arXiv subjects

D. G. Hawthorn

Publications and source records attributed to D. G. Hawthorn.

At least 19 recordsLinked to original sources

arXiv2025

Anisotropic Spin Stripe Domains in Bilayer La$_3$Ni$_2$O$_7$

The discovery of superconductivity in La$_3$Ni$_2$O$_7$ under pressure has motivated the investigation of a parent spin density wave (SDW) state, which could provide the underlying pairing interaction. Here, we employ resonant soft x-ray scattering and polarimetry on thin films of bilayer La$_3$Ni$_2$O$_7$ to determine that the magnetic structure of the SDW forms unidirectional diagonal spin stripes with moments lying within the NiO$_2$ plane and perpendicular to $\mathbf{Q}_{SDW}$, but without evidence of the strong charge disproportionation typically associated with other nickelates. These stripes form anisotropic domains with shorter correlation lengths perpendicular versus parallel to $\mathbf{Q}_{SDW}$, revealing nanoscale rotational and translational symmetry breaking analogous to the cuprate and Fe-based superconductors, with possible Bloch-like antiferromagnetic domain walls separating orthogonal domains.

cond-mat.supr-con↗

arXiv2024

Superconductivity in the parent infinite-layer nickelate NdNiO$_2$

We report evidence for superconductivity with onset temperatures up to 11 K in thin films of the infinite-layer nickelate parent compound NdNiO$_2$. A combination of oxide molecular-beam epitaxy and atomic hydrogen reduction yields samples with high crystallinity and low residual resistivities, a substantial fraction of which exhibit superconducting transitions. We survey a large series of samples with a variety of techniques, including electrical transport, scanning transmission electron microscopy, x-ray absorption spectroscopy, and resonant inelastic x-ray scattering, to investigate the possible origins of superconductivity. We propose that superconductivity could be intrinsic to the undoped infinite-layer nickelates but suppressed by disorder due to its nodal order parameter, a finding which would necessitate a reconsideration of the nickelate phase diagram. Another possible hypothesis is that the parent materials can be hole doped from randomly dispersed apical oxygen atoms, which would suggest an alternative pathway for achieving superconductivity.

cond-mat.supr-con↗

arXiv2023

Absence of $3a_0$ Charge Density Wave Order in the Infinite Layer Nickelates

A hallmark of many unconventional superconductors is the presence of many-body interactions which give rise to broken symmetry states intertwined with superconductivity. Recent resonant soft x-ray scattering experiments report commensurate $3a_0$ charge density wave order in the infinite layer nickelates, which has important implications regarding the universal interplay between charge order and superconductivity in both the cuprates and nickelates. Here, we present x-ray scattering and spectroscopy measurements on a series of NdNiO$_{2+x}$ samples which reveal that the signatures of charge density wave order are absent in fully reduced, single-phase NdNiO$_2$. The $3a_0$ superlattice peak instead originates from a partially reduced impurity phase where excess apical oxygens form ordered rows with 3 unit cell periodicity. The absence of any observable charge density wave order in NdNiO$_2$ highlights a crucial difference between the phase diagrams of the cuprate and nickelate superconductors.

cond-mat.supr-con↗

arXiv2022

Enhanced charge density wave coherence in a light-quenched, high-temperature superconductor

Superconductivity and charge density waves (CDW) are competitive, yet coexisting orders in cuprate superconductors. To understand their microscopic interdependence, a probe capable of discerning their interaction on its natural length and time scales is necessary. We use ultrafast resonant soft x-ray scattering to track the transient evolution of CDW correlations in YBa$_{2}$Cu$_{3}$O$_{6+x}$ following the quench of superconductivity by an infrared laser pulse. We observe a non-thermal response of the CDW order characterized by a near doubling of the correlation length within $\approx$ 1 picosecond of the superconducting quench. Our results are consistent with a model in which the interaction between superconductivity and CDW manifests inhomogeneously through disruption of spatial coherence, with superconductivity playing the dominant role in stabilizing CDW topological defects, such as discommensurations.

cond-mat.supr-con↗

arXiv2021

Vanishing nematic order beyond the pseudogap phase in overdoped cuprate superconductors

