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J. van den Brink

Publications and source records attributed to J. van den Brink.

At least 55 records · Page 3Linked to original sources

Tuning Magnetic Coupling in Sr$_2$IrO$_4$ Thin Films with Epitaxial Strain

We report x-ray resonant magnetic scattering (XRMS) and resonant inelastic x-ray scattering (RIXS) studies of epitaxially-strained $\mathrm{Sr_2IrO_4}$ thin films. The films were grown on $\mathrm{SrTiO_3}$ and $\mathrm{(LaAlO_3)_{0.3}(Sr_2AlTaO_6)_{0.7}}$ substrates, under slight tensile and compressive strains, respectively. Although the films develop a magnetic structure reminiscent of bulk $\mathrm{Sr_2IrO_4}$, the magnetic correlations are extremely anisotropic, with in-plane correlation lengths significantly longer than the out-of-plane correlation lengths. In addition, the compressive (tensile) strain serves to suppress (enhance) the magnetic ordering temperature $\mathrm{T_N}$, while raising (lowering) the energy of the zone boundary magnon. Quantum chemical calculations show that the tuning of magnetic energy scales can be understood in terms of strain-induced change in bond lengths.

cond-mat.str-el↗

The quantum origins of skyrmions and half-skyrmions in Cu2OSeO3

The Skyrme-particle, the $skyrmion$, was introduced over half a century ago and used to construct field theories for dense nuclear matter. But with skyrmions being mathematical objects - special types of topological solitons - they can emerge in much broader contexts. Recently skyrmions were observed in helimagnets, forming nanoscale spin-textures that hold promise as information carriers. Extending over length-scales much larger than the inter-atomic spacing, these skyrmions behave as large, classical objects, yet deep inside they are of quantum origin. Penetrating into their microscopic roots requires a multi-scale approach, spanning the full quantum to classical domain. By exploiting a natural separation of exchange energy scales, we achieve this for the first time in the skyrmionic Mott insulator Cu$_2$OSeO$_3$. Atomistic ab initio calculations reveal that its magnetic building blocks are strongly fluctuating Cu$_4$ tetrahedra. These spawn a continuum theory with a skyrmionic texture that agrees well with reported experiments. It also brings to light a decay of skyrmions into half-skyrmions in a specific temperature and magnetic field range. The theoretical multiscale approach explains the strong renormalization of the local moments and predicts further fingerprints of the quantum origin of magnetic skyrmions that can be observed in Cu$_2$OSeO$_3$, like weakly dispersive high-energy excitations associated with the Cu$_4$ tetrahedra, a weak antiferromagnetic modulation of the primary ferrimagnetic order, and a fractionalized skyrmion phase.

cond-mat.str-el↗

Frustrated magnetism and resonating valence bond physics in two-dimensional kagome-like magnets

We explore the phase diagram and the low-energy physics of three Heisenberg antiferromagnets which, like the kagome lattice, are networks of corner-sharing triangles but contain two sets of inequivalent short-distance resonance loops. We use a combination of exact diagonalization, analytical strong-coupling theories, and resonating valence bond approaches, and scan through the ratio of the two inequivalent exchange couplings. In one limit, the lattices effectively become bipartite, while at the opposite limit heavily frustrated nets emerge. In between, competing tunneling processes result in short-ranged spin correlations, a manifold of low-lying singlets (which can be understood as localized bound states of magnetic excitations), and the stabilization of valence bond crystals with resonating building blocks.

cond-mat.str-el↗

Evidence of d-wave Superconductivity in K_(1-x)Na_xFe_2As_2 (x = 0, 0.1) Single Crystals from Low-Temperature Specific Heat Measurements

From the measurement and analysis of the specific heat of high-quality K_(1-x)Na_xFe_2As_2 single crystals we establish the presence of large T^2 contributions with coefficients alpha_sc ~ 30 mJ/mol K^3 at low-T for both x=0 and 0.1. Together with the observed square root field behavior of the specific heat in the superconducting state both findings evidence d-wave superconductivity on almost all Fermi surface sheets with an average gap amplitude of Delta_0 in the range of 0.4 - 0.8 meV. The derived Delta_0 and the observed T_c agree well with the values calculated within the Eliashberg theory, adopting a spin-fluctuation mediated pairing in the intermediate coupling regime.

cond-mat.supr-con↗

The Role of Lattice Coupling in Establishing Electronic and Magnetic Properties in Quasi-One-Dimensional Cuprates

