arXiv subjects

N. B. Brookes

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

At least 37 records · Page 2Linked to original sources

arXiv2020

Charge density waves in YBa$_2$Cu$_3$O$_{6.67}$ probed by resonant x-ray scattering under uniaxial compression

We report a comprehensive Cu L$_3$-edge resonant x-ray scattering study of two- and three-dimensional (2D and 3D) incommensurate charge correlations in single crystals of the underdoped high-temperature superconductor YBa$_2$Cu$_3$O$_{6.67}$ under uniaxial compression up to 1% along the two inequivalent Cu-O-Cu bond directions (a and b) in the CuO$_2$ planes. The pressure response of the 2D charge correlations is symmetric: pressure along a enhances correlations along b, and vice versa. Our results imply that the underlying order parameter is uniaxial. In contrast, 3D long-range charge order is only observed along b in response to compression along a. Spectroscopic resonant x-ray scattering measurements show that the 3D charge order resides exclusively in the CuO$_2$ planes and may thus be generic to the cuprates. We discuss implications of these results for models of electronic nematicity and for the interplay between charge order and superconductivity.

cond-mat.supr-con↗

arXiv2019

Formation of Incommensurate Charge Density Waves in Cuprates

Although charge density waves (CDWs) are omnipresent in cuprate high-temperature superconductors, they occur at significantly different wavevectors, confounding efforts to understand their formation mechanism. Here, we use resonant inelastic x-ray scattering to investigate the doping- and temperature-dependent CDW evolution in La2-xBaxCuO4 (x=0.115-0.155). We discovered that the CDW develops in two stages with decreasing temperature. A precursor CDW with quasi-commensurate wavevector emerges first at high-temperature. This doping-independent precursor CDW correlation originates from the CDW phase mode coupled with a phonon and "seeds" the low-temperature CDW with strongly doping dependent wavevector. Our observation reveals the precursor CDW and its phase mode as the building blocks of the highly intertwined electronic ground state in the cuprates.

cond-mat.supr-con↗

arXiv2019

Spin-orbit coupling and crystal-field distortions for a low-spin $3d^5$ state in BaCoO$_{3}$

We have studied the electronic structure of BaCoO$_3$ using soft x-ray absorption spectroscopy at the Co-$L_{2,3}$ and O-$K$ edges, magnetic circular dichroism at the Co-$L_{2,3}$ edges, as well as valence band hard x-ray photoelectron spectroscopy. The quantitative analysis of the spectra established that the Co ions are in the formal low-spin tetravalent 3$d^5$ state and that the system is a negative charge transfer Mott insulator. The spin-orbit coupling plays also an important role for the magnetism of the system. At the same time, a trigonal crystal field is present with sufficient strength to bring the 3$d^5$ ion away from the $J_{eff} = 1/2$ state. The sign of this crystal field is such that the $a_{1g}$ orbital is doubly occupied, explaining the absence of a Peierl's transition in this system which consists of chains of face-sharing CoO$_6$ octahedra. Moreover, with one hole residing in the $e_g^π$, the presence of an orbital moment and strong magneto-crystalline anisotropy can be understood. Yet, we also infer that crystal fields with lower symmetry must be present to reproduce the measured orbital moment quantitatively, thereby suggesting the possibility for orbital ordering to occur in BaCoO$_3$.

cond-mat.str-el↗

arXiv2019

Resonant inelastic x-ray scattering study of bond order and spin excitations in nickelate thin-film structures

We used high-resolution resonant inelastic x-ray scattering (RIXS) at the Ni $L_3$ edge to simultaneously investigate high-energy interband transitions characteristic of Ni-O bond ordering and low-energy collective excitations of the Ni spins in the rare-earth nickelates $R$NiO$_3$ ($R$ = Nd, Pr, La) with pseudocubic perovskite structure. With the support of calculations based on a double-cluster model we quantify bond order (BO) amplitudes for different thin films and heterostructures and discriminate short-range BO fluctuations from long-range static order. Moreover we investigate magnetic order and exchange interactions in spatially confined $R$NiO$_3$ slabs by probing dispersive magnon excitations. While our study of superlattices (SLs) grown in the (001) direction of the perovskite structure reveals a robust non-collinear spin spiral magnetic order with dispersive magnon excitations that are essentially unperturbed by BO modulations and spatial confinement, we find magnons with flat dispersions and strongly reduced energies in SLs grown in the $(111)_{\text{pc}}$ direction that exhibit collinear magnetic order. These results give insight into the interplay of different collective ordering phenomena in a prototypical 3$d$ transition metal oxide and establish RIXS as a powerful tool to quantitatively study several order parameters and the corresponding collective excitations within one experiment.

