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Martin Greven

Publications and source records attributed to Martin Greven.

At least 19 recordsLinked to original sources

Piezomagnetism in a model cubic noncollinear altermagnet

Altermagnets constitute a distinct class of magnetic materials that combine compensated magnetic order with spin-polarized electronic bands, hence carrying characteristics of both antiferromagnets and ferromagnets. Piezomagnetism - the linear relationship between lattice strain and a net magnetic moment - has emerged as smoking-gun evidence of altermagnetism that distinguishes it from antiferromagnetism. Here, we uncover a large piezomagnetic response in MnTe2, a cubic altermagnet with a noncollinear spin arrangement and weak spin-orbit coupling. We combine dilatometry with nuclear magnetic resonance, a bulk local probe, to observe signatures of both direct and inverse piezomagnetism consistent with symmetry considerations and first-principles calculations. The dilatometry measurements reveal a shear deformation proportional to an applied magnetic field, while magnetic resonance detects a ferromagnetic moment induced by shear strain. The respective results for the piezomagnetic coupling strength are in good agreement, and they are captured by first-principles results. These findings for simple binary MnTe2 position this material as a model altermagnet, demonstrate the utility of nuclear magnetic resonance in investigations of piezomagnetism, and open new avenues for multimodal strain and magnetic-field control in spintronic and memory applications.

cond-mat.mtrl-sci

Vortex pinning of Ba$_{0.62}$K$_{0.38}$BiO$_3$ investigated by magneto-optical Kerr-effect and magnetization measurements

Vortex pinning plays a crucial role in determining properties of type-II superconductors. For example, it governs the irreversible magnetic response as well as dissipation caused by vortex motion. Here, we study vortex pinning in the three-dimensional oxide superconductor Ba1-xKxBiO3 using ultra-high-resolution magneto-optical Kerr effect (MOKE) and detailed magnetization measurements. We find that the zero-field MOKE signal in the superconducting state exhibits a pronounced magnetic-history dependence. This behavior closely resembles the remanent magnetization caused by trapped vortices. Furthermore, we demonstrate that the observed evolution of the MOKE signals is well described by Bean's critical-state model for trapped vortices. Our results establish MOKE as a viable optical and mesoscopic probe of vortex pinning in type-II superconductors, providing a new complementary approach to investigate mixed-state phenomena. We also find that the training-field dependence of the MOKE is linear near zero training field, without any anomalies indicative of spontaneous time-reversal-symmetry breaking in an unconventional superconducting state. Our study defines a clear protocol to distinguish vortex-induced MOKE responses from those associated with a time-reversal-symmetry broken superconducting order parameter.

cond-mat.supr-con

Tuning charge-transport properties and magnetic order in metallic EuTiO$_{3-\delta}$

The stoichiometric antiferromagnetic insulator EuTiO$_3$ is proximate to a ferroelectric phase. Whereas cation substitution has been used as a tuning parameter to introduce charge carriers and manipulate the magnetism, the effects of oxygen-vacancy doping have been less explored. Here we report a detailed study of the charge transport and magnetic properties of metallic, oxygen-vacancy-doped EuTiO$_{3-\delta}$. Using CaH$_2$ as an oxygen getter to achieve a higher carrier concentration than previously reported, we find that the phase diagram of the oxygen-vacancy-doped system is distinct from that obtained via cation doping. In particular, we uncover a change from antiferromagnetic to ferromagnetic order in the metallic state, with a maximum Curie temperature of TC $\approx$ 11 K at the highest carrier concentration of n $\approx$ 10$^{21}$ cm$^{-3}$. These findings are supported by density functional theory calculations, which indicate a significant change in the nearest-neighbor magnetic exchange constant with increasing electron doping. We also present x-ray diffuse scattering and complementary first-principles results that reveal that, similar to the prominent incipient ferroelectric perovskite SrTiO$_3$, the data for EuTiO$_3$ are consistent with thermal diffuse scattering and with the absence of quasi-elastic contributions. Finally, we report specific heat measurements that confirm the magnetic transition temperatures deduced from magnetization measurements and corroborate the lattice dynamics picture inferred from the diffuse scattering data.