High resolution resonant inelastic x-ray scattering has been performed to reveal the role of lattice-coupling in a family of quasi-1D insulating cuprates, Ca$_{2+5x}$Y$_{2-5x}$Cu$_5$O$_{10}$. Site-dependent low energy excitations arising from progressive emissions of a 70 meV lattice vibrational mode are resolved for the first time, providing a direct measurement of electron-lattice coupling strength. We show that such electron-lattice coupling causes doping-dependent distortions of the Cu-O-Cu bond angle, which sets the intra-chain spin exchange interactions. Our results indicate that the lattice degrees of freedom are fully integrated into the electronic behavior in low dimensional systems.

cond-mat.str-el↗

Persistent high-energy spin excitations in iron pnictide superconductors

Motivated by the premise that superconductivity in iron-based superconductors is unconventional and mediated by spin fluctuations, an intense research effort has been focused on characterizing the spin excitation spectrum in the magnetically ordered parent phases of the Fe-pnictides2,3 and - chalcogenides4. For these undoped materials it is well-established that the spin excitation spectrum consists of a sharp, highly dispersive magnon spanning an energy range of up to 200 meV (ref. 3). The fate of these high-energy magnetic modes upon sizable doping is hitherto unresolved. Using resonant inelastic x-ray scattering we show that optimally doped superconducting Ba0.6K0.4Fe2As2 retains well defined, dispersive high-energy modes of magnetic origin. These paramagnon modes are softer than, though as intense as, the magnon of undoped antiferromagnetic BaFe2As2. The persistence of spin excitations well into the superconducting phase suggests that, if spin fluctuations are responsible for superconducting pairing, they originate from a distinctly correlated spin-state. This connects Fe-pnictide superconductors to the high-Tc cuprates, for which in spite of fundamental differences in the electronic structure, similar paramagnon modes are present5.

cond-mat.supr-con↗

Spin excitations in a single La$_2$CuO$_4$ layer

The dynamics of S=1/2 quantum spins on a 2D square lattice lie at the heart of the mystery of the cuprates \cite{Hayden2004,Vignolle2007,Li2010,LeTacon2011,Coldea2001,Headings2010,Braicovich2010}. In bulk cuprates such as \LCO{}, the presence of a weak interlayer coupling stabilizes 3D Néel order up to high temperatures. In a truly 2D system however, thermal spin fluctuations melt long range order at any finite temperature \cite{Mermin1966}. Further, quantum spin fluctuations transfer magnetic spectral weight out of a well-defined magnon excitation into a magnetic continuum, the nature of which remains controversial \cite{Sandvik2001,Ho2001,Christensen2007,Headings2010}. Here, we measure the spin response of \emph{isolated one-unit-cell thick layers} of \LCO{}. We show that coherent magnons persist even in a single layer of \LCO{} despite the loss of magnetic order, with no evidence for resonating valence bond (RVB)-like spin correlations \cite{Anderson1987,Hsu1990,Christensen2007}. Thus these excitations are well described by linear spin wave theory (LSWT). We also observe a high-energy magnetic continuum in the isotropic magnetic response. This high-energy continuum is not well described by 2 magnon LSWT, or indeed any existing theories.

cond-mat.str-el↗

Bimagnon studies in cuprates with Resonant Inelastic X-ray Scattering at the O K edge. I - An assessment on La2CuO4 and a comparison with the excitation at Cu L3 and Cu K edges

We assess the capabilities of magnetic Resonant Inelastic X-ray Scattering (RIXS) at the O $K$ edge in undoped cuprates by taking La_{2}CuO_{4} as a benchmark case, based on a series of RIXS measurements that we present here. By combining the experimental results with basic theory we point out the fingerprints of bimagnon in the O $K$ edge RIXS spectra. These are a dominant peak around 450 meV, the almost complete absence of dispersion both with $π$ and $σ$ polarization and the almost constant intensity vs. the transferred momentum with $σ$ polarization. This behavior is quite different from Cu $L_3$ edge RIXS giving a strongly dispersing bimagnon tending to zero at the center of the Brillouin zone. This is clearly shown by RIXS measurements at the Cu $L_3$ edge that we present. The Cu $L_3$ bimagnon spectra and those at Cu $K$ edge - both from the literature and from our data - however, have the same shape. These similarities and differences are understood in terms of different sampling of the bimagnon continuum. This panorama points out the unique possibilities offered by O $K$ RIXS in the study of magnetic excitations in cuprates near the center of the BZ.

