SearcharxivSearch

arXiv subjects

Paul Steffens

Publications and source records attributed to Paul Steffens.

At least 19 recordsLinked to original sources

Ultralow-Field Triplon Condensation in a Spin-Ladder Magnet

We realise the first ultralow-field Bose-Einstein condensation of triplons in a spin-ladder magnet, uncovering a quantum critical point at only $\mu_0 H_{c1}=0.17$ T in Henmilite ($\mathrm{Ca_2Cu(OH)_4[B(OH)_4]_2}$). Unlike dimer magnets, a ladder retains extended one-dimensional correlations in its gapped parent state, making this limit strongly fluctuation dominated. Thermodynamic, magnetoelastic, $\mu$SR, and neutron-diffraction measurements overturn the previous assignment of zero-field antiferromagnetic order, establishing a quantum-disordered coupled-ladder parent state with persistent low-energy dynamics. The weak low-temperature anomaly instead marks a gap-controlled crossover from the correlated ladder regime into the activated quantum-disordered state. These measurements further reveal an exceptionally asymmetric ordered dome extending to $\mu_0 H_{c2}\simeq 8.2$ T. Quantum Monte Carlo simulations for the relevant spin Hamiltonian place Henmilite just on the gapped side of the zero-field ladder-ordering instability, naturally accounting for the strong separation between the exchange and residual-gap scales and the tiny critical field. Our findings extend ultralow-field triplon condensation beyond the dimer paradigm and establish Henmilite as a platform for controlled tuning across quantum criticality in a fluctuation-dominated spin ladder.

cond-mat.str-el

Tilted and Twisted Magnetic Moments in the Kitaev Magnet $\alpha$-RuCl$_3$

The layered honeycomb magnet $\alpha$-RuCl$_3$ has attracted intense scrutiny as a prime candidate for realizing the Kitaev quantum spin liquid, yet a consensus on its microscopic Hamiltonian remains elusive due to the material's extreme sensitivity to structural details. Here, we report a comprehensive reexamination of the low-temperature crystallographic and magnetic structures of high-quality $\alpha$-RuCl$_3$ single crystals using unpolarized and polarized neutron diffraction. We confirm a sharp, first-order structural phase transition to the rhombohedral $R\bar{3}$ space group with a pronounced thermal hysteresis. Crucially, using both spherical and longitudinal neutron polarization analysis, we determine the 3D orientation of the ordered magnetic moment without the ambiguity typically arising from domain distributions. We find that the Ru$^{3+}$ magnetic moments in the zigzag phase are tilted by $15.7^\circ$ out of the hexagonal plane and, remarkably, exhibit an additional in-plane twist of $-13.8^\circ$. This "tilted and twisted" geometry differentiates the ground state from the previously reported models based on unpolarized neutron diffraction or resonant elastic X-ray scattering (REXS) analysis.

cond-mat.str-el

Magnetic excitations in the Kitaev material Na$_2$IrO$_3$ studied by neutron scattering

Inelastic neutron scattering experiments with a large set of comounted Na$_2$IrO$_3$ crystals reveal the low-energy magnon dispersion in this candidate material for Kitaev physics. The magnon gap amounts to 1.7(1) meV and can be interpreted similarly to the sister compound $\alpha$-RuCl$_{3}$ to stem from the zone boundaries in the antiferromagnetic zigzag structure. The neutron experiments find no evidence for low-energy excitations with ferromagnetic character, which contrasts to the findings in $\alpha$-RuCl$_{3}$. Our results are consistent with a recently proposed microscopic model that involves an antiferromagnetic Heisenberg nearest-neighbor exchange in Na$_2$IrO$_3$ in contrast to the ferromagnetic one considered for $\alpha$-RuCl$_{3}$. Although the magnetic response shows the signatures of bond-directional anisotropy in both materials the different relative signs of Kitaev and Heisenberg interaction result in different deviations from the initial Kitaev model. Low-energy ferromagnetic fluctuations cannot be considered as a fingerprint of ferromagnetic Kitaev interaction.

