ordered magnetic moments in Mn1-xFexSi.

DOI: 10.1103/PhysRevB.109.184306

Fermi surface of the chiral topological semimetal CoSi

N. Huber, S. Mishra, I. Sheikin, K. Alpin, A. P. Schnyder, G. Benka, A. Bauer, C. Pfleiderer, M. A. Wilde

Physical Review B 109 (20), 205115 (2024).

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We report a study of the Fermi surface of the chiral semimetal CoSi and its relationship to a network of multifold topological crossing points, Weyl points, and topological nodal planes in the electronic band structure. Combining quantum oscillations in the Hall resistivity, magnetization, and torque magnetization with ab initio electronic structure calculations, we identify two groups of Fermi -surface sheets, one centered at the R point and the other centered at the 1 . ' point. The presence of topological nodal planes at the Brillouin zone boundary enforces topological protectorates on the Fermi -surface sheets centered at the R point. In addition, Weyl points exist close to the Fermi -surface sheets centered at the R and the 1 . ' points. In contrast, topological crossing points at the R point and the 1 . ' point, which have been advertised to feature exceptionally large Chern numbers, are located at a larger distance to the Fermi level. Representing a unique example in which the multitude of topological band crossings has been shown to form a complex network, our observations in CoSi highlight the need for detailed numerical calculations of the Berry curvature at the Fermi level, regardless of the putative existence and the possible character of topological band crossings in the band structure.

DOI: 10.1103/PhysRevB.109.205115

Topological aspects of multi-k antiferromagnetism in cubic rare-earth compounds

W. Simeth, M. C. Rahn, A. Bauer, M. Meven, C. Pfleiderer

Journal of Physics-Condensed Matter 36 (21), 215602 (2024).

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We advertise rare-earth intermetallics with high-symmetry crystal structures and competing interactions as a possible materials platform hosting spin structures with non-trivial topological properties. Focusing on the series of cubic RCu compounds, where R = Ho, Er, Tm, the bulk properties of these systems display exceptionally rich magnetic phase diagrams hosting an abundance of different phase pockets characteristic of antiferromagnetic order in the presence of delicately balanced interactions. The electrical transport properties exhibit large anomalous contributions suggestive of topologically non-trivial winding in the electronic and magnetic structures. Neutron diffraction identifies spontaneous long-range magnetic order in terms of commensurate and incommensurate variations of (pi pi 0) antiferromagnetism with the possibility for various multi- k configurations. Motivated by general trends in these materials, we discuss the possible existence of topologically non-trivial winding in real and reciprocal space in the class of RCu compounds including antiferromagnetic skyrmion lattices. Putatively bringing together different limits of non-trivial topological winding in the same material, the combination of properties in RCu systems promises access to advanced functionalities.

DOI: 10.1088/1361-648X/ad24bb

Optical creation and annihilation of skyrmion patches in a chiral magnet

J. Kalin, S. Sievers, H. W. Schumacher, R. Abram, H. Füser, M. Bieler, D. Kalin, A. Bauer, C. Pfleiderer

Physical Review Applied 21 (3), 34065 (2024).

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A key challenge for the realization of future skyrmion devices comprises the controlled creation, annihilation, and detection of these topologically nontrivial magnetic textures. In this study, we report an alloptical approach for writing, deleting, and reading skyrmions in the chiral magnet Fe0.75Co0.25Si based on thermal quenching. Using focused femtosecond laser pulses, patches of a thermally metastable skyrmion lattice state are created and annihilated locally, demonstrating unprecedented control of skyrmions in chiral magnets. The skyrmion state is read out by analyzing the microwave spin excitations in time-resolved magneto-optical Kerr effect measurements. Extracting the magnetic field and laser-fluence dependence, we find well-separated magnetic field regimes and different laser-fluence thresholds for the laser-induced creation and annihilation of skyrmions. The all-optical skyrmion control, as established in this study for a model system, represents a promising and energy-efficient approach for the realization of skyrmions as magnetic bits in future storage devices, reminiscent of magneto-optical storage devices in the past.

DOI: 10.1103/PhysRevApplied.21.034065

Quantum oscillations of the quasiparticle lifetime in a metal

N. Huber, V. Leeb, A. Bauer, G. Benka, J. Knolle, C. Pfleiderer, M. A. Wilde

Nature 621 (7978), 276-+ (2023).

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Following nearly a century of research, it remains a puzzle that the low-lying excitations of metals are remarkably well explained by effective single-particle theories of non-interacting bands(1-4). The abundance of interactions in real materials raises the question of direct spectroscopic signatures of phenomena beyond effective single-particle, single-band behaviour. Here we report the identification of quantum oscillations (QOs) in the three-dimensional topological semimetal CoSi, which defy the standard description in two fundamental aspects. First, the oscillation frequency corresponds to the difference of semiclassical quasiparticle (QP) orbits of two bands, which are forbidden as half of the trajectory would oppose the Lorentz force. Second, the oscillations exist up to above 50 K, in strong contrast to all other oscillatory components, which vanish below a few kelvin. Our findings are in excellent agreement with generic model calculations of QOs of the QP lifetime (QPL). Because the only precondition for their existence is a nonlinear coupling of at least two electronic orbits, for example, owing to QP scattering on defects or collective excitations, such QOs of the QPL are generic for any metal featuring Landau quantization with several orbits. They are consistent with certain frequencies in topological semimetals(5-9), unconventional superconductors(10,11), rare-earth compounds(12-14) and Rashba systems(15), and permit to identify and gauge correlation phenomena, for example, in two-dimensional materials(16,17) and multiband metals(18).

