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Marie-Aude Méasson

Publications and source records attributed to Marie-Aude Méasson.

At least 19 recordsLinked to original sources

Paramagnon softening upon doping in oxychloride cuprate superconductors

Understanding how magnetic excitations and exchange interactions evolve with doping is crucial for deciphering the physics that shapes the phase diagram of high-temperature cuprate superconductors. Here, we clearly determine the behavior of the paramagnon dispersion in the oxychloride cuprate Na$_{x}$Ca$_{2-x}$CuO$_2$Cl$_2$ up to the highest doping level. We find that the paramagnon bandwidth, defined by the energy at the $X$ zone boundary $(0.5,0,0)$, remains unchanged within experimental uncertainty, even though it exhibits significant broadening. In contrast, along the nodal direction $Γ-M$ (\textit{i.e.}, from $(0,0,0)$ to $(0.5,0.5,0)$), the paramagnon energy shows a marked softening with doping, with a shift of up to $ΔE\sim150$ meV at the midpoint of the zone for the highest doping, which is about half of its initial value in the antiferromagnetic phase. Calculations of the dynamical spin structure factor for a one-band Hubbard model, including hopping terms up to the third-nearest neighbor ($t^{\prime\prime}$), explain this behavior and accurately reproduce the observed wave vector dependence and directional variation in the Brillouin zone.

cond-mat.supr-con↗

Enhanced Charge-Density-Wave Order and Suppressed Superconductivity in Intercalated Bulk $\mathrm{Nb}{\mathrm{Se}}_{2}$

The electronic ground states of transition-metal dichalcogenides are strongly shaped by reduced dimensionality, yet the properties of atomically thin layers remain difficult to probe due to their small size and environmental sensitivity. Here we demonstrate that controlled electrochemical intercalation of organic cations provides a robust bulk platform for accessing monolayer-like physics in NbSe$_2$. Intercalation of tetrapropylammonium and tetrabutylammonium expands the interlayer spacing by nearly a factor of two, electronically decoupling the NbSe$_2$ layers while simultaneously introducing well-defined charge doping. Using a combination of Raman spectroscopy, scanning tunneling microscopy, X-ray diffraction, and photoemission, we uncover a pronounced enhancement of the charge-density-wave transition temperature to $\sim 130$ K together with a strong suppression of superconductivity, reproducing the phase diagram observed in exfoliated monolayers. The enhanced charge-density-wave order and reduced $T_c$ arise from the combined effects of dimensionality reduction and electron injection, and are accompanied by distinct dip-hump anomalies in the tunneling spectra suggestive of collective mode excitations. Our results establish molecular intercalation as a powerful and scalable route for engineering competing orders in layered quantum materials.

cond-mat.supr-con↗

Ising superconductivity in noncentrosymmetric bulk NbSe2

Ising superconductivity allows in-plane upper critical magnetic fields to vastly surpass Pauli limit by locking the antiparallel electron spins of Cooper pairs in the out-of-plane direction. It was first explicitly demonstrated in fully two-dimensional monolayers of transition metal dichalcogenides with large spin-orbit coupling and broken inversion symmetry. Since then, several studies have shown that it can be present in layered bulk materials, too. In our previous study, we have clarified the underlying microscopic mechanism of Ising superconductivity in bulk, based on a reduced electronic coupling between superconducting layers due to intercalation by insulating layers and restricted inversion symmetry. But earlier studies suggest that in some transition metal dichalcogenide polytypes Pauli paramagnetic limit is violated even without intercalation. Here, using heat capacity measurements we unambiguously demonstrate, that the pristine noncentrosymmetric bulk 4Ha-NbSe2 polytype significantly violates the Pauli limit. The band structure parameters obtained from ab initio calculations using the experimentally determined crystal structure are used in the theoretical model which provides the microscopic mechanism of the Ising protection based solely on broken inversion symmetry.

cond-mat.supr-con↗

Multilayer Crystal Field states from locally broken centrosymmetry

Local charge, spin, or orbital degrees of freedom with intersite interactions are oftentimes sufficient to construct most quantum orders. This is conventionally true for f-electron systems, where the extent of the f-electrons and their associated crystal-electric-field (CEF) states are strongly localized. Here, polarized Raman spectroscopy measurements of a locally non-centrosymmetric compound, CeCoSi, unveil more CEF excitations than expected in the local model. We interpret this as experimental evidence for the entanglement of CEF states between cerium layers. This composite sublattice, spin, and orbital degree of freedom provides an unconsidered means to form novel orders, not only in this system, but in any system exhibiting globally preserved yet locally broken centrosymmetry.

cond-mat.str-el↗

Easy-plane ferromagnetic ordering and crystal-field ground state in the Kondo lattice CeCuSi