cond-mat.str-el

Incipient modulated phase in Sr$_{1-x}$Ca$_{x}$TiO$_3$

Nanometer-scale modulations can spontaneously emerge in complex materials when multiple degrees of freedom interact. Here we demonstrate that ferroelectric Sr$_{1-x}$Ca$_x$TiO$_3$ lies in close proximity to an incipient structurally modulated phase. Using inelastic neutron and X-ray scattering, we show that upon cooling, dipolar fluctuations strongly couple to and soften the $c_{44}$ transverse acoustic mode. We identify the wavevector at which this softening is maximal, thereby defining the characteristic length scale of the modulation. Calcium substitution enhances both the amplitude and the wavevector of the softening by strengthening the ferroelectric and antiferrodistortive instabilities. Our results demonstrate that nonlinear flexoelectric phonon coupling tends to stabilize a modulated state that cooperates with, rather than competes against, the other lattice instabilities in SrTiO$_3$.

cond-mat.mtrl-sci

Single-$q$ Cycloid and Double-$q$ Vortex Lattices in Layered Magnetic Semimetal EuAg$_4$Sb$_2$

Recently, a host of exotic magnetic textures such as topologically protected skyrmion lattices has been discovered in several bulk metallic lanthanide compounds. In addition to hosting skyrmion phases, a hallmark of this class of materials is the appearance of numerous spin textures characterized by a superposition of multi-$q$ magnetic modulations: spin moir\'{e} superlattices. The nuanced energy landscape thus motivates detailed studies to understand the underlying interactions. Here, we comprehensively characterize and model the three zero-field magnetic textures present in one such material, EuAg$_4$Sb$_2$. Systematic symmetry breaking experiments using magnetic field and strain determine that the ground state incommensurate magnetic phase (ICM1) is single-$q$. In contrast, ICM2 and ICM3 are both double-$q$, \textit{i.e.}, spin moir\'{e} superlattices. Further, through application of polarized small angle neutron scattering and spherical neutron polarimetry, we demonstrate that ICM1 is a single-$q$ cycloid and ICM2 and ICM3 are double-$q$ vortex lattices, with Eu moments lying in the $ab$-plane in zero field and with a ferromagnetic component at finite field. Despite the quasi-2D nature of EuAg$_4$Sb$_2$, the modulations propagate out of the \textit{ab}-plane, leading to a shift of the spin texture between triangle lattice planes. Further, the ICM3 to ICM2 transition includes an unusual 45$^\circ$ rotation of the magnetic vortex lattice. Motivated by the coexistence of such drastically different phases in this compound, we conclude by developing a phenomenological model to understand the stability of these states. Our experimental probes and theoretical modeling definitively characterize three different and tunable phases in one material, and provide insight for the design of new topological spin-texture materials.

cond-mat.mes-hall

Non-Reciprocal Zone Boundary Magnon Propagation in Cu$_2$OSeO$_3$

Inelastic neutron scattering in the chiral magnet Cu$_2$OSeO$_3$ reveals strong non-reciprocal effects on magnon propagation at the boundary of the nuclear Brillouin zone. The non-reciprocal response is strongest at a central position between the zone corner and edge mid-point. We explain these results using an effective linear spin-wave model. While directional effects in chiral magnets have so far only been known to exist at low momenta close to the center of the Brillouin zone, the present study shows that non-reciprocity persists at the highest possible reduced momenta. The observed magnons show very little damping within the limits of our experimental resolution, making them of great interest for the fundamental research on compact, high-frequency magnonic applications.

cond-mat.str-el

Zeeman Ladders in Frustrated XYZ Spin Chains

We investigate the nature of the excitations captured by the dynamical response of XYZ triangular spin-1/2 ladders. We complement experimental inelastic neutron scattering results on the compound $\text{Cs}_\text{2}\text{CoBr}_\text{4}$ with numerically exact simulations based on time-dependent matrix product state methods. Our results show that bound states of spinon excitations can arise in XYZ beyond the requirement of strong Ising anisotropies. We analyze the role of the frustrated triangular couplings on the excitations giving rise to the spin dynamical structure factor and show how the features of the bound states manifest themselves in the different polarization channels.