DOI: 10.1038/s41586-023-06330-y

Resonant Elastic X-Ray Scattering of Antiferromagnetic Superstructures in EuPtSi3

W. Simeth, A. Bauer, C. Franz, A. Aqeel, P. J. Bereciartua, J. A. Sears, S. Francoual, C. H. Back, C. Pfleiderer

Physical Review Letters 130 (26), 266701 American Physical Society, (2023).

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We report resonant elastic x-ray scattering of long-range magnetic order in EuPtSi3, combining different scattering geometries with full linear polarization analysis to unambiguously identify magnetic scattering contributions. At low temperatures, EuPtSi3 stabilizes type A antiferromagnetism featuring various long -wavelength modulations. For magnetic fields applied in the hard magnetic basal plane, well-defined regimes of cycloidal, conical, and fanlike superstructures may be distinguished that encompass a pocket of commensurate type A order without superstructure. For magnetic field applied along the easy axis, the phase diagram comprises the cycloidal and conical superstructures only. Highlighting the power of polarized resonant elastic x-ray scattering, our results reveal a combination of magnetic phases that suggest a highly unusual competition between antiferromagnetic exchange interactions with Dzyaloshinsky-Moriya spin-orbit coupling of similar strength.

DOI: 10.1103/PhysRevLett.130.266701

Low-temperature antiferromagnetic order in orthorhombic CePdAl3

V. Kumar, A. Bauer, C. Franz, J. Spallek, R. Schönmann, M. Stekiel, A. Schneidewind, M. A. Wilde, C. Pfleiderer

Physical Review Research 5 (2), 23157 (2023).

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We report the magnetization, ac susceptibility, and specific heat of optically float-zoned single crystals of CePdAl3. In comparison to the properties of polycrystalline CePdAl3 reported in the literature, which displays a tetragonal crystal structure and no long-range magnetic order, our single crystals exhibit an orthorhombic structure (Cmcm) and antiferromagnetic order below a Neel temperature T1 = 5.6 K. The specific heat at zero field shows two anomalies, namely, a broad transition at T1 = 5.6 K followed by a λ-anomaly at T2 = 5.4 K. A conservative estimate of the Sommerfeld coefficient of the electronic specific heat, γ = 121 mJ K-2 mol-1, indicates a moderately enhanced heavy-fermion ground state. A twin microstructure evolves in the family of planes spanned by the basal plane lattice vectors ao and co, with the magnetic hard axis bo common to all twins. The antiferromagnetic state is characterized by a strong ao, co easy-plane magnetic anisotropy where the ao direction is the easy axis in the easy plane. A spin-flop transition induced under magnetic field along the easy directions, results in complex magnetic phase diagrams. Taken together, our results reveal a high sensitivity of the magnetic and electronic properties of CePdAl3 to its structural modifications.

DOI: 10.1103/PhysRevResearch.5.023157

Small-angle neutron scattering of long-wavelength magnetic modulations in reduced sample dimensions

G. L. Causer, A. Chacon, A. Heinemann, C. Pfleiderer

Journal of Applied Crystallography 56, 26-35 (2023).

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Magnetic small-angle neutron scattering (SANS) is ideally suited to providing direct reciprocal-space information on long-wavelength magnetic modulations, such as helicoids, solitons, merons or skyrmions. SANS of such structures in thin films or micro-structured bulk materials is strongly limited by the tiny scattering volume vis a vis the prohibitively high background scattering by the substrate and support structures. Considering near-surface scattering just above the critical angle of reflection, where unwanted signal contributions due to substrate or support structures become very small, it is established that the scattering patterns of the helical, conical, skyrmion lattice and fluctuation-disordered phases in a polished bulk sample of MnSi are equivalent for conventional transmission and near-surface SANS geometries. This motivates the prediction of a complete repository of scattering patterns expected for thin films in the near-surface SANS geometry for each orientation of the magnetic order with respect to the scattering plane.

DOI: 10.1107/s1600576722010755

Magnetocaloric Properties of R3Ga5O12 (R = Tb, Gd, Nd, Dy)

M. Kleinhans, K. Eibensteiner, J. C. Leiner, C. Resch, L. Worch, M. A. Wilde, J. Spallek, A. Regnat, C. Pfleiderer

Physical Review Applied 19 (1), 14038 (2023).

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We report the characteristic magnetic properties of several members of the family of rare-earth gar-nets, Gd3Ga5O12 (GGG), Dy3Ga5O12, Tb3Ga5O12, and Nd3Ga5O12, and compare their relative potential utility for magnetocaloric cooling, including their minimal adiabatic demagnetization refrigeration (ADR) temperatures and relative cooling parameters. A main objective of this work concerns the identification of potential improvements over the magnetocaloric properties of GGG for use in low-temperature ADR cryostats. Using Tb+3 and Dy+3 at the rare-earth site offers, in principle, a higher saturation magnetization and Nd+3 gives a lower de Gennes factor and therefore potentially reduced magnetic transition tempera-tures, limiting the useful temperature range. Our results show that Dy3Ga5O12 yields an optimal relative cooling parameter at low applied fields and low limiting temperatures, which would allow for the design of more efficient ADR cryostats.

DOI: 10.1103/PhysRevApplied.19.014038

Incommensurate antiferromagnetic order in CePtAl3

M. Stekiel, P. Cermak, C. Franz, W. Simeth, S. Weber, E. Ressouche, W. Schmidt, K. Nemkovski, H. Deng, A. Bauer, C. Pfleiderer, A. Schneidewind

Physical Review Research 5 (1), 13058 (2023).