cond-mat.str-el↗

arXiv2019

Polarization resolved Cu $L_3$-edge resonant inelastic x-ray scattering of orbital and spin excitations in NdBa$_{2}$Cu$_{3}$O$_{7-δ}$

High resolution resonant inelastic x-ray scattering (RIXS) has proven particularly effective in the determination of crystal field and spin excitations in cuprates. Its strength lies in the large Cu $L_{3}$ resonance and in the fact that the scattering cross section follows quite closely the single-ion model predictions, both in the insulating parent compounds and in the superconducting doped materials. However, the spectra become increasingly broader with (hole) doping, hence resolving and assigning spectral features has proven challenging even with the highest energy resolution experimentally achievable. Here we have overcome this limitation by measuring the complete polarization dependence of the RIXS spectra as function of momentum transfer and doping in thin films of NdBa$_{2}$Cu$_{3}$O$_{7-δ}$. Besides confirming the previous assignment of $dd$ and spin excitations (magnon, bimagnon) in the antiferromagnetic insulating parent compound, we unequivocally single out the actual spin-flip contribution at all dopings. We also demonstrate that the softening of $dd$ excitations is mainly attributed to the shift of the $xy$ peak to lower energy loss. These results provide a definitive assessment of the RIXS spectra of cuprates and demonstrate that RIXS measurements with full polarization control are practically feasible and highly informative.

cond-mat.supr-con↗

arXiv2019

Paramagnon dispersion in $β$-FeSe observed by Fe $L$-edge resonant inelastic x-ray scattering

We report an Fe $L$-edge resonant inelastic x-ray scattering (RIXS) study of the unusual superconductor $β$-FeSe. The high energy resolution of this RIXS experiment ($\approx\,$55$\,$meV FWHM) made it possible to resolve low-energy excitations of the Fe $3d$ manifold. These include a broad peak which shows dispersive trends between 100-200$\,$meV along the $(π,0)$ and $(π,π)$ directions of the one-Fe square reciprocal lattice, and which can be attributed to paramagnon excitations. The multi-band valence state of FeSe is among the most metallic in which such excitations have been discerned by soft x-ray RIXS.

cond-mat.supr-con↗

arXiv2018

Three dimensional collective charge excitations in electron-doped cuprate superconductors

High temperature cuprate superconductors consist of stacked CuO2 planes, with primarily two dimensional electronic band structures and magnetic excitations, while superconducting coherence is three dimensional. This dichotomy highlights the importance of out-of-plane charge dynamics, believed to be incoherent in the normal state, yet lacking a comprehensive characterization in energy-momentum space. Here, we use resonant inelastic x-ray scattering (RIXS) with polarization analysis to uncover the pure charge character of a recently discovered collective mode in electron-doped cuprates. This mode disperses along both the in- and, importantly, out-of-plane directions, revealing its three dimensional nature. The periodicity of the out-of-plane dispersion corresponds to the CuO2 plane distance rather than the crystallographic c-axis lattice constant, suggesting that the interplane Coulomb interaction drives the coherent out-of-plane charge dynamics. The observed properties are hallmarks of the long-sought acoustic plasmon, predicted for layered systems and argued to play a substantial role in mediating high temperature superconductivity.

cond-mat.supr-con↗

arXiv2018

Dynamical charge density fluctuations pervading the phase diagram of a Cu-based high-Tc superconductor

