arXiv subjects

M. -H. Julien

Publications and source records attributed to M. -H. Julien.

At least 19 recordsLinked to original sources

arXiv2026

Singular spin fluctuations in the strange-metal phase of La2-xSrxCuO4

Although spin fluctuations are central to the physics of high-Tc cuprates, their relevance to strange-metal behavior in the overdoped regime remains unclear. Here, we use high magnetic fields to suppress superconductivity and an NMR protocol tailored to electronic inhomogeneity to show that the low-energy limit of the dynamical spin susceptibility χ''(q,omega) at x=0.25 in La2-xSrxCuO4 increases continuously down to our lowest temperatures. This behavior is suggestive of quantum-critical fluctuations, a leading candidate mechanism for strange-metal transport, yet is observed well beyond the spin-stripe critical doping x=0.19. Our data further reveal that the spin dynamics are spatially inhomogeneous, suggesting that nanoscale electronic inhomogeneity may underlie this apparent paradox. These observations provide new insight into the electronic state from which strange-metal behavior emerges.

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arXiv2026

Stabilization of a non-superconducting, orthorhombic phase by over-hydrogenating LaFeSiH

Chemical composition provides a powerful route to tune the electronic ground state of iron-based superconductors and other quantum materials, yet access to highly doped phases remains limited. Here we demonstrate that high-pressure thermal decomposition of hydrogen-rich precursors enables over-hydrogenation of LaFeSi. Using anthracene, we synthesize tetragonal superconducting LaFeSiH, including a single hydrogen site, while ammonia borane yields a structurally distorted over-hydrogenated phase, LaFeSiH1+x, with an orthorhombic structure. Chemical analysis reveal excess hydrogen (x ~ 0.6), implying a second H site in LaFeSiH1.6 whose localization and occupancy are determined by neutron diffraction. In contrast to metallic LaFeSi and superconducting LaFeSiH, orthorhombic LaFeSiH1.6 exhibits semiconductor-like behavior. Upon hydrogen release near 100 °C, it transforms into tetragonal superconducting LaFeSiH1+δ (δ << 0.6). These results establish the chemical flexibility of the layered LaFeSiX (X = H, O, F) family and provide access to a high hydrogen-doping regime, creating new opportunities to investigate superconductivity in Fe-based silicides.

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arXiv2025

Spin-stripe order tied to the pseudogap phase in La1.8-xEu0.2SrxCuO4

Although spin and charge stripes in high-Tc cuprates have been extensively studied, the exact range of carrier concentration over which they form a static order remains uncertain, complicating efforts to understand their significance. In La2-xSrxCuO4 (LSCO) and in zero external magnetic field, static spin stripes are confined to a doping range well below p*, the pseudogap boundary at zero temperature. However, when high fields suppress the competing effect of superconductivity, spin stripe order is found to extend up to p*. Here, we investigated La1.8-xEu0.2SrxCuO4 (Eu-LSCO) using 139La nuclear magnetic resonance and observe field-dependent spin fluctuations suggesting a similar competition between superconductivity and spin order as in LSCO. Nevertheless, we find that static spin stripes are present practically up to p* irrespective of field strength: the stronger stripe order in Eu-LSCO prevents superconductivity from enforcing a non-magnetic ground state, except very close to p*. Thus, spin-stripe order is consistently bounded by p* in both LSCO and Eu-LSCO, despite their differing balances between stripe order and superconductivity. This indicates that the canonical stripe order, where spins and charges are intertwined in a static pattern, is fundamentally tied to the pseudogap phase, though the exact nature of this connection has yet to be elucidated. Any stripe order beyond the pseudogap endpoint must then be of a different nature: either spin and charge orders remain intertwined, but both fluctuating, or only spin order fluctuates while charge order remains static. The presence of spin-stripe order up to p*, the pervasive, slow, and field-dependent spin-stripe fluctuations, as well as the electronic inhomogeneity documented in this work, must all be carefully considered in discussions of Fermi surface transformations, quantum criticality, and strange metal behavior.