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We report on a neutron diffraction study of single-crystal CePtAl3 complemented by measurements of the specific heat under applied magnetic field. Below TN approximate to 3 K, CePtAl3 develops incommensurate antiferromag-netic order with a single modulation vector k = (0.676 0 0). Residual magnetic scattering intensity above TN and a broadening of the specific heat anomaly at TN may be consistently described in terms of a Gaussian distribution of transition temperatures with a standard deviation sigma approximate to 0.5 K. The distribution of TN may be attributed to the observation of occupational and positional disorder between the Pt and Al sites consistent with structural information inferred from neutron diffraction. Measurements under magnetic field reveal changes of the magnetic domain populations when the field is applied along the [010] direction consistent with a transition from cycloidal to amplitude-modulated magnetic order similar to 2.5 T.

DOI: 10.1103/PhysRevResearch.5.013058

Optimization strategies and artifacts of time-involved small-angle neutron scattering experiments

D. Mettus, A. Chacon, A. Bauer, S. Muhlbauer, C. Pfleiderer

Journal of Applied Crystallography 55, 1603-1612 (2022).

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Kinetic small-angle neutron scattering provides access to the microscopic properties of mesoscale systems under slow, periodic perturbations. By interlocking the phases of neutron pulse, sample modulation and detector signal, time-involved small-angle neutron scattering experiments (TISANE) allow one to exploit the neutron velocity spread and record data without major sacrifice in intensity at timescales down to microseconds. This article reviews the optimization strategies of TISANE that arise from specific aspects of the process of data acquisition and data analysis starting from the basic principles of operation. Typical artifacts of data recorded in TISANE due to the choice of time binning and neutron chopper pulse width are illustrated by virtue of the response of the skyrmion lattice in MnSi under periodic changes of the direction of the stabilizing magnetic field.

DOI: 10.1107/s1600576722009931

Neutron depolarization due to ferromagnetism and spin freezing in CePd1-xRhx

M. Seifert, P. Schmakat, M. Schulz, P. Jorba, V. Hutanu, C. Geibel, M. Deppe, C. Pfleiderer

Physical Review Research 4 (4), 43029 (2022).

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We report neutron depolarization measurements of the suppression of long-range ferromagnetism and the concomitant emergence of magnetic irreversibilities and spin freezing in CePd1-xRhx around x* approximate to 0.6. Tracking the temperature versus field history of the neutron depolarization, we find clear signatures of long-range Ising ferromagnetism below a Curie temperature TC for x = 0.4 and a spin freezing of ferromagnetic clusters below a freezing temperature TF1 for x > x*. Under zero-field-cooling/field-heating and for x > x* a reentrant temperature dependence of the neutron depolarization between TF2 < TF1 and TF1 is microscopically consistent with a thermally activated growth of the cluster size. The evolution of the depolarization as well as the reentrant temperature dependence as a function of Rh content are consistent with the formation of a Kondo cluster glass below TF1 adjacent to a ferromagnetic quantum phase transition at x*.

DOI: 10.1103/PhysRevResearch.4.043029

Emergence of mesoscale quantum phase transitions in a ferromagnet

A. Wendl, H. Eisenlohr, F. Rucker, C. Duvinage, M. Kleinhans, M. Vojta, C. Pfleiderer

Nature 609 (7925), 65-+ (2022).

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Mesoscale patterns as observed in, for example, ferromagnets, ferroelectrics, superconductors, monomolecular films or block copolymers(1,2) reflect spatial variations of a pertinent order parameter at length scales and time scales that may be described classically. This raises the question for the relevance of mesoscale patterns near zero-temperature phase transitions, also known as quantum phase transitions. Here we report the magnetic susceptibility of LiHoF4-a dipolar Ising ferromagnet-near a well-understood transverse-field quantum critical point (TF-QCP)(3,4). When tilting the magnetic field away from the hard axis such that the Ising symmetry is always broken, a line of well-defined phase transitions emerges from the TF-QCP, characteristic of further symmetry breaking, in stark contrast to a crossover expected microscopically. We show that the scenario of a continuous suppression of ferromagnetic domains, representing a breaking of translation symmetry on mesoscopic scales in an environment of broken magnetic Ising symmetry on microscopic scales, is in excellent qualitative and quantitative agreement with the field and temperature dependence of the susceptibility and the magnetic phase diagram of LiHoF4 under tilted field. This identifies a new type of phase transition that may be referred to as mesoscale quantum criticality, which emanates from the textbook example of a microscopic ferromagnetic TF-QCP. Our results establish the surroundings of quantum phase transitions as a regime of mesoscale pattern formation, in which non-analytical quantum dynamics and materials properties without classical analogue may be expected.

DOI: 10.1038/s41586-022-04995-5

Optically excited spin dynamics of thermally metastable skyrmions in Fe0.75Co0.25Si

J. Kalin, S. Sievers, H. Fuser, H. W. Schumacher, M. Bieler, F. Garcia-Sanchez, A. Bauer, C. Pfleiderer

Physical Review B 106 (5), 54430 (2022).

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We investigate the microwave spin excitations of the cubic chiral magnet Fe0.75Co0.25Si as driven by the thermal modulation of magnetic interactions via laser heating and probed by time-resolved measurements of the magneto-optical Kerr effect. Focusing on the topologically nontrivial skyrmion lattice state, the dynamic properties in thermodynamic equilibrium are compared with those of a metastable state prepared by means of rapid field cooling. In both cases, we find precessional and exponential contributions to the dynamic response, characteristic of a breathing mode and energy dissipation, respectively. When taking into account the universal scaling as a function of temperature, the precession frequencies in the equilibrium and metastable skyrmion state are in excellent quantitative agreement. This finding highlights that skyrmion states far from thermal equilibrium promise great flexibility, for instance, with respect to temperature and field scales, both for possible microwave applications and for the study of fundamental properties.