Charge density waves are a common occurrence in all families of high critical temperature superconducting cuprates. Although consistently observed in the underdoped region of the phase diagram and at relatively low temperatures, it is still unclear to what extent they influence the unusual properties of these systems. Using resonant x-ray scattering we carefully determined the temperature dependence of charge density modulations in (Y,Nd)Ba$_2$Cu$_3$O$_{7-δ}$ for three doping levels. We discovered short-range dynamical charge density fluctuations besides the previously known quasi-critical charge density waves. They persist up to well above the pseudogap temperature T*, are characterized by energies of few meV and pervade a large area of the phase diagram, so that they can play a key role in shaping the peculiar normal-state properties of cuprates.

cond-mat.supr-con↗

arXiv2018

Symmetry breaking at the (111) interfaces of SrTiO${_3}$ hosting a 2D-electron system

We used x-ray absorption spectroscopy to study the orbital symmetry and the energy band splitting of (111) LaAlO${_3}$/SrTiO${_3}$ and LaAlO${_3}$/EuTiO${_3}$/SrTiO${_3}$ heterostructures, hosting a quasi two-dimensional electron system (q2DES), and of a Ti-terminated (111) SrTiO${_3}$ single crystal, also known to form a q2DES at its surface. We demonstrate that the bulk tetragonal Ti-3d D${_4}$${_h}$ crystal field is turned into trigonal D${_3}$${_d}$ crystal field in all cases. The symmetry adapted a${_1}$${_g}$ and e${^π_g}$ orbitals are non-degenerate in energy and their splitting, Δ, is positive at the bare STO surface but negative in the heterostructures, where the a${_1}$${_g}$ orbital is lowest in energy. These results demonstrate that the interfacial symmetry breaking induced by epitaxial engineering of oxide interfaces has a dramatic effect on their electronic properties, and it can be used to manipulate the ground state of the q2DES.

cond-mat.mtrl-sci↗

arXiv2018

Dispersion, damping, and intensity of spin excitations in the single-layer (Bi,Pb)$_{2}$(Sr,La)$_{2}$CuO$_{6+δ}$ cuprate superconductor family

Using Cu-$L_3$ edge resonant inelastic x-ray scattering (RIXS) we measured the dispersion and damping of spin excitations (magnons and paramagnons) in the high-$T_\mathrm{c}$ superconductor (Bi,Pb)$_{2}$(Sr,La)$_{2}$CuO$_{6+δ}$ (Bi2201), for a large doping range across the phase diagram ($0.03\lesssim p\lesssim0.21$). Selected measurements with full polarization analysis unambiguously demonstrate the spin-flip character of these excitations, even in the overdoped sample. We find that the undamped frequencies increase slightly with doping for all accessible momenta, while the damping grows rapidly, faster in the (0,0)$\rightarrow$(0.5,0.5) nodal direction than in the (0,0)$\rightarrow$(0.5,0) antinodal direction. We compare the experimental results to numerically exact determinant quantum Monte Carlo (DQMC) calculations that provide the spin dynamical structure factor $S(\textbf{Q},ω)$ of the three-band Hubbard model. The theory reproduces well the momentum and doping dependence of the dispersions and spectral weights of magnetic excitations. These results provide compelling evidence that paramagnons, although increasingly damped, persist across the superconducting dome of the cuprate phase diagram; this implies that long range antiferromagnetic correlations are quickly washed away, while short range magnetic interactions are little affected by doping.

cond-mat.supr-con↗

arXiv2018

Site-selective Probe of Magnetic Excitations in Rare-earth Nickelates using Resonant Inelastic X-ray Scattering

We have used high-resolution resonant inelastic x-ray scattering (RIXS) to study a thin film of NdNiO$_3$, a compound whose unusual spin- and bond-ordered electronic ground state has been of long-standing interest. Below the magnetic ordering temperature, we observe well-defined collective magnon excitations along different high-symmetry directions in momentum space. The magnetic spectra depend strongly on the incident photon energy, which we attribute to RIXS coupling to different local electronic configurations of the expanded and compressed NiO$_6$ octahedra in the bond-ordered state. Both the noncollinear magnetic ground state and the observed site-dependent magnon excitations are well described by a model that assumes strong competition between the antiferromagnetic superexchange and ferromagnetic double-exchange interactions. Our study provides direct insight into the magnetic dynamics and exchange interactions of the rare-earth nickelates, and demonstrates that RIXS can serve as a site-selective probe of magnetism in these and other materials.