cond-mat.mtrl-sci

Ultrafast Two-Dimensional Spectroscopy Uncovers Ubiquitous Electron-Paramagnon Coupling in Cuprate Superconductors

The coupling between electronic excitations and collective bosonic modes is fundamental to the emergence of high-temperature superconductivity in cuprates. Despite extensive effort, conventional equilibrium and pump-probe optical spectroscopies still struggle to disentangle couplings to different bosonic modes when their energy scales overlap. Here we overcome this limitation using ultrafast two-dimensional electronic spectroscopy (2DES), which correlates coherent excitation and detection photon energies with femtosecond time resolution. Applied to optimally doped Bi$_2$Sr$_2$Ca$_{0.92}$Y$_{0.08}$Cu$_2$O$_{8+\delta}$, 2DES reveals a pronounced off-diagonal resonance arising from the ultrafast generation of non-thermal bosons with energy $\hbar\Omega_\mathbf{q}\simeq200$ meV. By comparing the measured spectra with a theoretical framework that explicitly includes the interaction between charge-transfer and magnetic excitations, we identify these bosons as paramagnons with momenta centered near $(\pi/2,\pi/2)$ and extending toward $(0,\pi)$ and $(\pi,0)$. The resonance persists across a large range of temperatures and doping concentrations, demonstrating that high-energy paramagnons are ubiquitously and strongly coupled to electronic excitations throughout the cuprate phase diagram. Time-domain analysis constrains the build-up of the paramagnon population to $\lesssim 10$ fs, placing a lower bound $\lambda \gtrsim 0.7$ on the coupling strength. More broadly, our results establish 2DES as a powerful approach for disentangling mode-selective electron-boson interactions and addressing decoherence dynamics, thereby establishing a new avenue for investigating strongly correlated quantum materials. These findings also provide a direct framework for future time-resolved resonant inelastic X-ray scattering experiments aimed at tracking the ultrafast dynamics of magnetic excitations.

cond-mat.supr-con

Gapped commensurate antiferromagnetic response in a strongly underdoped model cuprate superconductor

It is a distinct possibility that spin fluctuations are the pairing interactions in a wide range of unconventional superconductors. In the case of the high-transition-temperature (high-$T_c$) cuprates, in which superconductivity emerges upon doping an antiferromagnetic Mott-insulating state, spin correlations might furthermore drive unusual pseudogap phenomena. Here we use polarized and unpolarized magnetic neutron scattering to study the simple tetragonal cuprate $\mathrm{HgBa}_{2}\mathrm{CuO}_{4+\delta}$ at very low doping ($T_c \approx 55$ K, hole concentration $p \approx 0.064$). In stark contrast to prior results for other underdoped cuprates, we find no evidence of incommensurate spin-density-wave, charge-spin stripe, or $q = 0$ magnetic order. Instead, the antiferromagnetic response in both the superconducting and pseudogap states is gapped below $\Delta_\mathrm{AF} \approx 6$ meV, commensurate over a wide energy range, and disperses above about 55 meV. Given the documented model nature of $\mathrm{HgBa}_{2}\mathrm{CuO}_{4+\delta}$, which exhibits high structural symmetry and minimal point disorder effects, we conclude that the observed behavior signifies the unmasked response of the quintessential $\mathrm{CuO}_{2}$ planes near the Mott-insulating state. These results for $\mathrm{HgBa}_{2}\mathrm{CuO}_{4+\delta}$ can therefore be expected to serve as a benchmark for a refined theoretical understanding of the cuprates.

cond-mat.supr-con

Diffuse Scattering from Correlated Electron Systems

The role of inhomegeneity in determining the properties of correlated electron systems is poorly understood because of the dearth of structural probes of disorder at the nanoscale. Advances in both neutron and x-ray scattering instrumentation now allow comprehensive measurements of diffuse scattering in single crystals over large volumes of reciprocal space, enabling structural correlations to be characterized over a range of length scales from 10~{\AA} to 200~{\AA} or more. When combined with new analysis tools, such as three-dimensional difference pair-distribution functions, these advanced capabilities have produced novel insights into the interplay of structural fluctuations and electronic properties in a broad range of correlated electron materials. This review describes recent investigations that have demonstrated the importance of understanding structural inhomogeneity pertaining to phenomena as diverse as superconductivity, charge-density-wave modulations, metal-insulator transitions, and multipolar interactions.