DOI: 10.1103/PhysRevB.106.054430

Network of Topological Nodal Planes, Multifold Degeneracies, and Weyl Points in CoSi

N. Huber, K. Alpin, G. L. Causer, L. Worch, A. Bauer, G. Benka, M. M. Hirschmann, A. P. Schnyder, C. Pfleiderer, M. A. Wilde

Physical Review Letters 129 (2), 26401 (2022).

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We showcase the importance of global band topology in a study of the Weyl semimetal CoSi as a representative of chiral space group (SG) 198. We identify a network of band crossings comprising topological nodal planes, multifold degeneracies, and Weyl points consistent with the fermion doubling theorem. To confirm these findings, we combined the general analysis of the band topology of SG 198 with Shubnikov???de Haas oscillations and material-specific calculations of the electronic structure and Berry curvature. The observation of two nearly dispersionless Shubnikov???de Haas frequency branches provides unambiguous evidence of four Fermi surface sheets at the R point that reflect the symmetry-enforced orthogonality of the underlying wave functions at the intersections with the nodal planes. Hence, irrespective of the spin-orbit coupling strength, SG 198 features always six-and fourfold degenerate crossings at R and ?? that are intimately connected to the topological charges distributed across the network.

DOI: 10.1103/PhysRevLett.129.026401

Large curvature near a small gap

M. A. Wilde, C. Pfleiderer

Nature Physics 18 (7), 731-732 (2022).

DOI: 10.1038/s41567-022-01623-x

Compositional Studies of Metals with Complex Order by means of the Optical Floating-Zone Technique

A. Bauer, G. Benka, A. Neubauer, A. Regnat, A. Engelhardt, C. Resch, S. Wurmehl, C. G. F. Blum, T. Adams, A. Chacon, R. Jungwirth, R. Georgii, A. Senyshyn, B. Pedersen, M. Meven, C. Pfleiderer

Physica Status Solidi B-Basic Solid State Physics 259 (5), 2100159 (2022).

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The availability of large high-quality single crystals is an important prerequisite for many studies in solid-state research. The optical floating-zone technique is an elegant method to grow such crystals, offering potential to prepare samples that may be hardly accessible with other techniques. As elaborated in this report, examples include single crystals with intentional compositional gradients, deliberate off-stoichiometry, or complex metallurgy. For the cubic chiral magnets Mn1-xFexSi and Fe1-xCoxSi, single crystals are prepared in which the composition is varied during growth from x = 0 to 0.15 and from x = 0.1 to 0.3, respectively. Such samples allow us to efficiently study the evolution of the magnetic properties as a function of composition, as demonstrated by means of neutron scattering. For the archetypical chiral magnet MnSi and the itinerant antiferromagnet CrB2, single crystals with varying initial manganese (0.99-1.04) and boron (1.95-2.1) content are grown. Measurements of the low-temperature properties address the correlation between magnetic transition temperature and sample quality. Furthermore, single crystals of the diborides ErB2, MnB2, and VB2 are prepared. In addition to high vapor pressures, these materials suffer from peritectic formation, potential decomposition, and high melting temperature, respectively.

DOI: 10.1002/pssb.202100159

High-Pressure Studies of Correlated Electron Systems

P. Jorba, A. Regnat, A. Tong, M. Seifert, A. Bauer, M. Schulz, C. Franz, A. Schneidewind, S. Kunkemoller, K. Jenni, M. Braden, A. Deyerling, M. A. Wilde, J. S. Schilling, C. Pfleiderer

Physica Status Solidi B-Basic Solid State Physics 259 (5), 2100623 (2022).

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Tuning the electronic properties of transition-metal and rare-earth compounds by virtue of changes of the crystallographic lattice constants offers controlled access to new forms of order. The development of tungsten carbide (WC) and moissanite Bridgman cells conceived for studies of the electrical resistivity up to 10 GPa, as well as bespoke diamond anvil cells (DACs) developed for neutron depolarization studies up to 20 GPa is reviewed. For the DACs, the applied pressure changes as a function of temperature in quantitative agreement with the thermal expansion of the pressure cell. A setup is described that is based on focusing neutron guides for measurements of the depolarization of a neutron beam by samples in a DAC. The technical progress is illustrated in terms of three examples. Measurements of the resistivity and neutron depolarization provide evidence of ferromagnetic order in SrRuO3 up to 14 GPa close to a putative quantum phase transition. Combining hydrostatic, uniaxial, and quasi-hydrostatic pressure, the emergence of incipient superconductivity in CrB2 is observed. The temperature dependence of the electrical resistivity in CeCuAl3 is consistent with emergent Kondo correlations and an enhanced coupling of magneto-elastic excitations with the conduction electrons at low and intermediate temperatures, respectively.

DOI: 10.1002/pssb.202100623

Interplay of itinerant magnetism and spin-glass behavior in FexCr1-x

G. Benka, A. Bauer, P. Schmakat, S. Saubert, M. Seifert, P. Jorba, C. Pfleiderer

Physical Review Materials 6 (4), 44407 (2022).

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When suppressing the itinerant antiferromagnetism in chromium by doping with the isostructural itinerant ferromagnet iron, a dome of spin-glass behavior emerges around a putative quantum critical point at an iron concentration x approximate to 0.15. Here, we report a comprehensive investigation of polycrystalline samples of FexCr1-x in the range 0.05 <= x <= 0.30 using x-ray powder diffraction, magnetization, ac susceptibility, and neutron depolarization measurements, complemented by specific heat and electrical resistivity data for x = 0.15. Besides antiferromagnetic (x < 0.15) and ferromagnetic regimes (x >= 0.15), we identify a dome of spin-glass behavior at low temperatures for 0.10 <= x <= 0.25. Neutron depolarization measurements indicate an increase of the size of ferromagnetic clusters with increasing x and the Mydosh parameter phi, inferred from the ac susceptibility, implies a crossover from cluster-glass to superparamagnetic behavior. Taken together, these findings consistently identify FexCr1-x as an itinerant-electron system that permits to study the evolution of spin-glass behavior of gradually varying character in an unchanged crystalline environment.