During the last decade, translational and rotational symmetry-breaking phases -- density wave order and electronic nematicity -- have been established as generic and distinct features of many correlated electron systems, including pnictide and cuprate superconductors. However, in cuprates, the relationship between these electronic symmetry-breaking phases and the enigmatic pseudogap phase remains unclear. Here, we employ resonant x-ray scattering in a cuprate high-temperature superconductor La$_{1.6-x}$Nd$_{0.4}$Sr$_{x}$CuO$_{4}$ (Nd-LSCO) to navigate the cuprate phase diagram, probing the relationship between electronic nematicity of the Cu 3$d$ orbitals, charge order, and the pseudogap phase as a function of doping. We find evidence for a considerable decrease in electronic nematicity beyond the pseudogap phase, either by raising the temperature through the pseudogap onset temperature $T^{*}$ or increasing doping through the pseudogap critical point, $p^{*}$. These results establish a clear link between electronic nematicity, the pseudogap, and its associated quantum criticality in overdoped cuprates. Our findings anticipate that electronic nematicity may play a larger role in understanding the cuprate phase diagram than previously recognized, possibly having a crucial role in the phenomenology of the pseudogap phase.

cond-mat.str-el↗

arXiv2020

Evidence for bond-disproportionation in LiNiO2 from x-ray absorption spectroscopy

The electronic structure of LiNiO$_2$, a promising Li-ion battery cathode material, has remained a challenge to understand due to its highly covalent yet correlated nature. Here we elucidate the electronic structure in LiNiO$_2$ and the related compound NaNiO$_2$ using x-ray absorption spectra (XAS) and quantum many-body calculations. Notably, we use inverse partial fluorescence yield to correctly measure the Ni $L$-edge XAS, which is inaccurate using conventional methods. We show that the XAS are indicative of a strong Jahn-Teller effect in NaNiO$_2$ and a bond disproportionated state in LiNiO$_2$, supporting a theory of a high-entropy, glassy disproportionated state that stabilizes charging cycles in LiNiO$_2$.

cond-mat.str-el↗

arXiv2020

Orbital Symmetries of Charge Density Wave Order in YBa2Cu3O6+x

Charge density wave (CDW) order has been shown to compete and coexist with superconductivity in underdoped cuprates. Theoretical proposals for the CDW order include an unconventional $d$-symmetry form factor CDW, evidence for which has emerged from measurements, including resonant soft x-ray scattering (RSXS) in YBa$_2$Cu$_3$O$_{6+x}$ (YBCO). Here, we revisit RSXS measurements of the CDW symmetry in YBCO, using a variation in the measurement geometry to provide enhanced sensitivity to orbital symmetry. We show that the $(0\ 0.31\ L)$ CDW peak measured at the Cu $L$ edge is dominated by an $s$ form factor rather than a $d$ form factor as was reported previously. In addition, by measuring both $(0.31\ 0\ L)$ and $(0\ 0.31\ L)$ peaks, we identify a pronounced difference in the orbital symmetry of the CDW order along the $a$ and $b$ axes, with the CDW along the $a$ axis exhibiting orbital order in addition to charge order.

cond-mat.supr-con↗

arXiv2018

Synthesis of high-oxidation Y-Ba-Cu-O phases in superoxygenated thin films

It is known that solid-state reaction in high-pressure oxygen can stabilize high-oxidation phases of Y-Ba-Cu-O superconductors in powder form. We extend this superoxygenation concept of synthesis to thin films which, due to their large surface-to-volume ratio, are more reactive thermodynamically. Epitaxial thin films of $\rm{YBa_2Cu_3O_{7-δ}}$ grown by pulsed laser deposition are annealed at up to 700 atm O$_2$ and 900$^\circ$C, in conjunction with Cu enrichment by solid-state diffusion. The films show clear formation of $\rm{Y_2Ba_4Cu_7O_{15-δ}}$ and $\rm{Y_2Ba_4Cu_8O_{16}}$ as well as regions of $\rm{YBa_2Cu_5O_{9-δ}}$ and YBa$_2$Cu$_6$O$_{10-δ}$ phases, according to scanning transmission electron microscopy, x-ray diffraction and x-ray absorption spectroscopy. Similarly annealed $\rm{YBa_2Cu_3O_{7-δ}}$ powders show no phase conversion. Our results demonstrate a novel route of synthesis towards discovering more complex phases of cuprates and other superconducting oxides.

cond-mat.supr-con↗

arXiv2016

Orbital symmetry of charge density wave order in La1.875Ba0.125CuO4 and YBa2Cu3O6.67

Recent theories of charge density wave (CDW) order in high temperature superconductors have predicted a primarily d CDW orbital symmetry. Here, we report on the orbital symmetry of CDW order in the canonical cuprate superconductors La1.875Ba0.125CuO4 (LBCO) and YBa2Cu3O6.67 (YBCO), using resonant soft x-ray scattering and a model mapped to the CDW orbital symmetry. From measurements sensitive to the O sublattice, we conclude that LBCO has predominantly s' CDW orbital symmetry, in contrast to the d orbital symmetry recently reported in other cuprates. Additionally, we show for YBCO that the CDW orbital symmetry differs along the a and b crystal axes and that these both differ from LBCO. This work highlights CDW orbital symmetry as an additional key property that distinguishes the different cuprate families. We discuss how the CDW symmetry may be related to the "1/8--anomaly" and to static spin ordering.