cond-mat.str-el

Cu NMR study of lightly doped La$_{2-x}$Sr$_{x}$CuO$_4$

We present a single crystal Cu NMR study of the cuprate superconductor La$_{2-x}$Sr$_{x}$CuO$_4$ with hole doping levels between $x=2$\% and $8$\%. Measurements with short spin echo times enable us to systematically study the local properties of the electronic spin system in the region of the phase diagram where the material evolves from the insulating antiferromagnetic parent phase to the superconducting state. We find evidence for qualitative changes as the Sr concentration increases through $x=5$\% in both NMR spectra and relaxation times, which we interpret as signatures of a low-temperature transition from a state with disconnected metallic islands to a granular metal with tunneling between the grains. These results provide microscopic insight into the physics of a doped charge-transfer insulator in the presence of quenched substitutional disorder, indicate that a connectivity transition occurs, and demonstrate that complex nanoscale electronic phase separation is ubiquitous in LSCO around the doping level where superconductivity first appears in the phase diagram.

cond-mat.supr-con

Structural Properties of Plastically Deformed SrTiO3 and KTaO3

Dislocation engineering has the potential to open new avenues toward the exploration and modification of the properties of quantum materials. Strontium titanate (SrTiO3, STO) and potassium tantalate (KTaO3, KTO) are incipient ferroelectrics that show metallization and superconductivity at extremely low charge carrier concentrations, and have been the subject of resurgent interest. These materials also exhibit remarkable ambient-temperature ductility, and thus represent exceptional platforms for studies of the effects of deformation-induced dislocation structures on electronic properties. Recent work on plastically deformed STO revealed an enhancement of the superconducting transition temperature and the emergence of local ferroelectricity and magnetism near self-organized dislocation walls. Here we present a comprehensive structural analysis of plastically deformed STO and KTO, employing specially designed strain cells, diffuse neutron and x-ray scattering, Raman scattering, and nuclear magnetic resonance (NMR). Diffuse scattering and NMR provide insight into the dislocation configurations and densities and their dependence on strain. As in the prior work on STO, Raman scattering reveals evidence for local ferroelectric order near dislocation walls in plastically deformed KTO. Our findings provide valuable information about the self-organized defect structures in both materials, and they position KTO as a second model system with which to explore the associated emergent physics.

cond-mat.mtrl-sci

Nanoscale structural correlations in a model cuprate superconductor

Understanding the extent and role of inhomogeneity is a pivotal challenge in the physics of cuprate superconductors. While it is known that structural and electronic inhomogeneity is prevalent in the cuprates, it has proven difficult to disentangle compound-specific features from universally relevant effects. Here we combine advanced neutron and x-ray diffuse scattering with numerical modeling to obtain insight into bulk structural correlations in HgBa$_2$CuO$_{4+\delta}$. This cuprate exhibits a high optimal transition temperature of nearly 100 K, pristine charge-transport behavior, and a simple average crystal structure without long-range structural instabilities, and is therefore uniquely suited for investigations of intrinsic inhomogeneity. We uncover diffuse reciprocal-space patterns that correspond to prominent nanoscale correlations of atomic displacements perpendicular to the CuO$_2$ planes. The real-space nature of the correlations is revealed through three-dimensional pair distribution function analysis and complementary numerical refinement. We find that relative displacements of ionic and CuO$_2$ layers play a crucial role, and that the structural inhomogeneity is not directly caused by the presence of conventional point defects. The observed correlations are therefore intrinsic to HgBa$_2$CuO$_{4+\delta}$, and thus likely important for the physics of cuprates more broadly. It is possible that the structural correlations are closely related to the unusual superconducting correlations and Mott-localization in these complex oxides. As advances in scattering techniques yield increasingly comprehensive data, the experimental and analysis tools developed here for large volumes of diffuse scattering data can be expected to aid future investigations of a wide range of materials.