cond-mat.supr-con↗

Universal recovery of the bright-exciton level-degeneracy in quantum dots without structural symmetry

The lack of structural symmetry which usually characterizes semiconductor quantum dots lifts the energetic degeneracy of the bright excitonic states and hampers severely their use as high fidelity sources of entangled photons. We demonstrate experimentally and theoretically that it is always possible to restore the excitonic degeneracy by the simultaneous application of large strain and electric fields, despite the fact that this possibility has fundamentally been doubted. This is achieved by using one external perturbation to align the polarization of the exciton emission along the axis of the second perturbation, which then erases completely the energy splitting of the states. This result, which holds for any QD structure, highlights the potential of combining complementary external fields to create artificial atoms meeting the stringent requirements posed by scalable semiconductor-based quantum-technology.

cond-mat.mtrl-sci↗

Giant Magnon Gap in Bilayer Iridate Sr3Ir2O7: Enhanced Pseudo-dipolar Interactions Near the Mott Transition

Using resonant inelastic x-ray scattering, we observe in the bilayer iridate Sr3Ir2O7, a spin-orbit coupling driven magnetic insulator with a small charge gap, a magnon gap of ~92 meV for both acoustic and optical branches. This exceptionally large magnon gap exceeds the total magnon bandwidth of ~70 meV and implies a marked departure from the Heisenberg model, in stark contrast to the case of the single-layer iridate Sr2IrO4. Analyzing the origin of these observations, we find that the giant magnon gap results from bond-directional pseudo-dipolar interactions that are strongly enhanced near the metal-insulator transition boundary. This suggests that novel magnetism, such as that inspired by the Kitaev model built on the pseudo-dipolar interactions, may emerge in small charge-gap iridates.

cond-mat.str-el↗

Dimensionality Driven Spin-Flop Transition in Layered Iridates

Using resonant x-ray diffraction, we observe an easy c-axis collinear antiferromagnetic structure for the bilayer Sr$_3$Ir$_2$O$_7$, a significant contrast to the single layer Sr$_2$IrO$_4$ with in-plane canted moments. Based on a microscopic model Hamiltonian, we show that the observed spin-flop transition as a function of number of IrO$_2$ layers is due to strong competition among intra- and inter-layer bond-directional pseudo-dipolar interactions of the spin-orbit entangled $J_{eff}$=1/2 moments. With this we unravel the origin of anisotropic exchange interactions in a Mott insulator in the strong spin-orbit coupling regime, which holds the key to the various types of unconventional magnetism proposed in 5$d$ transition metal oxides.

cond-mat.str-el↗

Spin-Orbital Separation in the quasi 1D Mott-insulator Sr2CuO3

As an elementary particle the electron carries spin \hbar/2 and charge e. When binding to the atomic nucleus it also acquires an angular momentum quantum number corresponding to the quantized atomic orbital it occupies (e.g., s, p or d). Even if electrons in solids form bands and delocalize from the nuclei, in Mott insulators they retain their three fundamental quantum numbers: spin, charge and orbital[1]. The hallmark of one-dimensional (1D) physics is a breaking up of the elementary electron into its separate degrees of freedom[2]. The separation of the electron into independent quasi-particles that carry either spin (spinons) or charge (holons) was first observed fifteen years ago[3]. Using Resonant Inelastic X-ray Scattering on the 1D Mott-insulator Sr2CuO3 we now observe also the orbital degree of freedom separating. We resolve an orbiton liberating itself from spinons and propagating through the lattice as a distinct quasi-particle with a substantial dispersion of ~0.2 eV.

cond-mat.str-el↗

Probing the Unconventional Superconducting State of LiFeAs by Quasiparticle Interference

A crucial step in revealing the nature of unconventional superconductivity is to investigate the symmetry of the superconducting order parameter. Scanning tunneling spectroscopy has proven a powerful technique to probe this symmetry by measuring the quasiparticle interference (QPI) which sensitively depends on the superconducting pairing mechanism. A particularly well suited material to apply this technique is the stoichiometric superconductor LiFeAs as it features clean, charge neutral cleaved surfaces without surface states and a relatively high Tc~18K. Our data reveal that in LiFeAs the quasiparticle scattering is governed by a van-Hove singularity at the center of the Brillouin zone which is in stark contrast with other pnictide superconductors where nesting is crucial for both scattering and s+- superconductivity. Indeed, within a minimal model and using the most elementary order parameters, calculations of the QPI suggest a dominating role of the hole-like bands for the quasiparticle scattering. Our theoretical findings do not support the elementary singlet pairing symmetries s++, s+-, and d-wave. This brings to mind that the superconducting pairing mechanism in LiFeAs is based on an unusual pairing symmetry such as an elementary p-wave (which provides optimal agreement between the experimental data and QPI simulations) or a more complex order parameter (e.g. s+id-wave symmetry).