cond-mat.supr-con↗

arXiv2016

Nematicity in stripe ordered cuprates probed via resonant x-ray scattering

In underdoped cuprate superconductors, a rich competition occurs between superconductivity and charge density wave (CDW) order. Whether rotational symmetry breaking (nematicity) occurs intrinsically and generically or as a consequence of other orders is under debate. Here we employ resonant x-ray scattering in stripe-ordered (La,M)_2CuO_4 to probe the relationship between electronic nematicity of the Cu 3d orbitals, structure of the (La,M)_2O_2 layers, and CDW order. We find distinct temperature dependences for the structure of the (La,M)_2O_2 layers and the electronic nematicity of the CuO_2 planes, with only the latter being enhanced by the onset of CDW order. These results identify electronic nematicity as an order parameter that is distinct from a purely structural order parameter in underdoped striped cuprates.

cond-mat.supr-con↗

arXiv2015

The symmetry of charge order in cuprates

Charge-ordered ground states permeate the phenomenology of 3d-based transition metal oxides, and more generally represent a distinctive hallmark of strongly-correlated states of matter. The recent discovery of charge order in various cuprate families fueled new interest into the role played by this incipient broken symmetry within the complex phase diagram of high-Tc superconductors. Here we use resonant X-ray scattering to resolve the main characteristics of the charge-modulated state in two cuprate families: Bi2201 and YBCO. We detect no signatures of spatial modulations along the nodal direction in Bi2201, thus clarifying the inter-unit-cell momentum-structure of charge order. We also resolve the intra-unit-cell symmetry of the charge ordered state, which is revealed to be best represented by a bond-order with modulated charges on the O-2p orbitals and a prominent d-wave character. These results provide insights on the microscopic description of charge order in cuprates, and on its origin and interplay with superconductivity.

cond-mat.supr-con↗

arXiv2014

Impact of Quenched Oxygen Disorder on Charge Density Wave Order in YBa$_2$Cu$_3$O$_{6+x}$

The competition between superconductivity and charge density wave (CDW) order in underdoped cuprates has now been widely reported, but the role of disorder in this competition has yet to be fully resolved. A central question is whether disorder sets the length scale of the CDW order, for instance by pinning charge density fluctuations or disrupting an otherwise long range order. Using resonant soft x-ray scattering, we investigate the sensitivity of CDW order in YBa$_2$Cu$_3$O$_{6+x}$ (YBCO) to varying levels of oxygen disorder. We find that quench cooling YBCO$_{6.67}$ (YBCO$_{6.75}$) crystals to destroy their o-V and o-VIII (o-III) chains decreases the intensity of the CDW superlattice peak by a factor of 1.9 (1.3), but has little effect on the CDW correlation length, incommensurability, and temperature dependence. This reveals that while quenched oxygen disorder influences the CDW order parameter, the spatial extent of the CDW order is insensitive to the level of quenched oxygen disorder and may instead be a consequence of competition with superconductivity.

cond-mat.supr-con↗

arXiv2013

Electronic superlattice revealed by resonant scattering from random impurities in Sr3Ru2O7

Resonant elastic x-ray scattering (REXS) is an exquisite element-sensitive tool for the study of subtle charge, orbital, and spin superlattice orders driven by the valence electrons, which therefore escape detection in conventional x-ray diffraction (XRD). Although the power of REXS has been demonstrated by numerous studies of complex oxides performed in the soft x-ray regime, the cross section and photon wavelength of the material-specific elemental absorption edges ultimately set the limit to the smallest superlattice amplitude and periodicity one can probe. Here we show -- with simulations and REXS on Mn-substituted Sr$_3$Ru$_2$O$_7$ -- that these limitations can be overcome by performing resonant scattering experiments at the absorption edge of a suitably-chosen, dilute impurity. This establishes that -- in analogy with impurity-based methods used in electron-spin-resonance, nuclear-magnetic resonance, and Mössbauer spectroscopy -- randomly distributed impurities can serve as a non-invasive, but now momentum-dependent probe, greatly extending the applicability of resonant x-ray scattering techniques.

cond-mat.str-el↗

arXiv2013

Resonant X-Ray Scattering Measurements of a Spatial Modulation of the Cu 3d and O 2p Energies in Stripe-Ordered Cuprate Superconductors