We report the successful growth of CeCuSi single crystals using a metallic flux method and the physical properties using structural, magnetic, electrical transport, optical, and heat capacity measurements. CeCuSi crystallizes in a hexagonal-bar shape, and single crystal x-ray diffraction confirms the ZrBeSi-type structure (space group $P6_{3}/mmc$). CeCuSi orders ferromagnetically below $T_\textrm{C}=15.5$ K with easy magnetization direction within the basal plane. The Ce$^{3+}$ ions are situated within a triangular lattice with a point group of $D_{3d}$. We perform a detailed crystalline electric field (CEF) analysis of the anisotropic magnetic susceptibility, the Schottky anomaly in heat capacity, and the Raman-active excitations. The results indicate a ground state doublet with magnetic moment primarily in the basal plane, and a ferromagnetic interaction along both directions. The exponential behavior in resistivity and in heat capacity below $T_\textrm{C}$ can also be well explained by the ferromagnetic magnon model. We found that CeCuSi does not exhibit the CEF hard axis ordering observed in many ferromagnetic Kondo lattice (FM-KL) compounds. Our CEF analysis suggests that the exchange interactions along both axes are ferromagnetic, potentially explaining the absence of hard-axis ordering.

cond-mat.str-el↗

NbSe$_{2}$'s charge density wave collapse in the (LaSe)$_{1.14}$(NbSe$_{2}$)$_{2}$ misfit layer compound

Misfit layer compounds, heterostructures composed by a regular alternating stacking of rocksalt monochalcogenides bilayers and few-layer transition metal dichalchogenides, are an emergent platform to investigate highly doped transition metal dichalcogenides. Among them, (LaSe)$_{1.14}$(NbSe$_2$)$_2$ displays Ising superconductivity, while the presence of a charge density wave (CDW) in the material is still under debate. Here, by using polarized Raman spectroscopy and first-principles calculations, we show that NbSe$_2$ undergoes a doping-driven collapse of the CDW ordering within the misfit, and no signature of the CDW is detected down to 8~K. We provide a complete experimental and theoretical description of the lattice dynamics of this misfit compound. We show that the vibrational properties are obtained from those of the two subunits, namely the LaSe unit and the NbSe$_2$ bilayer, in the presence of a suitable field-effect doping, and then highlight the 2D nature of the lattice dynamics of NbSe$_2$ within the (LaSe)$_{1.14}$(NbSe$_2$)$_2$ 3D structure.

cond-mat.mtrl-sci↗

Lattice dynamics in the FeSi-based family of superconductors

The lattice dynamics of the superconducting materials LaFeSiH and LaFeSiO as well as their intermetallic precursor LaFeSi are investigated by polarized Raman spectroscopy and first-principles calculations, together with X-ray and advanced electron diffraction techniques for their structural analysis. We find that the Fe-dominated Raman-active modes reflect the chemical peculiarities of these silicides compared to their pnictide counterparts, with enhanced structural couplings between the FeSi layer and the spacer that can be related to the ionic vs covalent character of the latter. In addition, we find signatures of enhanced electron-phonon coupling for some of the Raman-active modes. Beyond that, our study reveals intriguing Fe-based Raman features as well as structural subtleties in LaFeSiH suggesting that this superconductor may formally be non-centrosymmetric.

cond-mat.supr-con↗

Pressure-induced formation of cubic lutetium hydrides derived from trigonal LuH$_3$

In recent years, there has been a fervent search for room-temperature superconductivity within the binary hydrides. However, as the number of untested compounds dwindled, it became natural to begin searching within the ternary hydrides. This led to the controversial discovery of room-temperature superconductivity at only 1GPa in nitrogen-doped lutetium hydride [Dasenbrock-Gammon et al., Nature 615, 244 (2023)] and consequently provided much impetus for the synthesis of nitrogen-based ternary hydrides. Here, we report the synthesis of stable trigonal LuH$_3$ by hydrogenating pure lutetium which was subsequently pressurised to $\sim$2GPa in a dilute-N$_2$/He-rich pressure medium. Raman spectroscopy and x-ray diffraction were used to characterise the structures throughout. After depressurising, energy-dispersive and wavelength-dispersive X-ray spectroscopies characterised the final compound. Though our compound under pressure exhibits similar structural behaviour to the Dasenbrock-Gammon et al. sample, we do not observe any nitrogen within the structure of the recovered sample at ambient pressure. We observe two cubic structures under pressure that simultaneously explain the X-ray diffraction and Raman spectra observed: the first corresponds well to $Fm\overline{3}m$ LuH$_{2+x}$, whilst the latter is an $Ia\overline{3}$-type structure.

