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N. B. Christensen

Publications and source records attributed to N. B. Christensen.

At least 19 recordsLinked to original sources

Magnetic and crystal electric field excitations in a spin-orbit coupled frustrated hyperkagome magnet Nd$_3$Li$_3$W$_2$O$_{12}$

Rare-earth based garnets provide a viable platform for studying the frustrated driven magnetic properties of the hyperkagome lattices. Herein, we report a comprehensive study of the magnetic properties and crystal electric field (CEF) scheme of a new Nd$^{3+}$ based hyperkagome antiferromagnet, Nd$_3$Li$_3$W$_2$O$_{12}$ belonging to the garnet family via magnetization, heat capacity, and inelastic neutron scattering (INS) measurements. Magnetization measurement reveals a dominant antiferromagnetic interaction with a low temperature Curie-Weiss temperature $θ_{\rm CW}^{\rm LT} \simeq -0.2$ K. Two broad maxima are observed in the magnetic heat capacity data under magnetic fields, implying multilevel Schottky anomalies due to the effect of CEF and display a two-step magnetic entropy release. No magnetic long-range order is observed down to 0.1 K. The CEF excitations of the Nd$^{3+}$ ($J=9/2$) ion with $D_2$ point group symmetry, probed via INS experiments, show non-dispersive excitations characterizing the transitions among the CEF energy levels. The simultaneous fit of the INS spectra at different temperatures enabled the mapping of the CEF Hamiltonian and the energy eigenvalues of the Kramers' doublets. The simulation using the obtained CEF parameters reproduces the experimental magnetic susceptibility, magnetic isotherms, and magnetic heat capacity data. The thermodynamic properties and INS-derived crystal-field scheme confirm a Kramers' doublet ground state with an effective spin $J_{\rm eff} = 1/2$ at low temperatures.

cond-mat.mtrl-sci

Field-induced quasi-bound state within the two-magnon continuum of a square-lattice Heisenberg antiferromagnet

Quantum magnets in two dimensions display strong quantum interaction effects even when magnetically ordered. Using the metal-organic framework material CuF$_2$(D$_2$O)$_2$(pyz), we investigate the field-dependent spin dynamics of the $S = 1/2$ square-lattice Heisenberg antiferromagnet by high-resolution inelastic neutron scattering to applied fields beyond one third of saturation. We discover an anomalously sharp, dispersive ``shadow mode'' residing within the two-magnon continuum, which shadows the dispersion of the transverse one-magnon branches across the Brillouin zone at an offset equal to the Larmor energy. We perform cylinder matrix-product-state (MPS) calculations that reproduce the field-induced spectrum quantitatively and apply a spectrally consistent $1/S$ spin-wave theory to deduce that the ``Larmor-shadow mode'' is a composite two-magnon resonance: a dispersing magnon at wavevector ${\bf Q}$ couples to the uniform Larmor precession at $Γ$, its small intrinsic linewidth indicating a non-perturbative effect of attractive magnon-magnon interactions. Another quantum-fluctuation phenomenon, the zero-field $(π,0)$ anomaly, is lost at increasing fields, which tighten the spectral weight into the one-magnon and Larmor-shadow modes. To our knowledge, these results constitute the first observation of a sharp quasi-bound state embedded in the continuum of a gapless two-dimensional antiferromagnet.

cond-mat.str-el

Dynamic Competition between Cooper-Pair and Spin-Density-Wave Condensation

Quantum matter phases may co-exist microscopically even when they display competing tendencies. A fundamental question is whether such a competition can be avoided through the elimination of one phase while the other one condenses into the ground state. Here, we present a high-resolution neutron spectroscopy study of the low-energy spin excitations in the high-temperature superconductor La1.855Sr0.145CuO4. In the normal state, we find low-energy magnetic fluctuations at incommensurate reciprocal lattice positions where spin-density-wave order emerges at lower Sr concentration or at high magnetic fields. While these spin excitations are largely suppressed by the emergence of the superconducting spin gap, some low-energy magnetic fluctuations persist deep inside the superconducting state. We interpret this result in terms of a dynamic competition between superconductivity and magnetism, where superconductivity impedes the condensation of low-energy magnetic fluctuations through the formation of magnetically-mediated Cooper pairs.

cond-mat.supr-con

Magnetic and crystal electric field studies in the rare-earth-based square lattice antiferromagnet NdKNaNbO$_5$