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arXiv2025

Signatures of two gaps in the spin susceptibility of a cuprate superconductor

A major obstacle to understanding high-Tc cuprates is that superconductivity precludes observing normal-state properties at low temperatures. One prime example is the normal-state spin susceptibility \c{hi}spin: although its decrease upon cooling far above Tc typifies pseudogap behavior, its behavior at low temperatures is generally unknown. Here, our measurements in high magnetic fields expose \c{hi}spin of YBa2Cu3Oy down to low temperatures. Even though superconductivity is suppressed by the field, we uncover two thermally-activated contributions alongside a residual \c{hi}spin(T=0) due to gapless excitations. We relate these two distinct gaps to short-range charge-density waves and to the formation of singlets as in certain quantum spin systems. Both phenomena thus contribute to the pseudogap at low temperature, supplementing short-lived antiferromagnetism that initiates pseudogap behavior at high temperatures. We therefore propose that the pseudogap ought to be regarded as a composite property and that, when not undergoing spin-stripe ordering, underdoped cuprates tend to form short-ranged spin singlets.

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arXiv2023

Magnetic and structural properties of the iron silicide superconductor LaFeSiH

The magnetic and structural properties of the recently discovered pnictogen/chalcogen-free superconductor LaFeSiH ($T_c\simeq10$~K) have been investigated by $^{57}$Fe synchrotron M{ö}ssbauer source (SMS) spectroscopy, x-ray and neutron powder diffraction and $^{29}$Si nuclear magnetic resonance spectroscopy (NMR). No sign of long range magnetic order or local moments has been detected in any of the measurements and LaFeSiH remains tetragonal down to 2 K. The activated temperature dependence of both the NMR Knight shift and the relaxation rate $1/T_1$ is analogous to that observed in strongly overdoped Fe-based superconductors. These results, together with the temperature-independent NMR linewidth, show that LaFeSiH is an homogeneous metal, far from any magnetic or nematic instability, and with similar Fermi surface properties as strongly overdoped iron pnictides. This raises the prospect of enhancing the $T_c$ of LaFeSiH by reducing its carrier concentration through appropriate chemical substitutions. Additional SMS spectroscopy measurements under hydrostatic pressure up to 18.8~GPa found no measurable hyperfine field.

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arXiv2022

Competition between spin ordering and superconductivity near the pseudogap boundary in La2-xSrxCuO4: insights from NMR

When superconductivity is suppressed by high magnetic fields in La2-xSrxCuO4, striped antiferromagnetic (AFM) order becomes the magnetic ground state of the entire pseudogap regime, up to its end at the doping p* [M. Frachet, I. Vinograd et al., Nat. Phys. 16, 1064 (2020)]. Glass-like freezing of this state is detected in 139La NMR measurements of the spin-lattice relaxation rate 1/T1. Here, we present a quantitative analysis of 1/T1 data in the hole-doping range p=x=0.12-0.171, based on the Bloembergen-Purcell-Pound (BPP) theory, modified to include statistical distribution of parameters arising from strong spatial inhomogeneity. We observe spin fluctuations to slow down at temperatures T near the onset of static charge order and, overall, the effect of the field B may be seen as equivalent to strengthening stripe order by approaching p=0.12 doping. In details however, our analysis reveals significant departure from usual field-induced magnetic transitions. The continuous growth of the amplitude of the fluctuating moment with increasing B suggests a nearly-critical state in the B->0 limit, with very weak quasi-static moments possibly confined in small areas like vortex cores. Further, the nucleation of spin order in the vortex cores is shown to account quantitatively for both the value and the p dependence of a field scale characterizing bulk spin freezing. The correlation time of the fluctuating moment appears to depend exponentially on B/T (over the investigated range). This explains the timescale dependence of various experimental manifestations, including why, for transport measurements, the AFM moments may be considered static over a considerable range of B and T. These results make the high-field magnetic ground state up to p* an integral part of the discussion on putative quantum criticality.