cond-mat.supr-con↗

Possible high temperature superconducting transitions in disordered graphite obtained from room temperature deintercalated KC$_8$

Although progress with twisted graphene nano-devices is boosting the superconductivity that is the consequence of their Moiré flat electronic bands, the immense choice for future development is an obstacle for their optimisation. We report here that soft-chemistry deintercalation of KC$_8$ breaks down graphite stacking generating a strong disorder that includes stacking twists and variable local doping. We obtain a bulk graphite whose individual crystallites have different stackings with arbitrary twists and doping, scanning in the same sample a huge number of stacking configurations. We perform magnetisation measurements on batches with different synthesis conditions. The disorder weakens the huge diamagnetism of graphite, revealing several phase transitions. A "ferromagnetic-like" magnetisation appears with Curie temperatures T$_0$$\sim$450K, that has to be subtracted from the measured magnetisation. Depending on sample synthesis, anomalies towards diamagnetic states appear at T$_c$$\sim$110K (3 samples), $\sim$240K (4 samples), $\sim$320K (2 samples). Electrical resistivity measurements yield anomalies for the T$_c\sim$240K transition, with one sample showing a 90% drop. We discuss the possibility that these (diamagnetic and resistitive) anomalies could be due to superconductivity.

cond-mat.supr-con↗

Effective model for $A_{2g}$ Raman signal in URu$_2$Si$_2$

We propose an effective model to describe the $A_{2g}$ signal in Raman scattering experiments in the URu$_{2}$Si$_{2}$ compound. We follow the scheme proposed earlier by Khveshchenko and Wiegmann [Phys. Rev. Lett. 73, 500 (1994)] to calculate the $A_{2g}$ scattering vertex. We extract the imaginary part of a two-point current-current correlation function and compare it directly with the Raman response. We obtain an inelastic peak at $A_{2g}$ channel owing to the interplay between a local staggered ordering and a possible quantum spin liquid behavior. Our results offer an explanation for the electronic Raman scattering experiments at the hidden order phase in URu$_{2}$Si$_{2}$ compound [Phys. Rev. Lett. 113, 266405 (2014)].

cond-mat.str-el↗

Raman Scattering as a Selective Probe of Chiral Electronic Excitations in Bilayer Graphene

We report a symmetry resolved electronic Raman scattering (ERS) study of a bilayer graphene device under gate voltage. We show that the ERS continuum is dominated by interband chiral excitations of $A_{2}$ symmetry and displays a characteristic Pauli-blocking behavior similar to the monolayer case. Crucially, we show that non-chiral excitations make a vanishing contribution to the Raman cross-section due to destructive interference effects in the Raman amplitude matrix elements. This is in a marked contrast to optical absorption measurements and opens interesting venues for the use of Raman scattering as a selective probe of chiral degrees of freedom in topological matter and other 2D crystals.

cond-mat.mes-hall↗

Pressure induced collapse of the charge density wave and Higgs mode visibility in 2H-TaS$_2$

The pressure evolution of the Raman active electronic excitations of the transition metal dichalcogenides 2H-TaS$_2$ is followed through the pressure phase diagram embedding incommensurate charge-density-wave and superconducting states. At high pressure, the charge-density-wave is found to collapse at 8.5~GPa. In the coexisting charge-density-wave and superconducting orders, we unravel a strong in-gap superconducting mode, attributed to a Higgs mode, coexisting with the expected incoherent Cooper-pair breaking signature. The latter remains in the pure superconducting state reached above 8.5~GPa. Our report constitutes the first observation of such Raman active Higgs mode since the longstanding unique case 2H-NbSe$_2$.

cond-mat.supr-con↗

Collapse of critical nematic fluctuations in FeSe under pressure

We report the evolution of the electronic nematic susceptibility in FeSe via Raman scattering as a function of hydrostatic pressure up to 5.8 GPa where the superconducting transition temperature $T_{c}$ reaches its maximum. The critical nematic fluctuations observed at low pressure vanish above 1.6 GPa, indicating they play a marginal role in the four-fold enhancement of $T_{c}$ at higher pressures. The collapse of nematic fluctuations appears to be linked to a suppression of low energy electronic excitations which manifests itself by optical phonon anomalies at around 2 GPa, in agreement with lattice dynamical and electronic structure calculations using local density approximation combined with dynamical mean field theory. Our results reveal two different regimes of nematicity in the phase diagram of FeSe under pressure: a d-wave Pomeranchuk instability of the Fermi surface at low pressure and a magnetic driven orthorhombic distortion at higher pressure.