The interplay of magnetic correlations, crystal electric field interactions, and spin-orbit coupling in low-dimensional frustrated magnets fosters novel ground states with unusual excitations. Here, we report the magnetic properties and crystal electric field (CEF) scheme of a rare-earth-based square-lattice antiferromagnet NdKNaNbO$_5$ investigated via magnetization, specific heat, electron spin resonance (ESR), and inelastic neutron scattering (INS) experiments. The low-temperature Curie-Weiss temperature $θ_{\rm CW} \simeq -0.6$ K implies net antiferromagnetic interactions between the Nd$^{3+}$ ions. Two broad maxima are observed in the low temperature specific heat data in magnetic fields, indicating multilevel Schottky anomalies due to the effect of CEF. No magnetic long-range-order is detected down to 0.4 K. The CEF excitations of Kramers' ion Nd$^{3+}$ ($J=9/2$) probed via INS experiments evince dispersionless excitations characterizing the transitions among the CEF energy levels. The fit of the INS spectra enabled the mapping of the CEF Hamiltonian and the energy eigenvalues of the Kramers' doublets. The simulation using the obtained CEF parameters reproduces the broad maxima in specific heat in zero-field as well as in different applied fields. The significant contribution from $J_z = \pm 1/2$ state to the wave function of the ground state doublet indicates the role of strong quantum fluctuations at low temperatures. The magnetic ground state is found to be a Kramers' doublet with effective spin $J_{\rm eff} = 1/2$ at low temperatures.

cond-mat.mtrl-sci

Engineering Phase Competition Between Stripe Order and Superconductivity in La$_{1.88}$Sr$_{0.12}$CuO$_4$

Unconventional superconductivity often couples to other electronic orders in a cooperative or competing fashion. Identifying external stimuli that tune between these two limits is of fundamental interest. Here, we show that strain perpendicular to the copper-oxide planes couples directly to the competing interaction between charge stripe order and superconductivity in La$_{1.88}$Sr$_{0.12}$CuO$_4$ (LSCO). Compressive $c$-axis pressure amplifies stripe order within the superconducting state, while having no impact on the normal state. By contrast, strain dramatically diminishes the magnetic field enhancement of stripe order in the superconducting state. These results suggest that $c$-axis strain acts as tuning parameter of the competing interaction between charge stripe order and superconductivity. This interpretation implies a uniaxial pressure-induced ground state in which the competition between charge order and superconductivity is reduced.

cond-mat.str-el

Magnon interactions in a moderately correlated Mott insulator

Quantum fluctuations in low-dimensional systems and near quantum phase transitions have significant influences on material properties. Yet, it is difficult to experimentally gauge the strength and importance of quantum fluctuations. Here we provide a resonant inelastic x-ray scattering study of magnon excitations in Mott insulating cuprates. From the thin film of SrCuO$_2$, single- and bi-magnon dispersions are derived. Using an effective Heisenberg Hamiltonian generated from the Hubbard model, we show that the single-magnon dispersion is only described satisfactorily when including significant quantum corrections stemming from magnon-magnon interactions. Comparative results on La$_2$CuO$_4$ indicate that quantum fluctuations are much stronger in SrCuO$_2$ suggesting closer proximity to a magnetic quantum critical point. Monte Carlo calculations reveal that other magnetic orders may compete with the antiferromagnetic Néel order as the ground state. Our results indicate that SrCuO$_2$ - due to strong quantum fluctuations - is a unique starting point for the exploration of novel magnetic ground states.

cond-mat.str-el

Field-induced electronic phase separation in the high-temperature superconductor La$_{1.94}$Sr$_{0.06}$CuO$_{4+y}$

We present a combined neutron diffraction and high field muon spin rotation ($μ$SR) study of the magnetically ordered and superconducting phases of the high-temperature superconductor La$_{1.94}$Sr$_{0.06}$CuO$_{4+y}$ ($T_{\rm c} = 37.5(2)$~K) in a magnetic field applied perpendicular to the CuO$_2$ planes. We observe a linear field-dependence of the intensity of the neutron diffraction peak that reflects the modulated antiferromagnetic stripe order. The magnetic volume fraction extracted from $μ$SR data likewise increases linearly with applied magnetic field. The combination of these two observations allows us to unambiguously conclude that stripe-ordered regions grow in an applied field, whereas the stripe-ordered magnetic moment itself is field-independent. This contrasts with earlier suggestions that the field-induced neutron diffraction intensity in La-based cuprates is due to an increase in the ordered moment. We discuss a microscopic picture that is capable of reconciling these conflicting viewpoints.