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arXiv2022

Superconductivity in the crystallogenide LaFeSiO$_{1-δ}$ with squeezed FeSi layers

Pnictogens and chalcogens are both viable anions for promoting Fe-based superconductivity and intense research activity in the related families has established systematic correlation between the Fe-anion height and the superconducting critical temperature $T_c$, with an optimum Fe-anion height of $\sim$ 1.38 Å. Here, we report the discovery of superconductivity in a novel compound LaFeSiO$_{1-δ}$ that incorporates a crystallogen element, Si, and challenges the above picture: considering the strongly squeezed Fe-Si height of 0.94 Å, the superconducting transition at $T_{c}$ = 10 K is unusually high. In the normal state, the resistivity displays non-Fermi-liquid behavior while NMR experiments evidence weak antiferromagnetic fluctuations. According to first-principles calculations, the Fermi surface of this material is dominated by hole pockets without nesting properties, which explains the strongly suppressed tendency towards magnetic order and suggests that the emergence of superconductivity materializes in a distinct set-up, as compared to the standard $s_\pm$- and $d$-wave electron-pocket-based situations. These properties and its simple-to-implement synthesis make LaFeSiO$_{1-δ}$ a particularly promising platform to study the interplay between structure, electron correlations and superconductivity.

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arXiv2021

Locally commensurate charge-density wave with three-unit-cell periodicity in YBCO

In order to identify the mechanism responsible for the formation of charge-density waves (CDW) in cuprate superconductors, it is important to understand which aspects of the CDW's microscopic structure are generic and which are material-dependent. Here, we show that, at the local scale probed by NMR, long-range CDW order in YBa2Cu3Oy is unidirectional with a commensurate period of three unit cells (lambda = 3b), implying that the incommensurability found in X-ray scattering is ensured by phase slips (discommensurations). Furthermore, NMR spectra reveal a predominant oxygen character of the CDW with an out-of-phase relationship between certain lattice sites but no specific signature of a secondary CDW with lambda = 6b associated with a putative pair-density wave. These results shed light on universal aspects of the cuprate CDW. In particular, its spatial profile appears to generically result from the interplay between an incommensurate tendency at long length scales, possibly related to properties of the Fermi surface, and local commensuration effects, due to electron-electron interactions or lock-in to the lattice.

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arXiv2020

High magnetic field ultrasound study of spin freezing in La$_{1.88}$Sr$_{0.12}$CuO$_4$

High-$T_{\rm{c}}$ cuprate superconductors host spin, charge and lattice instabilities. In particular, in the antiferromagnetic glass phase, over a large doping range, lanthanum based cuprates display a glass-like spin freezing with antiferromagnetic correlations. Previously, sound velocity anomalies in La$_{2-x}$Sr$_{x}$CuO$_4$ (LSCO) for hole doping $p\geq 0.145$ were reported and interpreted as arising from a coupling of the lattice to the magnetic glass [Frachet, Vinograd et al., Nat. Phys. 16, 1064-1068 (2020)]. Here we report both sound velocity and attenuation in LSCO $p=0.12$, i.e. at a doping level for which the spin freezing temperature is the highest. Using high magnetic fields and comparing with nuclear magnetic resonance (NMR) measurements, we confirm that the anomalies in the low temperature ultrasound properties of LSCO are produced by a coupling between the lattice and the spin glass. Moreover, we show that both sound velocity and attenuation can be simultaneously accounted for by a simple phenomenological model originally developed for canonical spin glasses. Our results point towards a strong competition between superconductivity and spin freezing, tuned by the magnetic field. A comparison of different acoustic modes suggests that the slow spin fluctuations have a nematic character.

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arXiv2020

Singular magnetic anisotropy in the nematic phase of FeSe

FeSe is arguably the simplest, yet the most enigmatic, iron-based superconductor. Its nematic but non-magnetic ground state is unprecedented in this class of materials and stands out as a current puzzle. Here, our NMR measurements in the nematic state of mechanically detwinned FeSe reveal that both the Knight shift and the spin-lattice relaxation rate 1/T_1 possess an in-plane anisotropy opposite to that of the iron pnictides LaFeAsO and BaFe2As2. Using a microscopic electron model that includes spin-orbit coupling, our calculations show that an opposite quasiparticle weight ratio between the d_xz and d_yz orbitals leads to an opposite anisotropy of the orbital magnetic susceptibility, which explains our Knight shift results. We attribute this property to a different nature of nematic order in the two compounds, predominantly bond-type in FeSe and onsite ferro-orbital in pnictides. The T_1 anisotropy is found to be inconsistent with existing neutron scattering data in FeSe, showing that the spin fluctuation spectrum reveals surprises at low energy, possibly from fluctuations that do not break C_4 symmetry. Therefore, our results reveal that important information is hidden in these anisotropies and they place stringent constraints on the low-energy spin correlations as well as on the nature of nematicity in FeSe.