cond-mat.supr-con

Optically Probing Unconventional Superconductivity in Atomically Thin Bi$_2$Sr$_2$Ca$_{0.92}$Y$_{0.08}$Cu$_2$O$_{8+{\delta}}$

Atomically thin cuprates exhibiting a superconducting phase transition temperature similar to bulk have recently been realized, although the device fabrication remains a challenge and limits the potential for many novel studies and applications. Here we use an optical pump-probe approach to noninvasively study the unconventional superconductivity in atomically thin Bi$_2$Sr$_2$Ca$_{0.92}$Y$_{0.08}$Cu$_2$O$_{8+{\delta}}$ (Y-Bi2212). Apart from finding an optical response due to the superconducting phase transition that is similar to bulk Y-Bi2212, we observe that the sign and amplitude of the pump-probe signal in the atomically thin flake vary significantly in different dielectric environments depending on the nature of the optical excitation. By exploiting the spatial resolution of the optical probe, we uncover the exceptional sensitivity of monolayer Y-Bi2212 to the environment. Our results provide the first optical evidence for the intralayer nature of the superconducting condensate in Bi2212, and highlight the role of double-sided encapsulation in preserving superconductivity in atomically thin cuprates.

cond-mat.mes-hall

Dynamics of non-thermal states in optimally-doped $Bi_2Sr_2Ca_{0.92}Y_{0.08}Cu_2O_{8+{\delta}}$ revealed by mid-infrared three-pulse spectroscopy

In the cuprates, the opening of a d-wave superconducting (SC) gap is accompanied by a redistribution of spectral weight at energies two orders of magnitude larger than this gap. This indicates the importance to the pairing mechanism of on-site electronic excitations, such as orbital transitions or charge transfer excitations. Here, we resort to a three-pulse pump-probe scheme to study the broadband non-equilibrium dielectric function in optimally-doped $Bi_2Sr_2Ca_{0.92}Y_{0.08}Cu_2O_{8+{\delta}}$ and we identify two distinct dynamical responses: i) a blueshift of the central energy of an interband excitation peaked at 2 eV and ii) a change in spectral weight in the same energy range. Photoexcitation with near-IR and mid-IR pulses, with photon energies respectively above and below the SC gap, reveals that the transient changes in the central energy are not modified by the onset of superconductivity and do not depend on the pump photon energy. Conversely, the spectral weight dynamics strongly depends on the pump photon energy and has a discontinuity at the critical temperature. The picture that emerges is that, while high-energy pulses excite quasiparticles in both nodal and thermally inaccessible antinodal states, photoexcitation by low-energy pulses mostly accelerates the condensate and creates excitations predominantly at the nodes of the SC gap. These results, rationalized by kinetic equations for d-wave superconducting gaps, indicate that dynamical control of the momentum-dependent distribution of non-thermal quasiparticles may be achieved by the selective tuning of the photoexcitation.

cond-mat.supr-con

Direct observation of the Higgs particle in a superconductor by non-equilibrium Raman scattering

Even before its role in electroweak symmetry breaking, the Anderson-Higgs mechanism was introduced to explain the Meissner effect in superconductors. Spontaneous symmetry-breaking yields massless phase modes representing the low-energy excitations of the Mexican-Hat potential. Only in superconductors the phase mode is shifted towards higher energies owing to the gauge field of the charged condensate. This results in a low-energy excitation spectrum governed by the Higgs mode. Consequently, the Meissner effect signifies a macroscopic quantum condensate in which a photon acquires mass, representing a one-to-one analogy to high-energy physics. We report on the direct observation of the Higgs particle in the high-temperature superconductor Bi-2212 by developing an innovative technique to study its symmetries and energies after a "soft quench" of the Mexican-Hat potential. Population inversion of the metastable Higgs particle induced by an initial laser pulse allows identifying the polarization-dependent Higgs modes as an additional anti-Stokes Raman-scattering signal. Within Ginzburg-Landau theory, the Higgs-mode energy is connected to the Cooper-pair coherence length. Within a BCS weak-coupling model we develop a quantitative and coherent description of single-particle and two-particle channels. This opens the avenue for Higgs Spectroscopy in quantum condensates and provides a unique pathway to control and explore Higgs physics.