cond-mat.supr-con

Single domain stripe order in a high-temperature superconductor

The coupling of spin, charge and lattice degrees of freedom results in the emergence of novel states of matter across many classes of strongly correlated electron materials. A model example is unconventional superconductivity, which is widely believed to arise from the coupling of electrons via spin excitations. In cuprate high-temperature superconductors, the interplay of charge and spin degrees of freedom is also reflected in a zoo of charge and spin-density wave orders that are intertwined with superconductivity. A key question is whether the different types of density waves merely coexist or are indeed directly coupled. Here we use a novel neutron diffraction technique with superior beam-focusing that allows us to probe the subtle spin-density wave order in the prototypical high-temperature superconductor La1.88Sr0.12CuO4 under applied uniaxial pressure to demonstrate that it is immediately coupled with charge-density wave order. Our result shows that suitable models for high-temperature superconductivity must equally account for charge and spin degrees of freedom via uniaxial charge-spin stripe fluctuations.

cond-mat.str-el

Uniaxial Pressure Induced Stripe Order Rotation in La$_{1.88}$Sr$_{0.12}$CuO$_4$

Static stripe order is detrimental to superconductivity. Yet, it has been proposed that transverse stripe fluctuations may enhance the inter-stripe Josephson coupling and thus promote superconductivity. Direct experimental studies of stripe dynamics, however, remain difficult. From a strong-coupling perspective, transverse stripe fluctuations are realized in the form of dynamic "kinks" -- sideways shifting stripe sections. Here, we show how modest uniaxial pressure tuning reorganizes directional kink alignment. Our starting point is La$_{1.88}$Sr$_{0.12}$CuO$_4$, where transverse kink ordering results in a rotation of stripe order away from the crystal axis. Application of mild uniaxial pressure changes the ordering pattern and pins the stripe order to the crystal axis. This reordering occurs at a much weaker pressure than that to detwin the stripe domains and suggests a rather weak transverse stripe stiffness. Weak spatial stiffness and transverse quantum fluctuations are likely key prerequisites for stripes to coexist with superconductivity.

cond-mat.supr-con

Disentangling Intertwined Quantum States in a Prototypical Cuprate Superconductor

Spontaneous symmetry breaking constitutes a paradigmatic classification scheme of matter. However, broken symmetry also entails domain degeneracy that often impedes identification of novel low symmetry states. In quantum matter, this is additionally complicated by competing intertwined symmetry breaking orders. A prime example is that of unconventional superconductivity and density-wave orders in doped cuprates in which their respective symmetry relation remains a key question. Using uniaxial pressure as a domain-selective stimulus in combination with x-ray diffraction, we unambiguously reveal that the fundamental symmetry of the charge order in the prototypical cuprate La$_{1.88}$Sr$_{0.12}$CuO$_4$ is characterized by uniaxial stripes. We further demonstrate the direct competition of this stripe order with unconventional superconductivity via magnetic field tuning. The stripy nature of the charge-density-wave state established by our study is a prerequisite for the existence of a superconducting pair-density-wave -- a theoretical proposal that clarifies the interrelation of intertwined quantum phases in unconventional superconductors -- and paves the way for its high-temperature realization.

cond-mat.str-el

High-Temperature Charge-Stripe Correlations in La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$

We use resonant inelastic x-ray scattering to investigate charge-stripe correlations in La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$. By differentiating elastic from inelastic scattering, it is demonstrated that charge-stripe correlations precede both the structural low-temperature tetragonal phase and the transport-defined pseudogap onset. The scattering peak amplitude from charge stripes decays approximately as $T^{-2}$ towards our detection limit. The in-plane integrated intensity, however, remains roughly temperature independent. Therefore, although the incommensurability shows a remarkably large increase at high temperature, our results are interpreted via a single scattering constituent. In fact, direct comparison to other stripe-ordered compounds (La$_{1.875}$Ba$_{0.125}$CuO$_4$, La$_{1.475}$Nd$_{0.4}$Sr$_{0.125}$CuO$_4$ and La$_{1.875}$Sr$_{0.125}$CuO$_4$) suggests a roughly constant integrated scattering intensity across all these compounds. Our results therefore provide a unifying picture for the charge-stripe ordering in La-based cuprates. As charge correlations in La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$ extend beyond the low-temperature tetragonal and pseudogap phase, their emergence heralds a spontaneous symmetry breaking in this compound.