cond-mat.str-el

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

Spin excitations arising from anisotropic Dirac spinons in YCu$_3$(OD)$_6$Br$_2$[Br$_{0.33}$(OD)$_{0.67}$]

A Dirac quantum spin liquid hosts Dirac spinons, which are low-energy fractionalized neutral quasiparticles with spin 1/2 that obey the Dirac equation. Recent inelastic neutron scattering studies have revealed a cone spin continuum in YCu$_3$(OD)$_6$Br$_2$[Br$_{x}$(OD)$_{1-x}$], consistent with the convolution of two Dirac spinons. In this work, we further studied spin excitations using the inelastic neutron scattering technique. The width of low-energy spin excitations shows a linear temperature dependence, which can be explained by spinon-spinon interactions with a Dirac dispersion. Polarized neutron scattering measurements reveal that in-plane magnetic fluctuations are about 1.5 times stronger than the out-of-plane ones, suggesting the presence of Dzyaloshinskii-Moriya interaction and consistent with our theoretical modeling and simulations. Moreover, the high-energy spin excitations around 14 meV agree with the one-pair spinon-antispinon excitations in Raman studies. The real part of the dynamical susceptibility derived from the Kramers-Kronig relationship also agrees with the Knight shift measured by nuclear magnetic resonance, clearly demonstrating the negligible effects of magnetic impurities on static susceptibility. These results provide a rare example in studying quantum-spin-liquid materials where different experimental techniques can be directly compared, and they give further insights for the possible Dirac quantum spin liquid in this system.

cond-mat.str-el

Direct evidence for anisotropic magnetic interaction in $\alpha$-RuCl$_3$ from polarized inelastic neutron scattering

Polarized neutron scattering experiments reveal the anisotropy of magnetic correlations in the candidate Kitaev material $\alpha$-RuCl$_3$. The anisotropy of the inelastic response at the magnetic Bragg positions is just opposite to the expectation for a simple Heisenberg model. Near the antiferromagnetic $q$ vector, there are no low-energy transversal magnon modes directly documenting the fully anisotropic and bond-directional character of the magnetic interaction in $\alpha$-RuCl$_3$. However, other findings disagree with a simple or strongly dominant Kitaev component.

cond-mat.str-el

Emergent photons and fractionalized excitations in a quantum spin liquid

A quantum spin liquid (QSL) arises from a highly entangled superposition of many degenerate classical ground states in a frustrated magnet, and is characterized by emergent gauge fields and deconfined fractionalized excitations (spinons). Because such a novel phase of matter is relevant to high-transition-temperature superconductivity and quantum computation, the microscopic understanding of QSL states is a long-sought goal in condensed matter physics. The 3D pyrochlore lattice of corner-sharing tetrahedra can host a QSL with U(1) gauge fields called quantum spin ice (QSI), which is a quantum (with effective $S=1/2$) analog of the classical (with large effective moment) spin ice. A key difference between QSI and classical spin ice is the predicted presence of the linearly dispersing collective excitations near zero energy, dubbed the "photons", arising from emergent quantum electrodynamics, in addition to the spinons at higher energies. Recently, 3D pyrochlore systems Ce2M2O7 (M = Sn, Zr, Hf) have been suggested as effective $S=1/2$ QSI candidates, but there has been no evidence of quasielastic magnetic scattering signals from photons, a key signature for a QSI. Here, we use polarized neutron scattering experiments on single crystals of Ce2Zr2O7 to conclusively demonstrate the presence of magnetic excitations near zero energy at 50 mK in addition to signatures of spinons at higher energies. By comparing the energy (E), wave vector (Q), and polarization dependence of the magnetic excitations with theoretical calculations, we conclude that Ce2Zr2O7 is the first example of a dipolar-octupolar $\pi$ flux QSI with dominant dipolar Ising interactions, therefore identifying a microscopic Hamiltonian responsible for a QSL.