cond-mat.supr-con

Multiferroicity in plastically deformed SrTiO$_3$

A major challenge in the development of quantum technologies is to induce additional types of ferroic orders into materials that exhibit other useful quantum properties. Various techniques have been applied to this end, such as elastically straining, doping, or interfacing a compound with other materials. Plastic deformation introduces permanent topological defects and large local strains into a material, which can give rise to qualitatively new functionality. Here we show via local magnetic imaging that plastic deformation induces robust magnetism in the quantum paraelectric SrTiO3, in both conducting and insulating samples. Our analysis indicates that the magnetic order is localized along dislocation walls and coexists with polar order along the walls. The magnetic signals can be switched on and off in a controllable manner with external stress, which demonstrates that plastically deformed SrTiO3 is a quantum multiferroic. These results establish plastic deformation as a versatile platform for quantum materials engineering.

cond-mat.str-el

Structural changes induced by electric currents in a single crystal of Pr$_2$CuO$_4$

We demonstrate a novel approach to the structural and electronic property modification of perovskites, focusing on Pr$_2$CuO$_4$, an undoped parent compound of a class of electron-doped copper-oxide superconductors. Currents were passed parallel or perpendicular to the copper-oxygen layers with the voltage ramped up until a rapid drop in the resistivity was achieved, a process referred to as "flash". The current was then further increased tenfold in current-control mode. This state was quenched by immersion into liquid nitrogen. Flash can drive many compounds into different atomic structures with new properties, whereas the quench freezes them into a long-lived state. Single-crystal neutron diffraction of as-grown and modified Pr$_2$CuO$_4$ revealed a $\sqrt{10}$x$\sqrt{10}$ superlattice due to oxygen-vacancy order. The diffraction peak intensities of the superlattice of the modified sample were significantly enhanced relative to the pristine sample. Raman-active phonons in the modified sample were considerably sharper. Measurements of electrical resistivity, magnetization and two-magnon Raman scattering indicate that the modification affected only the Pr-O layers, but not the Cu-O planes. These results point to enhanced oxygen-vacancy order in the modified samples well beyond what can be achieved without passing electrical current. Our work opens a new avenue toward electric field/quench control of structure and properties of layered perovskite oxides.

cond-mat.supr-con

Magnetic resonance study of rare-earth titanates

We present a nuclear magnetic resonance (NMR) and electron spin resonance (ESR) study of rare-earth titanates derived from the spin-1/2 Mott insulator YTiO$_3$. Measurements of single-crystalline samples of (Y,Ca,La)TiO$_3$ in a wide range of isovalent substitution (La) and hole doping (Ca) reveal several unusual features in the paramagnetic state of these materials. $^{89}$Y NMR demonstrates a clear discrepancy between the static and dynamic local magnetic susceptibilities, with deviations from Curie-Weiss behavior far above the Curie temperature $T_C$. No significant changes are observed close to $T_C$, but a suppression of fluctuations is detected in the NMR spin-lattice relaxation time at temperatures of about $3\times T_C$. Additionally, the nuclear spin-spin relaxation rate shows an unusual peak in dependence on temperature for all samples. ESR of the unpaired Ti electron shows broad resonance lines at all temperatures and substitution/doping levels, which we find to be caused by short electronic spin-lattice relaxation times. We model the relaxation as an Orbach process that involves a low-lying electronic excited state, which enables the determination of the excited-state gap from the temperature dependence of the ESR linewidths. We ascribe the small gap to Jahn-Teller splitting of the two lower Ti $t_{2g}$ orbitals. The value of the gap closely follows $T_C$ and is consistent with the temperatures at which deviations from Curie-Weiss fluctuations are observed in NMR. These results provide insight into the interplay between orbital and spin degrees of freedom in rare-earth titanates and indicate that full orbital degeneracy lifting is associated with ferromagnetic order.

cond-mat.str-el

Electrochemically-driven insulator-metal transition in ionic-liquid-gated antiferromagnetic Mott-insulating NiS$_2$ single crystals

