arXiv subjects

N. B. Brookes

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

At least 19 recordsLinked to original sources

arXiv2026

High temperature ferromagnetism in epitaxial monolayers of Co-doped Fe5GeTe2

Magnetic van der Waals materials have mainly been investigated in their bulk form or as few-layers flakes. Due to the challenges in producing atomically thin films, only a few have been isolated as monolayers, which typically exhibit long-range magnetic order below 150 K. In this work, we use molecular beam epitaxy to synthesize Co-doped Fe5GeTe2, achieving precise control over both thickness and composition. We demonstrate ferromagnetism well above room temperature in multilayer samples and present clear evidence of ferromagnetic ordering in monolayers up to $\sim$200 K. The changes in Curie temperature and magnetic anisotropy with composition exhibit similar trends in both monolayers and thicker films, indicating that the magnetic properties are primarily governed by intralayer magnetic interactions. Through element-specific X-ray magnetic circular dichroism and density functional theory, we identify the substitution site of Co dopants and reveal the mechanism behind the Curie temperature enhancement induced by Co doping. Our findings suggest that, despite their weak magnetic moment, Co dopants strengthen the magnetic moments on neighboring Fe atoms and enhance the intralayer ferromagnetic exchange interactions.

cond-mat.mtrl-sci↗

arXiv2026

Collective spin excitations in trilayer nickelate La$_4$Ni$_3$O$_{10}$

Ruddlesden-Popper (RP) nickelates have recently emerged as a new family of high-temperature superconductors. In bilayer RP nickelates, magnetic excitations with large exchange couplings have been observed, supporting a spin-mediated pairing mechanism. Whether comparable spin correlations persist in trilayer nickelates, however, remains unknown. Here, we present a Ni $L$-edge resonant inelastic X-ray scattering (RIXS) study of La$_4$Ni$_3$O$_{10}$ single crystals. While the orbital excitations remain similar to those of La$_3$Ni$_2$O$_{7}$, the collective spin excitations in La$_4$Ni$_3$O$_{10}$ exhibit a comparable bandwidth of about $60$ meV but substantially suppressed spectral weight, implying a weaker electronic correlation in the trilayer compounds. Our results underscore the three-dimensional and multi-orbital electronic character in La$_4$Ni$_3$O$_{10}$, highlighting important differences from the bilayer nickelates. These findings provide crucial insights into the evolution of magnetism across the RP nickelate family and its connection to superconductivity.

cond-mat.supr-con↗

arXiv2026

Contrasting Spin Excitations in Octahedral and Square-Planar n=8 Ruddlesden-Popper Nickelates

The discovery of superconductivity in reduced square-planar nickelates marked a major advance in identifying structural and electronic analogs to the high-$T_c$ cuprates. The more recent observation of superconductivity in parent Ruddlesden-Popper (RP) octahedral nickelates with a clear difference in electron count with respect to cuprates raises new questions about the nature of superconductivity across these related but distinct nickelate families. Here, we use Ni $L_3$-edge resonant inelastic x-ray scattering (RIXS) to probe the low-energy excitations in a representative compound of both families: the parent octahedral $n=8$ RP phase Nd$_9$Ni$_8$O$_{25}$ (p-RP), which is non-superconducting, and its reduced square-planar counterpart Nd$_9$Ni$_8$O$_{18}$ (r-RP), which exhibits superconducting correlations with a $T_c \approx 5$ K. The $n=8$ p-RP develops a spin-density-wave (SDW) ground state with ordering wave vector $q_{\mathrm{SDW}} = (1/4,\, 1/4)$, analogous to the bilayer RP, while the $n=8$ r-RP shows an elastic peak at $q^\star = (1/3,\, 0)$. Polarimetric RIXS shows that the p-RP exhibits low-energy spectra dominated by weakly dispersive paramagnons along the 0$\rightarrowπ$ and $π\!\rightarrow\! π$ directions, whereas the r-RP with superconducting correlations displays dispersionless magnetic excitations. Our results comprehensively map out the spin excitations and reveal fundamental differences in the ground state between these two distinct structural families.