DOI: 10.1103/PhysRevMaterials.6.044407

Topological magnon band structure of emergent Landau levels in a skyrmion lattice

T. Weber, D. M. Fobes, J. Waizner, P. Steffens, G. S. Tucker, M. Bohm, L. Beddrich, C. Franz, H. Gabold, R. Bewley, D. Voneshen, M. Skoulatos, R. Georgii, G. Ehlers, A. Bauer, C. Pfleiderer, P. Boni, M. Janoschek, M. Garst

Science 375 (6584), 1025-+ (2022).

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The motion of a spin excitation across topologically nontrivial magnetic order exhibits a deflection that is analogous to the effect of the Lorentz force on an electrically charged particle in an orbital magnetic field. We used polarized inelastic neutron scattering to investigate the propagation of magnons (i.e., bosonic collective spin excitations) in a lattice of skyrmion tubes in manganese silicide. For wave vectors perpendicular to the skyrmion tubes, the magnon spectra are consistent with the formation of finely spaced emergent Landau levels that are characteristic of the fictitious magnetic field used to account for the nontrivial topological winding of the skyrmion lattice. This provides evidence of a topological magnon band structure in reciprocal space, which is borne out of the nontrivial real-space topology of a magnetic order.

DOI: 10.1126/science.abe4441

Magnetic properties of the noncentrosymmetric tetragonal antiferromagnet EuPtSi3

A. Bauer, A. Senyshyn, R. Bozhanova, W. Simeth, C. Franz, S. Gottlieb-Schonmeyer, M. Meven, T. E. Schrader, C. Pfleiderer

Physical Review Materials 6 (3), 34406 (2022).

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We report a comprehensive study of single crystals of the noncentrosymmetric rare-earth compound EuPtSi3 grown by the optical floating-zone technique. Measurements of the magnetization, ac susceptibility, and specific heat consistently establish antiferromagnetic order of localized Eu2+ moments below the Ned temperature T-N = 17 K, followed by a second magnetic transition at T-N1 = 16 K. For a magnetic field along the easy [001] axis, the magnetic phase diagram is composed of these two phases. For fields applied in the magnetically hard basal plane, two additional phases emerge under magnetic field, where the in-plane anisotropy is weak with [100] being the hardest axis. At the phase transitions, the magnetic properties exhibit hysteresis and discrepancies between differential and ac susceptibility, suggesting slow reorientation processes of mesoscale magnetic textures. Consistently, powder and single-crystal neutron diffraction in zero field identify magnetic textures that are modulated on a length scale of the order of 100 angstrom, most likely in the form of Ned-type antiferromagnetic cycloids.

DOI: 10.1103/PhysRevMaterials.6.034406

Tunable cooperativity in coupled spin-cavity systems

L. Liensberger, F. X. Haslbeck, A. Bauer, H. Berger, R. Gross, H. Hübl, C. Pfleiderer, M. Weiler

Physical Review B 104 (10), L100415 (2021).

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We experimentally study the tunability of the cooperativity in coupled spin-cavity systems by changing the magnetic state of the spin system via an external control parameter. As a model system, we use the skyrmion host material Cu2OSeO3 coupled to a microwave cavity resonator. We measure a dispersive coupling between the resonator and magnon modes in different magnetic phases of the material and model our results by using the input-output formalism. Our results show a strong tunability of the normalized coupling rate by magnetic field, allowing us to change the magnon-photon cooperativity from 1 to 60 at the phase boundaries of the skyrmion lattice state.

DOI: 10.1103/PhysRevB.104.L100415

Confined dipole and exchange spin waves in a bulk chiral magnet with Dzyaloshinskii-Moriya interaction

P. Che, I. Stasinopoulos, A. Mucchietto, J. N. Li, H. Berger, A. Bauer, C. Pfleiderer, D. Grundler

Physical Review Research 3 (3), 33104 (2021).

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The Dzyaloshinskii-Moriya interaction (DMI) has an impact on excited spin waves in the chiral magnet Cu2OSeO3 by means of introducing asymmetry in their dispersion relations. The confined eigenmodes of a chiral magnet are hence no longer the conventional standing spin waves. Here we report a combined experimental and micromagnetic modeling study by broadband microwave spectroscopy, and we observe confined spin waves up to eleventh order in bulk Cu2OSeO3 in the field-polarized state. In micromagnetic simulations we find similarly rich spectra. They indicate the simultaneous excitation of both dipole- and exchange-dominated spin waves with wavelengths down to (47.2 +/- 0.05) nm attributed to the exchange interaction modulation. Our results suggest the DMI to be effective in creating exchange spin waves in a bulk sample without the challenging nanofabrication and thereby in exploring their scattering with noncollinear spin textures.

DOI: 10.1103/PhysRevResearch.3.033104

Symmetry-enforced topological nodal planes at the Fermi surface of a chiral magnet

M. A. Wilde, M. Dodenhoft, A. Niedermayr, A. Bauer, M. M. Hirschmann, K. Alpin, A. P. Schnyder, C. Pfleiderer

Nature 594 (7863), 374-+ (2021).