cond-mat.supr-con↗

Ab initio determination of excitation energies and magnetic couplings in correlated, quasi two-dimensional iridates

To determine the strength of essential electronic and magnetic interactions in the iridates Sr$_2$IrO$_4$ and Ba$_2$IrO$_4$ - potential platforms for high-temperature superconductivity - we use many-body techniques from wavefunction-based electronic-structure theory. Multiplet physics, spin-orbit interactions, and Ir-O hybridization are all treated on equal footing, fully {\it ab initio}. Our calculations put the lowest d-d excitations of Sr$_2$IrO$_4$/Ba$_2$IrO$_4$ at 0.69/0.64 eV, substantially lower than in isostructural cuprates. Charge-transfer excitations start at 3.0/1.9 eV and the magnetic nearest-neighbor exchange coupling is 51/58 meV. Available experimental results are fully consistent with these values, which strongly constrains the parametrization of effective iridate Hamiltonians.

cond-mat.str-el↗

Ca2Y2Cu5O10: the first frustrated quasi-1D ferromagnet close to criticality

Ca2Y2Cu5O10 is build up from edge-shared CuO4 plaquettes forming spin chains. From inelastic neutron scattering data we extract an in-chain nearest neighbor exchange J1 approximately -170 K and the frustrating next neighbor J2 approximately 32 K interactions, both significantly larger than previous estimates. The ratio alpha= J2/J1 approximately 0.19 places the system very close to the critical point alpha_c=0.25 of the J1-J2 chain, but in the ferromagnetic regime. We establish that the vicinity to criticality only marginally affects the dispersion and coherence of the elementary spin-wave-like magnetic excitations, but instead results in a dramatic T-dependence of high-energy Zhang-Rice singlet excitation intensities.

cond-mat.str-el↗

Delta Doping of Ferromagnetism in Antiferromagnetic Manganite Superlattices

We demonstrate that delta-doping can be used to create a dimensionally confined region of metallic ferromagnetism in an antiferromagnetic (AF) manganite host, without introducing any explicit disorder due to dopants or frustration of spins. Delta-doped carriers are inserted into a manganite superlattice (SL) by a digital-synthesis technique. Theoretical consideration of these additional carriers show that they cause a local enhancement of ferromagnetic (F) double-exchange with respect to AF superexchange, resulting in local canting of the AF spins. This leads to a highly modulated magnetization, as measured by polarized neutron reflectometry. The spatial modulation of the canting is related to the spreading of charge from the doped layer, and establishes a fundamental length scale for charge transfer, transformation of orbital occupancy and magnetic order in these manganites. Furthermore, we confirm the existence of the canted, AF state as was predicted by de Gennes [P.-G. de Gennes, Phys. Rev. 118, 141 (1960)], but had remained elusive.

cond-mat.str-el↗

Isospin Dynamics in Sr2IrO4 : Forging Links to Cuprate Superconductivity

We used resonant inelastic x-ray scattering to reveal the nature of magnetic interactions in Sr2IrO4, a 5d transition-metal oxide with a spin-orbit entangled ground state and Jeff=1/2 magnetic momemts, referred to as 'isospins'. The magnon dispersion in Sr2IrO4 is well described by an antiferromagnetic Heisenberg model with isospin one-half moments on a square lattice, which renders the low-energy effective physics of Sr2IrO4 much akin to that in superconducting cuprates. This is further supported by the observation of exciton modes in Sr2IrO4 whose dispersion is strongly renormalized by magnons, which can be understood by analogy to the hole propagation in the background of antiferromagnetically ordered spins in the cuprates.

cond-mat.str-el↗

Probing high-energy electronic excitations using inelastic neutron scattering

High-energy, local multiplet excitations of the d-electrons are revealed in our inelastic neutron scattering measurements on the prototype magnetic insulator NiO. These become allowed by the presence of both non-zero crystal field and spin-orbit coupling. The observed excitations are consistent with optical, x-ray, and EELS measurements of d-d excitations. This experiment serves as a proof of principle that high-energy neutron spectroscopy is a reliable and useful technique for probing electronic excitations in systems with significant crystal field and spin-orbit interactions.

cond-mat.str-el↗