cond-mat.str-el

Quantum Fisher information in a strange metal

A strange metal is an exotic state of correlated quantum matter; intensive efforts are ongoing to decipher its nature. Here we explore whether the quantum Fisher information (QFI), a concept from quantum metrology, can provide new insight. We use inelastic neutron scattering and quantum Monte Carlo simulations to study a Kondo destruction quantum critical point, where strange metallicity is associated with fluctuations beyond a Landau order parameter. We find that the QFI probed away from magnetic Bragg peaks, where the effect of magnetic ordering is minimized, increases strongly and without a characteristic scale as the strange metal forms with decreasing temperature, evidencing its unusual entanglement properties. Our work opens a new direction for studies across strange metal platforms.

cond-mat.str-el

Exchange renormalized crystal field excitation in a quantum Ising magnet KTmSe$_2$

Rare-earth delafossite compounds, ARCh$_2$ (A = alkali or monovalent ion, R = rare earth, Ch = chalcogen), have been proposed for a range of novel quantum phenomena. Particularly, the Tm series, ATmCh$_2$, featuring Tm ions on a triangular lattice, serves as a representative group of compounds to illustrate the interplay and competition between spin-orbit coupling, crystal fields, and exchange couplings in the presence of geometric frustration. Here we report the thermodynamic and inelastic neutron scattering studies on the newly discovered triangular-lattice magnet KTmSe$_2$. Both heat capacity and neutron diffraction reveal the absence of long-range magnetic order. Magnetic susceptibility shows strong Ising-like interactions with antiferromagnetic correlations. Furthermore, inelastic neutron scattering measurements reveal a branch of dispersive crystal field excitations. To analyze these observations, we employ both the transverse field Ising model and the full crystal field scheme, along with exchange interactions. Our results suggest a strong competition between spin exchange interactions and crystal field effects. This work is expected to offer a valuable framework for understanding low-temperature magnetism in KTmSe$_2$ and similar materials.

cond-mat.str-el

Universality of the {\bf q}=1/2 Orbital Magnetism in the Pseudogap Phase of the High-$T_c$ superconductor $\rm YBa_{2}Cu_{3}O_{6+x}$

Several decades of debate have centered around the nature of the enigmatic pseudo-gap state in high temperature superconducting copper oxides. Recently, we reported polarized neutron diffraction measurements that suggested the existence of a magnetic texture bound to the pseudo-gap phase [Bounoua, {\it et al}. Communications Physics 5, 268 (2022)]. Such a magnetic texture is likely to involve the spontaneous appearance of loop currents within the CuO$_2$ unit cells, which give birth to complex correlated patterns. In the underdoped ${\rm YBa_{2}Cu_{3}O_{6.6}}$, the magnetic structure factor of such an orbital magnetic texture gives rise to two distinct magnetic responses at {\bf q}=0 and {\bf q}=1/2. As this pattern alters the lattice translation invariance, such a state of matter could contribute to an instability of the Fermi surface. Here, we report polarized neutron scattering measurements on a nearly optimally doped high quality single crystal of ${\rm YBa_{2}Cu_{3}O_{6.9}}$ that exhibits the same {\bf q}=1/2 magnetism and a weakly overdoped ${\rm YBa_{2}Cu_{3}O_{7}}$ sample where this signal is no longer sizeable. The in-plane and out-of-plane magnetic neutron scattering intensities in ${\rm YBa_{2}Cu_{3}O_{6.9}}$ (at {\bf q}=1/2) and ${\rm YBa_{2}Cu_{3}O_{6.85}}$ (at {\bf q}=0), reported previously, display the same temperature dependent hallmarks. The magnitudes of both {\bf q}=0 and {\bf q}=1/2 magnetic signals further exhibit the same trends upon doping in ${\rm YBa_{2}Cu_{3}O_{6+x}}$, confirming that they are likely intertwined.