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arXiv2019

NMR study of charge density waves under hydrostatic pressure in YBa2Cu3Oy

The effect of hydrostatic pressure (P) on charge density waves (CDW) in YBa2Cu3Oy has recently been controversial. Using NMR, we find that both the short-range CDW in the normal state and the long-range CDW in high fields are, at most, slightly weakened at P=1.9 GPa. This result is in contradiction with x-ray scattering results finding complete suppression of the CDW at ~1 GPa and we discuss possible explanations of this discrepancy. Quantitative analysis, however, shows that the NMR data is not inconsistent with a disappearance of the CDW on a larger pressure scale, typically ~10-20 GPa. We also propose a simple model reconciling transport data with such a hypothesis, provided the pressure-induced change in doping is taken into account. We conclude that it is therefore possible that most of the spectacular increase in Tc upon increasing pressure up to ~15~GPa arises from a concomitant decrease of CDW strength.

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arXiv2018

Intimate link between Charge Density Wave, Pseudogap and Superconducting Energy Scales in Cuprates

The cuprate high temperature superconductors develop spontaneous charge density wave (CDW) order below a temperature $T_{CDW}$ and over a wide range of hole doping (p). An outstanding challenge in the field is to understand whether this modulated phase is related to the more exhaustively studied pseudogap and superconducting phases. To address this issue it is important to extract the energy scale $Δ_{CDW}$ associated with the charge modulations, and to compare it with the pseudogap (PG) $Δ_{PG}$ and the superconducting gap $Δ_{SC}$. However, while $T_{CDW}$ is well-characterized from earlier works little has been known about $Δ_{CDW}$ until now. Here, we report the extraction of $Δ_{CDW}$ for several cuprates using electronic Raman spectroscopy. Crucially, we find that, upon approaching the parent Mott state by lowering $p$, $Δ_{CDW}$ increases in a manner similar to the doping dependence of $Δ_{PG}$ and $Δ_{SC}$. This shows that CDW is an unconventional order, and that the above three phases are controlled by the same electronic correlations. In addition, we find that $Δ_{CDW} \approx Δ_{SC}$ over a substantial doping range, which is suggestive of an approximate emergent symmetry connecting the charge modulated phase with superconductivity.

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arXiv2018

Unusual interplay between superconductivity and field-induced charge order in YBa2Cu3Oy

We present a detailed study of the temperature (T) and magnetic field (H) dependence of the electronic density of states (DOS) at the Fermi level, as deduced from specific heat and Knight shift measurements in underdoped YBa2Cu3Oy. We find that the DOS becomes field-independent above a characteristic field H_{DOS} and that the H_{DOS}(T) line displays an unusual inflection near the onset of the long range 3D charge-density wave order. The unusual S-shape of H_{DOS}(T) is suggestive of two mutually-exclusive orders that eventually establish a form of cooperation in order to coexist at low T. On theoretical grounds, such a collaboration could result from the stabilisation of a pair-density wave state, which calls for further investigations in this region of the phase diagram