cond-mat.str-el↗

arXiv2026

Magnetic Excitations of a Half-Filled Tl-based Cuprate

Strong electron correlations drive Mott insulator transitions. Yet, there exists no framework to classify Mott insulators by their degree of correlation. Cuprate superconductors, with their tunable doping and rich phase diagrams, offer a unique platform to investigate the evolution of these interactions. However, spectroscopic access to a clean half-filled Mott-insulating state is lacking in compounds with the highest superconducting onset temperature. To fill this gap, we introduce a pristine, half-filled thallium-based cuprate system, Tl$_2$Ba$_5$Cu$_4$O$_{x}$. Using high-resolution resonant inelastic x-ray scattering, we probe long-lived magnon excitations and uncover a pronounced kink in the magnon dispersion, marked by a simultaneous change in group velocity and lifetime broadening. Modeling the dispersion within a Hubbard-Heisenberg approach, we extract the interaction strength and compare it with other cuprate systems. Our results establish a cuprate universal relation between electron-electron interaction and magnon zone-boundary dispersion. Superconductivity seems to be optimal at intermediate correlation strength, suggesting an optimal balance between localization and itinerancy.

cond-mat.supr-con↗

arXiv2025

Impact of Electron Correlations on Infinite-Layer Cuprates and Nickelates

Optimization of unconventional superconductivity involves a balance of interaction strengths. Precise determination of correlation strength across different material families is therefore important. Here, we present a combined X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS) study of infinite-layer PrNiO$_2$ and SrCuO$_2$ that enables fair comparison of their interaction strengths. For both compounds, we study the orbital and magnetic excitations and extract their dispersions along high-symmetry directions. Using a single-band Hubbard model and including higher-order exchange interactions, we derive the correlation factor $U/t$ for both compounds. A key finding is that despite a smaller Coulomb repulsion $U$, PrNiO$_2$ exhibits a correlation strength that is 20% stronger than that of its isostructural cuprate counterpart SrCuO$_2$. This indicates that a moderation of the correlation strength may further optimize superconductivity in nickelates.

cond-mat.supr-con↗

arXiv2025

Observation of anisotropic dispersive dark exciton dynamics in CrSBr

Many-body excitons in CrSBr are attracting intense interest in view of their highly anisotropic magneto-optical coupling and their potential for novel optical interfaces within spintronic and magnonic devices. Characterizing the orbital character and propagation of these electronic excitations is crucial for understanding and controlling their behavior; however, this information is challenging to access. Ultra-high resolution resonant inelastic x-ray scattering is a momentum-resolved technique that can address these crucial questions. We present measurements collected at the Cr $L_3$-edge which show a rich spectrum of excitations with a variety of spin-orbital characters. While most of these excitations appear to be localized, the dispersion of the lowest energy dark exciton indicates that it is able to propagate along both the $a$ and $b$ directions within the planes of the crystal. This two-dimensional character is surprising as it contrasts with electrical conductivity and the behavior of the bright exciton, both of which are strongly one-dimensional. The discovery of this propagating dark exciton highlights an unusual coexistence of one- and two-dimensional electronic behaviors in CrSBr.

cond-mat.str-el↗

arXiv2025

Coincident onset of charge order and pseudogap in a homogeneous high-temperature superconductor

Understanding high-temperature superconductivity in cuprates requires knowledge of the metallic phase it evolves from, particularly the pseudogap profoundly affecting the electronic properties at low carrier densities. A key question is the influence of chemical disorder, which is ubiquitous but exceedingly difficult to model. Using resonant x-ray scattering, we identified two-dimensional charge order in stoichiometric YBa$_2$Cu$_4$O$_8$ ($T_c$ = 80 K), which is nearly free of chemical disorder. The charge order amplitude shows a concave temperature dependence and vanishes sharply at $T^*$ = 200 K, the onset of a prominent pseudogap previously determined by spectroscopy, suggesting a causal link between these phenomena. The gradual onset of charge order in other cuprates is thus likely attributable to an inhomogeneous distribution of charge ordering temperatures due to disorder induced by chemical substitution. The relationship between the pseudogap and the disorder-induced gradual freeze-out of charge carriers remains a central issue in research on high-$T_c$ superconductors.