cond-mat.supr-con↗

Higgs-mode radiance and charge-density-wave order in 2H-NbSe$_2$

Despite being usually considered two competing phenomena, charge-density-wave and superconductivity coexist in few systems, the most emblematic one being the transition metal dichalcogenide 2H-NbSe$_2$. This unusual condition is responsible for specific Raman signatures across the two phase transitions in this compound. While the appearance of a soft phonon mode is a well-established fingerprint of the charge-density-wave order, the nature of the sharp sub-gap mode emerging below the superconducting temperature is still under debate. In this work we use the external pressure as a knob to unveil the delicate interplay between the two orders, and consequently the nature of the superconducting mode. Thanks to an advanced extreme-conditions Raman technique we are able to follow the pressure evolution and the simultaneous collapse of the two intertwined charge density wave and superconducting modes. The comparison with microscopic calculations in a model system supports the Higgs-type nature of the superconducting mode and suggests that charge-density-wave and superconductivity in 2H-NbSe$_2$ involve mutual electronic degrees of freedom. These findings fill knowledge gap on the electronic mechanisms at play in transition metal dichalcogenides, a crucial step to fully exploit their properties in few-layers systems optimized for devices applications.

cond-mat.supr-con↗

Raman Active High Energy Excitations in URu$_2$Si$_2$

We have performed Raman scattering measurements on URu$_2$Si$_2$ single crystals on a large energy range up to $\sim$ 1300 cm$^{-1}$ and in all the Raman active symmetries as a function of temperature down to 15 K. A large excitation, active only in the E$_{g}$ symmetry, is reported. It has been assigned to a crystal electric field excitation on the Uranium site. We discuss how this constrains the crystal electric field scheme of the Uranium ions. Furthermore, three excitations in the A$_{1g}$ symmetry are observed. They have been associated to double Raman phonon processes consistently with ab initio calculations of the phonons dispersion.

cond-mat.str-el↗

Damping and non-linearity of a levitating magnet in rotation above a superconductor

We study the dissipation of moving magnets in levitation above a superconductor. The rotation motion is analyzed using optical tracking techniques. It displays a remarkable regularity together with long damping time up to several hours. The magnetic contribution to the damping is investigated in detail by comparing 14 distinct magnetic configurations, and points towards amplitude-dependent dissipation mechanisms. The non-linear dynamics of the mechanical rotation motion is also revealed and described with an effective Duffing model. The obtained picture of the coupling of levitating magnets to their environment sheds light on their potential as ultra-low dissipation mechanical oscillators for high precision physics.

cond-mat.mes-hall↗

Anharmonic suppression of Charge density wave in 2H-NbS$_2$

The temperature dependence of the phonon spectrum in the superconducting transition metal dichalcogenide 2H-NbS$_2$ is measured by diffuse and inelastic x-ray scattering. A deep, wide and strongly temperature dependent softening, of the two lowest energy longitudinal phonons bands, appears along the $\mathrm{ΓM}$ symmetry line in reciprocal space. In sharp contrast to the iso-electronic compounds 2H-NbSe$_2$, the soft phonons energies are finite, even at very low temperature, and no charge density wave instability occurs, in disagreement with harmonic ab-initio calculations. We show that 2H-NbS$_2$ is at the verge of the charge density wave transition and its occurrence is only suppressed by the large anharmonic effects. Moreover, the anharmonicity and the electron phonon coupling both show a strong in-plane anisotropy.

cond-mat.supr-con↗

Pseudogap in Cuprates by Electronic Raman Scattering

We present Raman experiments on underdoped and overdoped Bi2Sr2CaCu2O(8+d) (Bi-2212) single crystals. We reveal the pseudogap in the electronic Raman spectra in the B1g and B2g geometries. In these geometries we probe respectively, the antinodal (AN) and nodal (N) regions corresponding to the principal axes and the diagonal of the Brillouin zone. The pseudogap appears in underdoped regime and manifests itself in the B1g spectra by a strong depletion of the low energy electronic continuum as the temperature decreases. We define a temperature T* below which the depletion appears and the pseudogap energy, omegaPG the energy at which the depeletion closes. The pseudogap is also present in the B2g spectra but the depletion opens at higher energy than in the B1g spectra. We observe the creation of new electronic states inside the depletion as we enter the superconducting phase. This leads us to conclude (as proposed by S. Sakai et al.) that the pseudogap has a different structure than the superconducting gap and competes with it. We show that the nodal quasiparticle dynamic is very robust and almost insensitive to the pseudogap phase contrary to the antinodal quasiparticle dynamic. We finally reveal, in contrast to what it is usually admitted,an increase of the nodal quasiparticle spectral weight with underdoping. We interpret this result as the consequence of a possible Fermi surface disturbances in the doping range p=0.1-0.2.

cond-mat.supr-con↗