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Despite recent efforts to advance spintronics devices and quantum information technology using materials with non-trivial topological properties, three key challenges are still unresolved(1-9). First, the identification of topological band degeneracies that are generically rather than accidentally located at the Fermi level. Second, the ability to easily control such topological degeneracies. And third, the identification of generic topological degeneracies in large, multisheeted Fermi surfaces. By combining de Haas-van Alphen spectroscopy with density functional theory and band-topology calculations, here we show that the non-symmorphic symmetries(10-17) in chiral, ferromagnetic manganese silicide (MnSi) generate nodal planes (NPs)(11,12), which enforce topological protectorates (TPs) with substantial Berry curvatures at the intersection of the NPs with the Fermi surface (FS) regardless of the complexity of the FS. We predict that these TPs will be accompanied by sizeable Fermi arcs subject to the direction of the magnetization. Deriving the symmetry conditions underlying topological NPs, we show that the 1,651 magnetic space groups comprise 7 grey groups and 26 black-and-white groups with topological NPs, including the space group of ferromagnetic MnSi. Thus, the identification of symmetry-enforced TPs, which can be controlled with a magnetic field, on the FS of MnSi suggests the existence of similar properties-amenable for technological exploitation-in a large number of materials.

DOI: 10.1038/s41586-021-03543-x

Atomistic investigation of surface characteristics and electronic features at high-purity FeSi(110) presenting interfacial metallicity

B. Yang, M. Uphoff, Y. Q. Zhang, J. Reichert, A. P. Seitsonen, A. Bauer, C. Pfleiderer, J. V. Barth

Proceedings of the National Academy of Sciences of the United States of America 118 (17), e2021203118 (2021).

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Iron silicide (FeSi) is a fascinating material that has attracted extensive research efforts for decades, notably revealing unusual temperature-dependent electronic and magnetic characteristics, as well as a close resemblance to the Kondo insulators whereby a coherent picture of intrinsic properties and underlying physics remains to be fully developed. For a better understanding of this narrow-gap semiconductor, we prepared and examined FeSi(110) single-crystal surfaces of high quality. Combined insights from low-temperature scanning tunneling microscopy and density functional theory calculations (DFT) indicate an unreconstructed surface termination presenting rows of Fe?Si pairs. Using high-resolution tunneling spectroscopy (STS), we identify a distinct asymmetric electronic gap in the sub-10 K regime on defect-free terraces. Moreover, the STS data reveal a residual density of states in the gap regime whereby two in-gap states are recognized. The principal origin of these features is rationalized with the help of the DFT-calculated band structure. The computational modeling of a (110)-oriented slab notably evidences the existence of interfacial intragap bands accounting for a markedly increased density of states around the Fermi level. These findings support and provide further insight into the emergence of surface metallicity in the low-temperature regime.

DOI: 10.1073/pnas.2021203118

Microwave Spectroscopy of the Low-Temperature Skyrmion State in Cu2OSeO3

A. Aqeel, J. Sahliger, T. Taniguchi, S. Mandl, D. Mettus, H. Berger, A. Bauer, M. Garst, C. Pfleiderer, C. H. Back

Physical Review Letters 126 (1), 17202 (2021).

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In the cubic chiral magnet Cu2OSeO3 a low-temperature skyrmion state (LTS) and a concomitant tilted conical state are observed for magnetic fields parallel to h100i. Here, we report on the dynamic resonances of these novel magnetic states. After promoting the nucleation of the LTS by means of field cycling, we apply broadband microwave spectroscopy in two experimental geometries that provide either predominantly in-plane or out-of-plane excitation. By comparing the results to linear spin-wave theory, we clearly identify resonant modes associated with the tilted conical state, the gyrational and breathing modes associated with the LTS, as well as the hybridization of the breathing mode with a dark octupole gyration mode mediated by the magnetocrystalline anisotropies. Most intriguingly, our findings suggest that under decreasing fields the hexagonal skyrmion lattice becomes unstable with respect to an oblique deformation, reflected in the formation of elongated skyrmions.

DOI: 10.1103/PhysRevLett.126.017202

Field-induced reorientation of helimagnetic order in Cu2OSeO3 probed by magnetic force microscopy

P. Milde, L. Kohler, E. Neuber, P. Ritzinger, M. Garst, A. Bauer, C. Pfleiderer, H. Berger, L. M. Eng

Physical Review B 102 (2), 24426 (2020).

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Cu2OSeO3 is an insulating skyrmion-host material with a magnetoelectric coupling giving rise to an electric polarization with a characteristic dependence on the magnetic-field (H) over right arrow. We report a magnetic force microscopy imaging of the helical real-space spin structure on the surface of a bulk single crystal of Cu2OSeO3. In the presence of a magnetic field, the helimagnetic order, in general, reorients and acquires a homogeneous component of the magnetization, resulting in a conical arrangement at larger fields. We investigate this reorientation process at a temperature of 10 K for fields close to the crystallographic < 110 > direction that involves a phase transition at H-c1. Experimental evidence is presented for the formation of magnetic domains in real space as well as for the microscopic origin of relaxation events that accompany the reorientation process. In addition, the electric polarization is measured by means of Kelvin-probe force microscopy. We show that the characteristic field dependency of the electric polarization originates in this helimagnetic reorientation process. Our experimental results are well described by an effective Landau theory previously invoked for MnSi, that captures the competition between magnetocrystalline anisotropies and Zeeman energy.

DOI: 10.1103/PhysRevB.102.024426

The 2020 Skyrmionics roadmap

C.H. Back, V. Cros, H. Ebert, K. Everschor-Sitte, A. Fert, M. Garst, Tianping Ma, S. Mankovsky, T. L. Monchesky, M. Mostovoy, N. Nagaosa, S.S.P. Parkin, C. Pfleiderer, N. Reyren, A. Rosch, Y. Taguchi, Y. Tokura, K. von Bergmann, J. Zang

Journal of Physics D: Applied Physics 53, 363001 (2020).