cond-mat.supr-con↗

arXiv2024

Interplay between electronic and lattice superstructures in La$_{2-x}$Ca$_{x}$CuO$_{4}$

Complex oxides are well known to develop oxygen ordering patterns with well defined periodicities, but their interplay with electronic correlations remains largely unexplored. Here, we report resonant and non-resonant x-ray diffraction data indicating a four-unit-cell periodic superstructure related to oxygen vacancy ordering in La$_{2-x}$Ca$_{x}$CuO$_{4}$ films with doping levels from the underdoped ($x = 0.15$) to the extremely overdoped ($x = 0.50$) regime. Whereas the lattice superstructure is temperature independent up to 300 K, a strongly temperature dependent electronic charge density wave (CDW) is observed in the underdoped and slightly overdoped regimes ($x\leq0.20$). The periodicity, in-plane and out-of-plane correlation lengths of the CDW are locked in by the lattice superstructure. Our results highlight the necessity to consider lattice and electronic energetics on equal footing in the high-temperature oxygen-disordered phase to explain oxygen ordering phenomena in complex oxides.

cond-mat.str-el↗

arXiv2024

Strain-Tuned Magnetic Frustration in a Square Lattice $J_1$-$J_2$ Material

Magnetic frustration is a route that can lead to the emergence of novel ground states, including spin liquids and spin ices. Such frustration can be introduced through either the geometry of lattice structures or by incompatible exchange interactions. Identifying suitable strategies to control the degree of magnetic frustration in real systems is an active field of research. In this study, we devise a design principle for the tuning of frustrated magnetism on the square lattice through the manipulation of nearest (NN) and next-nearest neighbor (NNN) antiferromagnetic (AF) exchange interactions. By studying the magnon excitations in epitaxially-strained La$_2$NiO$_4$ films using resonant inelastic x-ray scattering (RIXS) we show that, in contrast to the cuprates, the dispersion peaks at the AF zone boundary. This indicates the presence of an AF-NNN spin interaction. Using first principles simulations and an effective spin-model, we demonstrate the AF-NNN coupling to be a consequence of the two-orbital nature of La$_2$NiO$_4$. Our results demonstrate that compressive strain can enhance this coupling, providing a design principle for the tunability of frustrated magnetism on a square lattice.

cond-mat.str-el↗

arXiv2024

Plasmon dispersion in bilayer cuprate superconductors

The essential building blocks of cuprate superconductors are two-dimensional CuO$_2$ sheets interspersed with charge reservoir layers. In bilayer cuprates, two closely spaced CuO$_2$ sheets are separated by a larger distance from the subsequent pair in the next unit cell. In contrast to single-layer cuprates, prior theoretical work on bilayer systems has predicted two distinct acoustic plasmon bands for a given out-of-plane momentum transfer. Here we report random phase approximation (RPA) calculations for bilayer systems which corroborate the existence of two distinct plasmons bands. We find that the intensity of the lower-energy band is negligibly small, whereas the higher-energy band carries significant spectral weight. We also present resonant inelastic x-ray scattering (RIXS) experiments at the O $K$-edge on the bilayer cuprate Y$_{0.85}$Ca$_{0.15}$Ba$_2$Cu$_3$O$_7$ (Ca-YBCO), which show only one dispersive plasmon branch, in agreement with the RPA calculations. In addition, the RPA results indicate that the dispersion of the higher-energy plasmon band in Ca-YBCO is not strictly acoustic, but exhibits a substantial energy gap of approximately 250 meV at the two-dimensional Brillouin zone center.

cond-mat.supr-con↗

arXiv2024

Evidence of temperature-dependent interplay between spin and orbital moment in van der Waals ferromagnet VI3