cond-mat.str-el↗

arXiv2018

Similar temperature scale for valence changes in Kondo lattices with different Kondo temperatures

The Kondo model predicts that both the valence at low temperatures and its temperature dependence scale with the characteristic energy T_K of the Kondo interaction. Here, we study the evolution of the 4f occupancy with temperature in a series of Yb Kondo lattices using resonant X-ray emission spectroscopy. In agreement with simple theoretical models, we observe a scaling between the valence at low temperature and T_K obtained from thermodynamic measurements. In contrast, the temperature scale T_v at which the valence increases with temperature is almost the same in all investigated materials while the Kondo temperatures differ by almost four orders of magnitude. This observation is in remarkable contradiction to both naive expectation and precise theoretical predictions of the Kondo model, asking for further theoretical work in order to explain our findings. Our data exclude the presence of a quantum critical valence transition in YbRh2Si2.

cond-mat.str-el↗

arXiv2018

Coupling between dynamic magnetic and charge-order correlations in the cuprate superconductor Nd$_{2-x}$Ce$_{x}$CuO$_4$

Charge order has now been observed in several cuprate high-temperature superconductors. We report a resonant inelastic x-ray scattering experiment on the electron-doped cuprate Nd$_{2-x}$Ce$_{x}$CuO$_4$ that demonstrates the existence of dynamic correlations at the charge order wave vector. Upon cooling we observe a softening in the electronic response, which has been predicted to occur for a d-wave charge order in electron-doped cuprates. At low temperatures, the energy range of these excitations coincides with that of the dispersive magnetic modes known as paramagnons. Furthermore, measurements where the polarization of the scattered photon is resolved indicate that the dynamic response at the charge order wave vector primarily involves spin-flip excitations. Overall, our findings indicate a coupling between dynamic magnetic and charge-order correlations in the cuprates.

cond-mat.supr-con↗

arXiv2018

High-resolution resonant inelastic soft X-ray scattering as a probe of the crystal electrical field in lanthanides demonstrated for the case of CeRh2Si2

The magnetic properties of rare earth compounds are usually well captured by assuming a fully localized f shell and only considering the Hund's rule ground state multiplet split by a crystal electrical field (CEF). Currently, the standard technique for probing CEF excitations in lanthanides is inelastic neutron scattering. Here we show that with the recent leap in energy resolution, resonant inelastic soft X-ray scattering has become a serious alternative for looking at CEF excitations with some distinct advantages compared to INS. As an example we study the CEF scheme in CeRh2Si2, a system that has been intensely studied for more than two decades now but for which no consensus has been reached yet as to its CEF scheme. We used two new features that have only become available very recently in RIXS, high energy resolution of about 30 meV as well as polarization analysis in the scattered beam, to find a unique CEF description for CeRh2Si2. The result agrees well with previous INS and magnetic susceptibility measurements. Due to its strong resonant character, RIXS is applicable to very small samples, presents very high cross sections for all lanthanides, and further benefits from the very weak coupling to phonon excitation. The rapid progress in energy resolution of RIXS spectrometers is making this technique increasingly attractive for the investigation of the CEF scheme in lanthanides.

cond-mat.str-el↗

arXiv2018

Systematics of electronic and magnetic properties in the transition metal doped Sb$_2$Te$_3$ quantum anomalous Hall platform