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The notion of non-trivial topological winding in condensed matter systems represents a major area of present-day theoretical and experimental research. Magnetic materials offer a versatile platform that is particularly amenable for the exploration of topological spin solitons in real space such as skyrmions. First identified in non-centrosymmetric bulk materials, the rapidly growing zoology of materials systems hosting skyrmions and related topological spin solitons includes bulk compounds, surfaces, thin films, heterostructures, nano-wires and nano-dots. This underscores an exceptional potential for major breakthroughs ranging from fundamental questions to applications as driven by an interdisciplinary exchange of ideas between areas in magnetism which traditionally have been pursued rather independently. The skyrmionics Roadmap provides a review of the present state of the art and the wide range of research directions and strategies currently under way. These are, for instance, motivated by the identification of the fundamental structural properties of skyrmions and related textures, processes of nucleation and annihilation in the presence of non-trivial topological winding, an exceptionally efficient coupling to spin currents generating spin transfer torques at tiny current densities, as well as the capability to purpose-design broad-band spin dynamic and logic devices.

DOI: 10.1088/1361-6463/ab8418

Orientation dependence of the magnetic phase diagram of Yb2Ti2O7

S. Saubert, A. Scheie, C. Duvinage, J. Kindervater, S. Zhang, H. J. Changlani, G. Y. Xu, S. M. Koohpayeh, O. Tchernyshyov, C. L. Broholm, C. Pfleiderer

Physical Review B 101 (17), 174434 (2020).

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In the quest to realize a quantum spin liquid (QSL), magnetic long-range order is hardly welcome. Yet it can offer deep insights into a complex world of strong correlations and fluctuations. Much hope was placed in the cubic pyrochlore Yb2Ti2O7 as a putative U(1) QSL but a new class of ultrapure single crystals make it abundantly clear that the stoichiometric compound is a ferromagnet. Here we present a detailed experimental and theoretical study of the corresponding field-temperature phase diagram. We find it to be richly anisotropic with a critical endpoint for B parallel to < 100 >, while a field parallel to < 110 > or < 111 > enhances the critical temperature by up to a factor of two and shifts the onset of the field-polarized state to finite fields. Landau theory shows that Yb2Ti2O7 in some ways is remarkably similar to pure iron. However, it also pinpoints anomalies that cannot be accounted for at the classical mean-field level including a dramatic enhancement of T-C and a reentrant phase boundary under applied magnetic fields with a component transverse to the easy axes, as well as the anisotropy of the upper critical field in the quantum limit.

DOI: 10.1103/PhysRevB.101.174434

Evolution of magnetocrystalline anisotropies in Mn1-xFexSi and Mn1-xCoxSi as inferred from small-angle neutron scattering and bulk properties

J. Kindervater, T. Adams, A. Bauer, F. X. Haslbeck, A. Chacon, S. Muhlbauer, F. Jonietz, A. Neubauer, U. Gasser, G. Nagy, N. Martin, W. Haussler, R. Georgii, M. Garst, C. Pfleiderer

Physical Review B 101 (10), 104406 (2020).

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We report a comprehensive small-angle neutron scattering (SANS) study of magnetic correlations in Mn1-xFexSi at zero magnetic field. To delineate changes of magnetocrystalline anisotropies (MCAs) from effects due to defects and disorder, we recorded complementary susceptibility and high-resolution specific heat data and investigated selected compositions of Mn1-xCoxSi. For all systems studied, the helimagnetic transition temperature and magnetic phase diagrams evolve monotonically with composition consistent with literature. The SANS intensity patterns of the spontaneous magnetic order recorded under zero-field cooling, which were systematically tracked over forty angular positions, display strong changes of the directions of the intensity maxima and smeared out intensity distributions as a function of composition. We show that cubic MCAs account for the complex evolution of the SANS patterns, where for increasing x the character of the MCAs shifts from terms that are fourth order to terms that are sixth order in spin-orbit coupling. The magnetic field dependence of the susceptibility and SANS establishes that the helix reorientation as a function of magnetic field for Fe- or Co-doped MnSi is dominated by pinning due to defects and disorder. The presence of well-defined thermodynamic anomalies of the specific heat at the phase boundaries of the skyrmion lattice phase in the doped samples and properties observed in Mn1-xCoxSi establishes that the pinning due to defects and disorder remains, however, weak and comparable to the field scale of the helix reorientation. The observation that MCAs, which are sixth order in spin-orbit coupling, play an important role for the spontaneous order in Mn1-xFexSi and Mn1-xCoxSi offers a fresh perspective for a wide range of topics in cubic chiral magnets such as the generic magnetic phase diagram, the morphology of topological spin textures, the paramagnetic-to-helical transition, and quantum phase transitions.

DOI: 10.1103/PhysRevB.101.104406

Weak Crystallization of Fluctuating Skyrmion Textures in MnSi

J. Kindervater, I. Stasinopoulos, A. Bauer, F. X. Haslbeck, F. Rucker, A. Chacon, S. Muhlbauer, C. Franz, M. Garst, D. Grundler, C. Pfleiderer

Physical Review X 9 (4), 41059 (2019).