Van der Waals materials provide a versatile toolbox for the emergence of new quantum phenomena and the fabrication of functional heterostructures. Among them, the trihalide VI3 stands out for its unique magnetic and structural landscape. Here we investigate the spin and orbital magnetic degrees of freedom in the layered ferromagnet VI3 by means of temperature-dependent x-ray absorption spectroscopy and x-ray magnetic circular and linear dichroism. We detect localized electronic states and reduced magnetic dimensionality, due to electronic correlations. We furthermore provide experimental evidence of (a) an unquenched orbital magnetic moment (up to 0.66(7)) in the ferromagnetic state, and (b) an instability of the orbital moment in proximity of the spin reorientation transition. Our results support a coherent picture where electronic correlations give rise to a strong magnetic anisotropy and a large orbital moment, and establish VI3 as a prime candidate for the study of orbital quantum effects.

cond-mat.mtrl-sci↗

arXiv2024

Evolution of the magnetic excitations in electron-doped $\mathrm{La}_{2-x} \mathrm{Ce}_x \mathrm{CuO}_{4}$

We investigated the high energy spin excitations in electron-doped $\mathrm{La}_{2-x} \mathrm{Ce}_x \mathrm{CuO}_{4}$, a cuprate superconductor, by resonant inelastic x-ray scattering (RIXS) measurements. Efforts were paid to disentangle the paramagnon signal from non-spin-flip spectral weight mixing in the RIXS spectrum at $\bf{Q_{\|}}$ = $(0.6π, 0)$ and $(0.9π, 0)$ along the (1 0) direction. Our results show that, for doping level x from 0.07 to 0.185, the variation of the paramagnon excitation energy is marginal. We discuss the implication of our results in connection with the evolution of the electron correlation strength in this system.

cond-mat.str-el↗

arXiv2023

Signature of quantum criticality in cuprates by charge density fluctuations

The universality of the strange metal phase in many quantum materials is often attributed to the presence of a quantum critical point (QCP), a zero-temperature phase transition ruled by quantum fluctuations. In cuprates, where superconductivity hinders direct QCP observation, indirect evidence comes from the identification of fluctuations compatible with the strange metal phase. Here we show that the recently discovered charge density fluctuations (CDF) possess the right properties to be associated to a quantum phase transition. Using resonant x-ray scattering, we studied the CDF in two families of cuprate superconductors across a wide doping range (up to $p$=0.22). At $p^*\approx$0.19, the putative QCP, the CDF intensity peaks, and the characteristic energy $Δ$ is minimum, marking a wedge-shaped region in the phase diagram indicative of a quantum critical behavior, albeit with anomalies. These findings strengthen the role of charge order in explaining strange metal phenomenology and provide insights into high-temperature superconductivity.

cond-mat.supr-con↗

arXiv2023

Anisotropic hybridization probed by polarization dependent x-ray absorption spectroscopy in VI3 van der Waals Mott ferromagnet

Polarization dependent x-ray absorption spectroscopy was used to study the magnetic ground state and the orbital occupation in bulk-phase VI$_3$ van der Waals crystals below and above the ferromagnetic and structural transitions. X-ray natural linear dichroism and X-ray magnetic circular dichroism spectra acquired at the V $L_{2,3}$ edges are compared against multiplet cluster calculations within the frame of the ligand field theory to quantify the intra-atomic electronic interactions at play and evaluate the effects of symmetry reduction occurring in a trigonally distorted VI$_6$ unit. We observed a non zero linear dichroism proving the presence of an anisotropic charge density distribution around the V$^{3+}$ ion due to the unbalanced hybridization between the Vanadium and the ligand states. Such hybridization acts as an effective trigonal crystal field, slightly lifting the degeneracy of the $t_{2g}^2$ ground state. However, the energy splitting associated to the distortion underestimates the experimental band gap, suggesting that the insulating ground state is stabilized by Mott correlation effects rather than via a Jahn-Teller mechanism. Our results clarify the role of the distortion in VI$_3$ and establish a benchmark for the study of the spectroscopic properties of other van der Waals halides, including emerging 2D materials with mono and few-layers thickness, whose fundamental properties might be altered by reduced dimensions and interface proximity.