cond-mat.supr-con

Spatially Inhomogeneous Competition between Superconductivity and the Charge Density Wave in YBa$_2$Cu$_3$O$_{6.67}$

The charge density wave in the high-temperature superconductor YBa$_2$Cu$_3$O$_{7-x}$ (YBCO) is now known to have two different ordering tendencies differentiated by their $c$-axis correlations. These correspond to ferro- (F-CDW) and antiferro- (AF-CDW) couplings between CDW in neighbouring CuO$_2$ bilayers. This discovery has prompted a number of fundamental questions. For example, how does superconductivity adjust to two competing orders and are either of these orders responsible for the electronic reconstruction? Here we use high-energy x-ray diffraction to study YBa$_2$Cu$_3$O$_{6.67}$ as a function of magnetic field and temperature. We show that regions of the sample with F-CDW correlations suppress superconductivity more strongly than those with AF-CDW correlations. This implies that an inhomogeneous superconducting state exists, in which some regions show a weak or fragile form of superconductivity. By comparison of F-CDW and AF-CDW correlation lengths, it is furthermore concluded that F-CDW ordering is sufficiently long-range to modify the electronic structure. Our study thus suggests that F-CDW correlations have an important impact on superconducting and normal state properties of underdoped YBCO.

cond-mat.supr-con

Temperature dependence of the $(π,0)$ anomaly in the excitation spectrum of the 2D quantum Heisenberg antiferromagnet

It is well established that in the low-temperature limit, the two-dimensional quantum Heisenberg antiferromagnet on a square lattice (2DQHAFSL) exhibits an anomaly in its spectrum at short-wavelengths on the zone-boundary. In the vicinity of the $(π,0)$ point the pole in the one-magnon response exhibits a downward dispersion, is heavily damped and attenuated, giving way to an isotropic continuum of excitations extending to high energies. The origin of the anomaly and the presence of the continuum are of current theoretical interest, with suggestions focused around the idea that the latter evidences the existence of spinons in a two-dimensional system. Here we present the results of neutron inelastic scattering experiments and Quantum Monte Carlo calculations on the metallo-organic compound Cu(DCOO)$_2\cdot 4$D$_2$O (CFTD), an excellent physical realisation of the 2DQHAFSL, designed to investigate how the anomaly at $(π,0)$ evolves up to finite temperatures $T/J\sim2/3$. Our data reveal that on warming the anomaly survives the loss of long-range, three-dimensional order, and is thus a robust feature of the two-dimensional system. With further increase of temperature the zone-boundary response gradually softens and broadens, washing out the $(π,0)$ anomaly. This is confirmed by a comparison of our data with the results of finite-temperature Quantum Monte Carlo simulations where the two are found to be in good accord. At lower energies, in the vicinity of the antiferromagnetic zone centre, there was no significant softening of the magnetic excitations over the range of temperatures investigated.

cond-mat.str-el

Strain-Engineering Mott-Insulating La$_2$CuO$_4$

The transition temperature $T_\textrm{c}$ of unconventional superconductivity is often tunable. For a monolayer of FeSe, for example, the sweet spot is uniquely bound to titanium-oxide substrates. By contrast for La$_{2-\mathrm{x}}$Sr$_\mathrm{x}$CuO$_4$ thin films, such substrates are sub-optimal and the highest $T_\textrm{c}$ is instead obtained using LaSrAlO$_4$. An outstanding challenge is thus to understand the optimal conditions for superconductivity in thin films: which microscopic parameters drive the change in $T_\mathrm{c}$ and how can we tune them? Here we demonstrate, by a combination of x-ray absorption and resonant inelastic x-ray scattering spectroscopy, how the Coulomb and magnetic-exchange interaction of La$_2$CuO$_4$ thin films can be enhanced by compressive strain. Our experiments and theoretical calculations establish that the substrate producing the largest $T_\textrm{c}$ under doping also generates the largest nearest neighbour hopping integral, Coulomb and magnetic-exchange interaction. We hence suggest optimising the parent Mott state as a strategy for enhancing the superconducting transition temperature in cuprates.

cond-mat.str-el

Spin-Orbital Excitations in Ca$_{2}$RuO$_4$ Revealed by Resonant Inelastic X-ray Scattering