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We report an experimental study of the emergence of nontrivial topological winding and long-range order across the paramagnetic-to-skyrmion lattice transition in the transition metal helimagnet MnSi. Combining measurements of the susceptibility with small-angle neutron scattering, neutron-resonance spin-echo spectroscopy, and all-electrical microwave spectroscopy, we find evidence of skyrmion textures in the paramagnetic state exceeding 10(3) angstrom, with lifetimes above several 10(-9) s. Our experimental findings establish that the paramagnetic-to-skyrmion lattice transition in MnSi is well described by the Landau soft-mode mechanism of weak crystallization, originally proposed in the context of the liquid-to-crystal transition. As a key aspect of this theoretical model, the modulation vectors of periodic small-amplitude components of the magnetization form triangles that add to zero. In excellent agreement with our experimental findings, these triangles of the modulation vectors entail the presence of the nontrivial topological winding of skyrmions already in the paramagnetic state of MnSi when approaching the skyrmion lattice transition.

DOI: 10.1103/PhysRevX.9.041059

Ferromagnetic Resonance with Magnetic Phase Selectivity by Means of Resonant Elastic X-Ray Scattering on a Chiral Magnet

S. Pollath, A. Aqeel, A. Bauer, C. Luo, H. Ryll, F. Radu, C. Pfleiderer, G. Woltersdorf, C. H. Back

Physical Review Letters 123 (16), 167201 (2019).

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Cubic chiral magnets, such as Cu2OSeO3, exhibit a variety of noncollinear spin textures, including a trigonal lattice of spin whirls, the so-called skyrmions. Using magnetic resonant elastic x-ray scattering (REXS) on a crystalline Bragg peak and its magnetic satellites while exciting the sample with magnetic fields at gigahertz frequencies, we probe the ferromagnetic resonance (FMR) modes of these spin textures by means of the scattered intensity. Most notably, the three eigenmodes of the skyrmion lattice are detected with large sensitivity. As this novel technique, which we label REXS FMR, is carried out at distinct positions in reciprocal space, it allows us to distinguish contributions originating from different magnetic states, providing information on the precise character, weight, and mode mixing as a prerequisite of tailored excitations for applications.

DOI: 10.1103/PhysRevLett.123.167201

MIEZE Neutron Spin-Echo Spectroscopy of Strongly Correlated Electron Systems

C. Franz, S. Saubert, A. Wendl, F. X. Haslbeck, O. Soltwedel, J. K. Jochum, L. Spitz, J. Kindervater, A. Bauer, P. Boni, C. Pfleiderer

Journal of the Physical Society of Japan 88 (8), 81002 (2019).

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Recent progress in neutron spin-echo spectroscopy by means of longitudinal Modulation of IntEnsity with Zero Effort (MIEZE) is reviewed. Key technical characteristics are summarized which highlight that the parameter range accessible in momentum and energy, as well as its limitations, are extremely well understood and controlled. Typical experimental data comprising quasi-elastic and inelastic scattering are presented, featuring magneto-elastic coupling and crystal field excitations in Ho2Ti2O7, the skyrmion lattice to paramagnetic transition under applied magnetic field in MnSi, ferromagnetic criticality and spin waves in Fe. In addition bench marking studies of the molecular dynamics in H2O are reported. Taken together. the advantages of MIEZE spectroscopy in studies at small and intermediate momentum transfers comprise an exceptionally wide dynamic range of over seven orders of magnitude, the capability to perform straight forward studies on depolarizing samples or under depolarizing sample environments, as well as on incoherently scattering materials.

DOI: 10.7566/jpsj.88.081002

Surface pinning and triggered unwinding of skyrmions in a cubic chiral magnet

P. Milde, E. Neuber, A. Bauer, C. Pfleiderer, L.M. Eng

Physical Review B 100, 24408 (2019).

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In the cubic chiral magnet Fe1−xCoxSi a metastable state comprising topologically nontrivial spin whirls, so-called skyrmions, may be preserved down to low temperatures by means of field cooling the sample. This metastable skyrmion state is energetically separated from the topologically trivial ground state by a considerable potential barrier, a phenomenon also referred to as topological protection. Using magnetic force microscopy on the surface of a bulk crystal, we show that certain positions are preferentially and reproducibly decorated with metastable skyrmions, indicating that surface pinning plays a crucial role. Increasing the magnetic field allows an increasing number of skyrmions to overcome the potential barrier and hence to transform into the ground state. Most notably, we find that the unwinding of individual skyrmions may be triggered by the magnetic tip sample interaction itself, however, only when its magnetization is aligned parallel to the external field. This implies that the stray field of the tip is key for locally overcoming the topological protection. Both the control of the position of topologically nontrivial states and their creation and annihilation on demand pose important challenges in the context of potential skyrmionic applications.

DOI: 10.1103/PhysRevB.100.024408

Putative spin-nematic phase in BaCdVO(PO4)(2)

M. Skoulatos, F. Rucker, G. J. Nilsen, A. Bertin, E. Pomjakushina, J. Olliver, A. Schneidewind, R. Georgii, O. Zaharko, L. Keller, C. Ruegg, C. Pfleiderer, B. Schmidt, N. Shannon, A. Kriele, A. Senyshyn, A. Smerald

Physical Review B 100 (1), 14405 (2019).

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We report neutron-scattering and ac magnetic susceptibility measurements of the two-dimensional spin-1/2 frustrated magnet BaCdVO(PO4)(2). At temperatures well below T-N approximate to 1 K, we show that only 34% of the spin moment orders in an up-up-down-down stripe structure. Dominant magnetic diffuse scattering and comparison to published muon-spin-rotation measurements indicates that the remaining 66% is fluctuating. This demonstrates the presence of strong frustration, associated with competing ferromagnetic and antiferromagnetic interactions, and points to a subtle ordering mechanism driven by magnon interactions. On applying magnetic field, we find that at T = 0.1 K the magnetic order vanishes at 3.8 T, whereas magnetic saturation is reached only above 4.5 T. We argue that the putative high-field phase is a realization of the long-sought bond-spin-nematic state.

DOI: 10.1103/PhysRevB.100.014405

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