cond-mat.str-el

Gradual emergence of superconductivity in underdoped LSCO

We present triple-axis neutron scattering studies of low-energy magnetic fluctuations in strongly underdoped La$_{2-x}$Sr$_{x}$CuO$_{4}$ with $x=0.05$, $0.06$ and $0.07$, providing quantitative evidence for a direct competition between these fluctuations and superconductivity. At dopings $x=0.06$ and $x=0.07$, three-dimensional superconductivity is found, while only a very weak signature of two-dimensional superconductivity residing in the CuO$_2$ planes is detectable for $x=0.05$. We find a surprising suppression of the low-energy fluctuations by an external magnetic field at all three dopings. This implies that the response of two-dimensional superconductivity to a magnetic field is similar to that of a bulk superconductor. Our results provide direct evidence of a very gradual onset of superconductivity in cuprates.

cond-mat.supr-con

Hidden Magnetic Texture in the Pseudogap Phase of High-Tc $YBa_{2}Cu_{3}O_{6.6}$

Despite decades of intense researches, the enigmatic pseudo-gap (PG) phase of superconducting cuprates remains an unsolved mystery. In the last 15 years, various symmetry breakings in the PG state have been discovered, spanning an intra-unit cell (IUC) magnetism, preserving the lattice translational (LT) symmetry but breaking time-reversal symmetry and parity, and an additional incipient charge density wave breaking the LT symmetry upon cooling. However, none of these states can (alone) account for the partial gapping of the Fermi surface. Here we report a hidden LT-breaking magnetism uisng polarized neutron diffraction. Our measurements reveal magnetic correlations, in two different underdoped $\rm YBa_{2}Cu_{3}O_{6.6}$ single crystals, that settle at the PG onset temperature with i) a planar propagation wave vector $(π,0) \equiv (0,π)$, yielding a doubling or quadrupling of the magnetic unit cell and ii) magnetic moments mainly pointing perpendicular to the $CuO_{2}$ layers. The LT-breaking magnetism is at short range suggesting the formation of clusters of 5-6 unit cells. Together with the previously reported IUC magnetism, it yields a hidden magnetic texture of the $CuO_{2}$ unit cells hosting loop currents, forming large supercells which may be crucial for elucidating the PG puzzle.

cond-mat.supr-con

Mesoscopic tunneling in strontium titanate

Spatial correlation between atoms can generate a depletion in the energy dispersion of acoustic phonons. Two well known examples are rotons in superfluid helium and the Kohn anomaly in metals. Here we report on the observation of a large softening of the transverse acoustic mode in quantum paraelectric SrTiO$_3$ by means of inelastic neutron scattering. In contrast to other known cases, this softening occurs at a tiny wave vector implying spatial correlation extending over a distance as long as 40 lattice parameters. We attribute this to the formation of mesoscopic fluctuating domains due to the coupling between local strain and quantum ferroelectric fluctuations. Thus, a hallmark of the ground state of insulating SrTiO$_3$ is the emergence of hybridized optical-acoustic phonons. Mesoscopic fluctuating domains play a role in quantum tunneling, which impedes the emergence of a finite macroscopic polarisation.

cond-mat.mtrl-sci

Field-Tuned Quantum Effects in a Triangular-Lattice Ising Magnet

We report thermodynamic and neutron scattering measurements of the triangular-lattice quantum Ising magnet TmMgGaO 4 in longitudinal magnetic fields. Our experiments reveal a quasi-plateau state induced by quantum fluctuations. This state exhibits an unconventional non-monotonic field and temperature dependence of the magnetic order and excitation gap. In the high field regime where the quantum fluctuations are largely suppressed, we observed a disordered state with coherent magnon-like excitations despite the suppression of the spin excitation intensity. Through detailed semi-classical calculations, we are able to understand these behaviors quantitatively from the subtle competition between quantum fluctuations and frustrated Ising interactions.

cond-mat.str-el