The strongly correlated insulator Ca$_{2}$RuO$_4$ is considered as a paradigmatic realization of both spin-orbital physics and a band-Mott insulating phase, characterized by orbitally selective coexistence of a band and a Mott gap. We present a high-resolution oxygen $K$-edge resonant inelastic X-ray scattering study of the antiferromagnetic Mott insulating state of Ca$_{2}$RuO$_4$. A set of low-energy ($\sim$80 and 400 meV) and high-energy ($\sim$1.3 and 2.2 eV) excitations are reported that show strong incident light polarization dependence. Our results strongly support a spin-orbit coupled band-Mott scenario and explore in detail the nature of its exotic excitations. Guided by theoretical modelling, we interpret the low-energy excitations as a result of composite spin-orbital excitations. Their nature unveil the intricate interplay of crystal-field splitting and spin-orbit coupling in the band-Mott scenario. The high-energy excitations correspond to intra-atomic singlet-triplet transitions at an energy scale set by the Hund's coupling. Our findings give a unifying picture of the spin and orbital excitations in the band-Mott insulator Ca$_{2}$RuO$_4$.

cond-mat.str-el

Stability of charge-stripe ordered La2-xSrxNiO4+delta at one third doping

The stability of charge ordered phases is doping dependent, with different materials having particularly stable ordered phases. In the half filled charge ordered phases of the cuprates this occurs at one eighth doping, whereas in charge-stripe ordered La2-xSrxNiO4+delta there is enhanced stability at one third doping. In this paper we discuss the known details of the charge-stripe order in La2-xSrxNiO4+delta, and how these properties lead to the one third doping stability.

cond-mat.str-el

Damped spin excitations in a doped cuprate superconductor with orbital hybridization

A resonant inelastic x-ray scattering (RIXS) study of overdamped spin-excitations in slightly underdoped La$_{2-x}$Sr$_{x}$CuO$_4$ (LSCO) with $x=0.12$ and $0.145$ is presented. Three high-symmetry directions have been investigated: (1) the antinodal $(0,0)\rightarrow (1/2,0)$, (2) the nodal $(0,0)\rightarrow (1/4,1/4)$ and (3) the zone boundary direction $(1/2,0)\rightarrow (1/4,1/4)$ connecting these two. The overdamped excitations exhibit strong dispersions along (1) and (3), whereas a much more modest dispersion is found along (2). This is in strong contrast to the undoped compound La$_{2}$CuO$_4$ (LCO) for which the strongest dispersions are found along (1) and (2). The $t-t^{\prime}-t^{\prime\prime}-U$ Hubbard model used to explain the excitation spectrum of LCO predicts $-$ for constant $U/t$ $-$ that the dispersion along (3) scales with $(t^{\prime}/t)^2$. However, the diagonal hopping $t^{\prime}$ extracted on LSCO using single-band models is low ($t^{\prime}/t\sim-0.16$) and decreasing with doping. We therefore invoked a two-orbital ($d_{x^2-y^2}$ and $d_{z^2}$) model which implies that $t^{\prime}$ is enhanced. This effect acts to enhance the zone-boundary dispersion within the Hubbard model. We thus conclude that hybridization of $d_{x^2-y^2}$ and $d_{z^2}$ states has a significant impact on the zone-boundary dispersion in LSCO.

cond-mat.supr-con

Magnetic field controlled charge density wave coupling in underdoped YBa$_2$Cu$_3$O$_{6+x}$

The application of large magnetic fields ($B \sim B_{c2}$) to layered cuprates suppresses their high temperature superconducting behaviour and reveals competing ground states. In the widely-studied material YBa$_2$Cu$_3$O$_{6+x}$ (YBCO), underdoped ($p \sim 1/8$) samples show signatures of field-induced electronic and structural changes at low temperatures. However, the microscopic nature of the field-induced reconstruction and the high-field state are unclear. Here we report an x-ray study of the high-field charge density wave (CDW) in YBCO, for doping, $0.1 \lesssim p \lesssim 0.13$. For $p \sim 0.123$, we find that a field ($B \sim 10$~T) induces new CDW correlations along the CuO chain ($b$) direction only, leading to a 3-D ordered state along this direction at $B \sim 15$~T. The CDW signal along the $a$-direction is also enhanced by field, but does not develop a new pattern of correlations. We find that field modifies the coupling between the CuO$_2$ bilayers in the YBCO structure, and causes the sudden appearance of 3D CDW order. The mirror symmetry of individual bilayers is broken by the CDW at low and high fields, allowing recently suggested Fermi surface reconstruction.

cond-mat.supr-con