Motivated by the existence of superconductivity in pyrite-structure CuS$_2$, we explore the possibility of ionic-liquid-gating-induced superconductivity in the proximal antiferromagnetic Mott insulator NiS$_2$. A clear gating-induced transition from a two-dimensional insulating state to a three-dimensional metallic state is observed at positive gate bias on single crystal surfaces. No evidence for superconductivity is observed down to the lowest measured temperature of 0.45 K, however. Based on transport, energy-dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, atomic force microscopy, and other techniques, we deduce an electrochemical gating mechanism involving a substantial decrease in the S:Ni ratio (over hundreds of nm), which is both non-volatile and irreversible. This is in striking contrast to the reversible, volatile, surface-limited, electrostatic gate effect in pyrite FeS$_2$. We attribute this stark difference in electrochemical vs. electrostatic gating response in NiS$_2$ and FeS$_2$ to the much larger S diffusion coefficient in NiS$_2$, analogous to the different behaviors observed among electrolyte-gated oxides with differing O-vacancy diffusivities. The gating irreversibility, on the other hand, is associated with the lack of atmospheric S; this is in contrast to the better understood oxide case, where electrolysis of atmospheric H$_2$O provides an O reservoir. This study of NiS$_2$ thus provides new insight into electrolyte gating mechanisms in functional materials, in a previously unexplored limit.

cond-mat.mtrl-sci

Uniaxial strain control of bulk ferromagnetism in rare-earth titanates

The perovskite rare-earth titanates are model Mott insulators with magnetic ground states that are very sensitive to structural distortions. These distortions couple strongly to the orbital degrees of freedom and, in principle, it should be possible to tune the superexchange and the magnetic transition with strain. We investigate the representative system (Y,La,Ca)TiO$_3$, which exhibits low crystallographic symmetry and no structural instabilities. From magnetic susceptibility measurements of the Curie temperature, we demonstrate direct, reversible and continuous control of ferromagnetism by influencing the TiO$_6$ octahedral tilts and rotations with uniaxial strain. The relative change in $T_C$ as a function of strain is well described by ab initio calculations, which provides detailed understanding of the complex interactions among structural, orbital and magnetic properties in rare-earth titanates. The demonstrated manipulation of octahedral distortions opens up far-reaching possibilities for investigations of electron-lattice coupling, competing ground states, and magnetic quantum phase transitions in a wide range of quantum materials.

cond-mat.str-el

Phenomenological model for the third-harmonic magnetic response of superconductors: application to Sr$_{2}$RuO$_{4}$

We employ the phenomenological Lawrence-Doniach model to compute the contributions of the superconducting fluctuations to the third-harmonic magnetic response, denoted here by $\overline{M_{3}}$, which can be measured in a precise way using ac magnetic fields and lock-in techniques. We show that, in an intermediate temperature regime, this quantity behaves as the third-order nonlinear susceptibility, which shows a power-law dependence with the reduced temperature $\epsilon=\frac{T-T_{c}}{T_{c}}$ as $\epsilon^{-5/2}$. Very close to $T_{c}$, however, $\overline{M_{3}}$ saturates due to the nonzero amplitude of the ac field. We compare our theoretical results with experimental data for three conventional superconductors -- lead, niobium, and vanadium -- and for the unconventional superconductor Sr$_{2}$RuO$_{4}$ (SRO). We find good agreement between theory and experiment for the elemental superconductors, although the theoretical values for the critical field systematically deviate from the experimental ones. In the case of SRO, however, the phenomenological model completely fails to describe the data, as the third-harmonic response remains sizable over a much wider reduced temperature range compared to Pb, Nb, and V. We show that an inhomogeneous distribution of $T_{c}$ can partially account for this discrepancy, since regions with a locally higher $T_{c}$ contribute to the fluctuation $\overline{M_{3}}$ significantly more than regions with the "nominal" $T_{c}$ of the clean system. However, the exponential temperature dependence of $\overline{M_{3}}$ first reported in Ref. [3] is not captured by the model with inhomogeneity. We conclude that, while inhomogeneity is an important ingredient to understand the superconducting fluctuations of SRO and other perovskite superconductors, additional effects may be at play, such as non-Gaussian fluctuations or rare-region effects.

cond-mat.supr-con