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arXiv2017

Spin susceptibility of charge ordered YBa2Cu3Oy across the upper critical field

The value of the upper critical field Hc2, a fundamental characteristic of the superconducting state, has been subject to strong controversy in high-Tc copper-oxides. Since the issue has been tackled almost exclusively by macroscopic techniques so far, there is a clear need for local-probe measurements. Here, we use 17O NMR to measure the spin susceptibility $χ_{spin}$ of the CuO2 planes at low temperature in charge ordered YBa2Cu3Oy. We find that $χ_{spin}$ increases (most likely linearly) with magnetic field H and saturates above field values ranging from 20 to 40 T. This result is consistent with Hc2 values claimed by G. Grissonnanche et al. [Nat. Commun. 5, 3280 (2014)] and with the interpretation that the charge-density-wave (CDW) reduces Hc2 in underdoped YBa2Cu3Oy. Furthermore, the absence of marked deviation in $χ_{spin}(H)$ at the onset of long-range CDW order indicates that this Hc2 reduction and the Fermi-surface reconstruction are primarily rooted in the short-range CDW order already present in zero field, not in the field-induced long-range CDWorder. Above Hc2, the relatively low values of $χ_{spin}$ at T=2 K show that the pseudogap is a ground-state property, independent of the superconducting gap.

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arXiv2016

Observation of electronic bound states in charge-ordered YBa$_2$Cu$_3$O$_y$

Observing how electronic states in solids react to a local symmetry breaking provides insight into their microscopic nature. A striking example is the formation of bound states when quasiparticles are scattered off defects. This is known to occur, under specific circumstances, in some metals and superconductors but not, in general, in the charge-density-wave (CDW) state. Here, we report the unforeseen observation of bound states when a magnetic field quenches superconductivity and induces long-range CDW order in YBa$_2$Cu$_3$O$_y$. Bound states indeed produce an inhomogeneous pattern of the local density of states $N(E_F)$ that leads to a skewed distribution of Knight shifts which is detected here through an asymmetric profile of $^{17}$O NMR lines. We argue that the effect arises most likely from scattering off defects in the CDW state, which provides a novel case of disorder-induced bound states in a condensed-matter system and an insightful window into charge ordering in the cuprates.

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arXiv2016

Cu-NMR study of oxygen disorder in ortho-II YBa2Cu3Oy

We show that 63Cu NMR spectra place strong constraints on both the nature and the concentration of oxygen defects in ortho-II YBa2Cu3Oy. Systematic deviation from ideal ortho-II order is revealed by the presence of inequivalent Cu sites in either full or empty chains. The results can be explained by two kinds of defects: oxygen clustering into additional chains, or fragments thereof, most likely present at all concentrations (6.4<y<6.6) and oxygen vacancies randomly distributed in the full chains for y<6.50 only. Furthermore, the remarkable reproducibility of the spectra in different samples with optimal ortho-II order (y=6.55) shows that chain-oxygen disorder, known to limit electronic coherence, is ineluctable because it is inherent to these compounds.

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arXiv2015

Incipient charge order observed by NMR in the normal state of YBa2Cu3Oy

The pseudogap regime of high-temperature cuprates harbours diverse manifestations of electronic ordering whose exact nature and universality remain debated. Here, we show that the short-ranged charge order recently reported in the normal state of YBa2Cu3Oy corresponds to a truly static modulation of the charge density. We also show that this modulation impacts on most electronic properties, that it appears jointly with intra-unit-cell nematic, but not magnetic, order, and that it exhibits differences with the charge density wave observed at lower temperatures in high magnetic fields. These observations prove mostly universal, they place new constraints on the origin of the charge density wave and they reveal that the charge modulation is pinned by native defects. Similarities with results in layered metals such as NbSe2, in which defects nucleate halos of incipient charge density wave at temperatures above the ordering transition, raise the possibility that order-parameter fluctuations, but no static order, would be observed in the normal state of most cuprates if disorder were absent.

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arXiv2013

Emergence of charge order from the vortex state of a high temperature superconductor

Evidence is mounting that charge order competes with superconductivity in high Tc cuprates. Whether this has any relationship to the pairing mechanism is unknown since neither the universality of the competition nor its microscopic nature has been established. Here using nuclear magnetic resonance, we show that, similar to La214, charge order in YBCO has maximum strength inside the superconducting dome, at doping levels p = 0.11 - 0.12.We further show that the overlap of halos of incipient charge order around vortex cores, similar to those visualised in Bi2212, can explain the threshold magnetic field at which long-range charge order emerges. These results reveal universal features of a competition in which charge order and superconductivity appear as joint instabilities of the same normal state, whose relative balance can be field-tuned in the vortex state.

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