The quantum anomalous Hall effect (QAHE) has recently been reported to emerge in magnetically-doped topological insulators. Although its general phenomenology is well established, the microscopic origin is far from being properly understood and controlled. Here we report on a detailed and systematic investigation of transition-metal (TM)-doped Sb$_2$Te$_3$. By combining density functional theory (DFT) calculations with complementary experimental techniques, i.e., scanning tunneling microscopy (STM), resonant photoemission (resPES), and x-ray magnetic circular dichroism (XMCD), we provide a complete spectroscopic characterization of both electronic and magnetic properties. Our results reveal that the TM dopants not only affect the magnetic state of the host material, but also significantly alter the electronic structure by generating impurity-derived energy bands. Our findings demonstrate the existence of a delicate interplay between electronic and magnetic properties in TM-doped TIs. In particular, we find that the fate of the topological surface states critically depends on the specific character of the TM impurity: while V- and Fe-doped Sb$_2$Te$_3$ display resonant impurity states in the vicinity of the Dirac point, Cr and Mn impurities leave the energy gap unaffected. The single-ion magnetic anisotropy energy and easy axis, which control the magnetic gap opening and its stability, are also found to be strongly TM impurity-dependent and can vary from in-plane to out-of-plane depending on the impurity and its distance from the surface. Overall, our results provide general guidelines for the realization of a robust QAHE in TM-doped Sb$_2$Te$_3$ in the ferromagnetic state.

cond-mat.mes-hall↗

arXiv2017

High-temperature charge density wave correlations in La$_{1.875}$Ba$_{0.125}$CuO$_{4}$ without spin-charge locking

Although all superconducting cuprates display charge-ordering tendencies, their low-temperature properties are distinct, impeding efforts to understand the phenomena within a single conceptual framework. While some systems exhibit stripes of charge and spin, with a locked periodicity, others host charge density waves (CDWs) without any obviously related spin order. Here we use resonant inelastic x-ray scattering (RIXS) to follow the evolution of charge correlations in the canonical stripe ordered cuprate La$_{1.875}$Ba$_{0.125}$CuO$_{4}$ (LBCO~$1/8$) across its ordering transition. We find that high-temperature charge correlations are unlocked from the wavevector of the spin correlations, signaling analogies to CDW phases in various other cuprates. This indicates that stripe order at low temperatures is stabilized by the coupling of otherwise independent charge and spin density waves, with important implications for the relation between charge and spin correlations in the cuprates.

cond-mat.supr-con↗

arXiv2017

Re-entrant charge order in overdoped (Bi,Pb)$_{2.12}$Sr$_{1.88}$CuO$_{6+δ}$ outside the pseudogap regime

Charge modulations are considered as a leading competitor of high-temperature superconductivity in the underdoped cuprates, and their relationship to Fermi surface reconstructions and to the pseudogap state is an important subject of current research. Overdoped cuprates, on the other hand, are widely regarded as conventional Fermi liquids without collective electronic order. For the overdoped (Bi,Pb)2.12Sr1.88CuO6+δ (Bi2201) high-temperature superconductor, here we report resonant x-ray scattering measurements revealing incommensurate charge order reflections, with correlation lengths of 40-60 lattice units, that persist up to at least 250K. Charge order is markedly more robust in the overdoped than underdoped regime but the incommensurate wave vectors follow a common trend; moreover it coexists with a single, unreconstructed Fermi surface, without pseudogap or nesting features, as determined from angle-resolved photoemission spectroscopy. This re-entrant charge order is reproduced by model calculations that consider a strong van Hove singularity within a Fermi liquid framework.

cond-mat.supr-con↗

arXiv2017

Crossover from Collective to Incoherent Spin Excitations in Superconducting Cuprates Probed by Detuned Resonant Inelastic X-ray Scattering

Spin excitations in the overdoped high temperature superconductors Tl$_2$Ba$_2$CuO$_{6+δ}$ and (Bi,Pb)$_2$(Sr,La)$_{2}$CuO$_{6+δ}$ were investigated by resonant inelastic x-ray scattering (RIXS) as functions of doping and detuning of the incoming photon energy above the Cu-$L_3$ absorption peak. The RIXS spectra at optimal doping are dominated by a paramagnon feature with peak energy independent of photon energy, similar to prior results on underdoped cuprates. Beyond optimal doping, the RIXS data indicate a sharp crossover to a regime with a strong contribution from incoherent particle/hole excitations whose maximum shows a fluorescence-like shift upon detuning. The spectra of both compound families are closely similar, and their salient features are reproduced by exact-diagonalization calculations of the single-band Hubbard model on a finite cluster. The results are discussed in the light of recent transport experiments indicating a quantum phase transition near optimal doping.

cond-mat.supr-con↗