cond-mat.str-el↗

arXiv2022

Fate of charge order in overdoped La-based cuprates

In high-temperature cuprate superconductors, stripe order refers broadly to a coupled spin and charge modulation with a commensuration of eight and four lattice units, respectively. How this stripe order evolves across optimal doping remains a controversial question. Here we present a systematic resonant inelastic x-ray scattering (RIXS) study of weak charge correlations in La2-xSrxCuO4 (LSCO) and La1.8-xEu0.2SrxCuO4 (LESCO). Ultra high energy resolution experiments demonstrate the importance of the separation of inelastic and elastic scattering processes. Upon increasing doping x, the long-range temperature dependent stripe order is found to be replaced by short-range temperature independent correlations at a critical point xc = 0.15 distinct from the pseudogap critical doping. We argue that the doping and temperature independent short-range correlations originate from unresolved electron-phonon coupling that broadly peaks at the stripe ordering vector. In LSCO, long-range static stripe order vanishes in a quantum critical point around optimal doping.

cond-mat.supr-con↗

arXiv2021

Charge and spin order dichotomy in NdNiO$_2$ driven by SrTiO$_3$ capping layer

Superconductivity in infinite-layer nickelates holds exciting analogies with that of cuprates, with similar structures and $3d$-electron count. Using resonant inelastic x-ray scattering (RIXS) we studied electronic and magnetic excitations and charge density correlations in Nd$_{1-x}$Sr$_{x}$NiO$_2$ thin films with and without an SrTiO$_3$ capping layer. We observe dispersing magnons only in the capped samples, progressively dampened at higher doping. In addition, we detect an elastic resonant scattering peak in the uncapped $x=0$ compound at wave vector (1/3,0), remindful of the charge order signal in hole doped cuprates. The peak weakens at $x=0.05$ and disappears in the superconducting $x=0.20$ film. The uncapped samples also present a higher degree of Ni$3d$-Nd$5d$ hybridization and a smaller anisotropy of the Ni$3d$ occupation with respect to the capped samples. The role of the capping on the possible hydrogen incorporation or on other mechanisms responsible for the electronic reconstruction far from the interface remains to be understood.

cond-mat.supr-con↗

arXiv2021

Restored strange metal phase through suppression of charge density waves in underdoped YBa$_2$Cu$_3$O$_{7-δ}$

The normal state of optimally doped cuprates is dominated by the "strange metal" phase that shows a linear temperature ($T$) dependence of the resistivity persisting down to the lowest $T$. For underdoped cuprates this behavior is lost below the pseudogap temperature $T^*$, where Charge Density Waves (CDW) together with other intertwined local orders characterize the ground state. Here we show that the $T$-linear resistivity of highly strained, ultrathin and underdoped YBa$_2$Cu$_3$O$_{7-δ}$ films is restored when the CDW amplitude, detected by Resonant Inelastic X-ray scattering, is suppressed. This observation points towards an intimate connection between the onset of CDW and the departure from $T$-linear resistivity in underdoped cuprates. Our results illustrate the potential of using strain control to manipulate the ground state of quantum materials.

cond-mat.supr-con↗

arXiv2021

Coexistence of ferromagnetism and spin-orbit coupling by incorporation of platinum in two-dimensional VSe$_2$

We report on a novel material, namely two-dimensional (2D) V$_{1-x}$Pt$_x$Se$_2$ alloy, exhibiting simultaneously ferromagnetic order and Rashba spin-orbit coupling. While ferromagnetism is absent in 1T-VSe$_2$ due to the competition with the charge density wave phase, we demonstrate theoretically and experimentally that the substitution of vanadium by platinum in VSe$_2$ (10-50 %) to form an homogeneous 2D alloy restores ferromagnetic order with Curie temperatures of 6 K for 5 monolayers and 25 K for one monolayer of V$_{0.65}$Pt$_{0.35}$Se$_2$. Moreover, the presence of platinum atoms gives rise to Rashba spin-orbit coupling in (V,Pt)Se$_2$ providing an original platform to study the interplay between ferromagnetism and spin-orbit coupling in the 2D limit.

cond-mat.mtrl-sci↗