A prevailing description of the stripe phase in underdoped cuprate superconductors is that the charge carriers (holes) phase segregate on a microscopic scale into hole rich and hole poor regions. We report resonant elastic x-ray scattering measurements of stripe-ordered La$_{1.475}$Nd$_{0.4}$Sr$_{0.125}$CuO$_4$ at the Cu $L$ and O $K$ absorption edges that identify an additional feature of stripe order. Analysis of the energy dependence of the scattering intensity reveals that the dominant signature of the stripe order is a spatial modulation in the energies of Cu 3d and O 2p states rather than the large modulation of the charge density (valence) envisioned in the common stripe paradigm. These energy shifts are interpreted as a spatial modulation of the electronic structure and may point to a valence-bond-solid interpretation of the stripe phase.

cond-mat.supr-con↗

arXiv2012

Distinct Charge Orders in the Planes and Chains of Ortho-III-Ordered YBa$_2$Cu$_3$O$_{6+δ}$ Superconductors Identified by Resonant Elastic X-ray Scattering

Recently, charge density wave (CDW) order in the CuO$_2$ planes of underdoped YBa$_2$Cu$_3$O$_{6+δ}$ was detected using resonant soft x-ray scattering. An important question remains: is the chain layer responsible for this charge ordering? Here, we explore the energy and polarization dependence of the resonant scattering intensity in a detwinned sample of YBa$_2$Cu$_3$O$_{6.75}$ with ortho-III oxygen ordering in the chain layer. We show that the ortho-III CDW order in the chains is distinct from the CDW order in the planes. The ortho-III structure gives rise to a commensurate superlattice reflection at $Q$=[0.33 0 $L$] whose energy and polarization dependence agrees with expectations for oxygen ordering and a spatial modulation of the Cu valence in the chains. Incommensurate peaks at [0.30 0 $L$] and [0 0.30 $L$] from the CDW order in the planes are shown to be distinct in $Q$ as well as their temperature, energy, and polarization dependence, and are thus unrelated to the structure of the chain layer. Moreover, the energy dependence of the CDW order in the planes is shown to result from a spatial modulation of energies of the Cu 2$p$ to 3$d_{x^2-y^2}$ transition, similar to stripe-ordered 214 cuprates.

cond-mat.supr-con↗

arXiv2012

Long-range incommensurate charge fluctuations in (Y,Nd)Ba2Cu3O(6+x)

There are increasing indications that superconductivity competes with other orders in cuprate superconductors, but obtaining direct evidence with bulk-sensitive probes is challenging. We have used resonant soft x-ray scattering to identify two-dimensional charge fluctuations with an incommensurate periodicity of $\bf \sim 3.2$ lattice units in the copper-oxide planes of the superconductors (Y,Nd)Ba$_2$Cu$_3$O$_{6+x}$ with hole concentrations $0.09 \leq p \leq 0.13$ per planar Cu ion. The intensity and correlation length of the fluctuation signal increase strongly upon cooling down to the superconducting transition temperature, $T_c$; further cooling below $T_c$ abruptly reverses the divergence of the charge correlations. In combination with prior observations of a large gap in the spin excitation spectrum, these data indicate an incipient charge-density-wave instability that competes with superconductivity.

cond-mat.str-el↗

arXiv2012

Determination of total x-ray absorption coefficient using non-resonant x-ray emission

An alternative measure of x-ray absorption spectroscopy (XAS) called inverse partial fluorescence yield (IPFY) has recently been developed that is both bulk sensitive and free of saturation effects. Here we show that the angle dependence of IPFY can provide a measure directly proportional to the total x-ray absorption coefficient, $μ(E)$. In contrast, fluorescence yield (FY) and electron yield (EY) spectra are offset and/or distorted from $μ(E)$ by an unknown and difficult to measure amount. Moreover, our measurement can determine $μ(E)$ in absolute units with no free parameters by scaling to $μ(E)$ at the non-resonant emission energy. We demonstrate this technique with measurements on NiO and NdGaO$_3$. Determining $μ(E)$ across edge-steps enables the use of XAS as a non-destructive measure of material composition. In NdGaO$_3$, we also demonstrate the utility of IPFY for insulating samples, where neither EY or FY provide reliable spectra due to sample charging and self-absorption effects, respectively.

cond-mat.str-el↗

arXiv2012

Utility of the inverse partial fluorescence for electronic structure studies of battery materials

X-ray absorption spectroscopy (XAS) is one of the most widely used experimental techniques to study the electronic and spatial structure of materials. Fluorescence yield mode is bulk-sensitive, but has several serious problems coming from saturation effects. In this study, we show the usefulness of partial fluorescence yields in addressing these problems. We discuss the different behaviors of La2NiMnO6 and LiMnO2 at the Mn 2p absorption edges. The total fluorescence yield produces misleading spectra for LiMnO2 due to the absence of high-Z (Z: atomic number) elements. We conclude that the measurement of the inverse partial fluorescence yield is essential in studies of LiMnO2, which is a hotly debated Li-ion battery material.

cond-mat.mtrl-sci↗