arXiv subjects

Alain Sacuto

Publications and source records attributed to Alain Sacuto.

At least 19 recordsLinked to original sources

arXiv2026

Unveiling the Interplay of Charge and Magnetic Excitations in HgBa$_2$Ca$_2$Cu$_3$O$_{8+\delta}$

Unraveling the mechanism that binds electrons into Cooper pairs in cuprate high-temperature superconductors remains one of the most fundamental challenges in condensed-matter physics. While both magnetic interactions and lattice vibrations are known to govern key electronic properties, their possible cooperation has never been directly observed. We investigate HgBa$_2$Ca$_2$Cu$_3$O$_{8+\delta}$ (Hg1223) - the cuprate with the highest $T_{\mathrm{c}}$ at ambient pressure - as a magnifying glass to probe the possible entwining of the excitations at the core of the pairing. Using resonant inelastic X-ray scattering, we find that the charge response is dominated by dynamic charge density fluctuations (CDF) extending up to several hundred meV, where magnetic excitations reside. At the same momentum where CDF are most intense, the paramagnon energy exhibits a pronounced softening, revealing a strong interplay among charge, lattice, and spin excitations. Our results point to a cooperative mechanism in which dynamic charge fluctuations mediate the coupling between lattice, charge and spin degrees of freedom-shedding new light on the fundamental origin of high-$T_{\mathrm{c}}$ superconductivity.

cond-mat.supr-con↗

arXiv2026

Revealing the nature of the charge density wave order of ErTe$_3$ via Raman scattering under anisotropic strain

The nature of the charge density wave (CDW) order of the rare-earth tritelluride ErTe3 is investigated by Raman scattering under anisotropic strain. The CDW state of ErTe3 is unconventional since it is accompanied by an unusual mirror symmetry breaking, whose origin remains to be understood. Studying the polarization-resolved Raman spectrum of the CDW amplitude mode as a function of strain and temperature, we find that the mirror symmetry breakings of the CDW state are not independent, arguing against the recently proposed ferro-axial multi-component CDW order. Instead, we show that a single component CDW order parameter with an ordering wavevector tilted away from the principle crystallographic axis can reproduce the observed mirror symmetry breakings and their manifestation in the Raman spectra.

cond-mat.str-el↗

arXiv2025

Photo-induced carrier dynamics in InSb probed with broadband THz spectroscopy based on BNA crystals

We report an optical pump - terahertz (THz) probe study of the photoinduced transient carrier dynamics in the low bandgap semiconductor Indium Antimonide (InSb). Using an organic N-benzyl-2-methyl-nitroaniline (BNA) crystal as a broadband THz source, we access the full spectral response over more than 5 THz, for varying pump-probe delay following the optical excitation. Using the Drude-Lorentz model accounting for differences between the excited length in material and the penetration depth of THz beam in pumped InSb, we extract the absolute carrier density as a function of the pump-probe delay, and provide insights on the diffusion length at given carrier densities, for different pump fluences. The mismatch between the THz penetration depth and the actual excited sample depth after carrier diffusion is discussed, since their evolutions with time and pump fluence are not intuitive as both quantities depend on carrier density.

cond-mat.mtrl-sci↗

arXiv2025

Ultrafast Raman probe of the photoinduced superconducting to normal state transition in the cuprate Bi$_2$Sr$_2$CaCu$_2$O$_{8+\delta}$

We report an ultrafast Time-Resolved Raman scattering study of the out-of-equilibrium photoinduced dynamics across the superconducting to normal state phase transition of the cuprate Bi$_2$Sr$_2$CaCu$_2$O$_{8+\delta}$. Using the polarization-resolved momentum space selectivity of Raman scattering, we track the superconducting condensate destruction and recovery dynamics with sub-picoseconds time resolution in the anti-nodal region of the Fermi surface where the superconducting gap is maximum. Leveraging ultrafast Raman thermometry, we find a significant dichotomy between the superconducting condensate and the quasiparticle temperature dynamics near the anti-nodes, which cannot be framed in terms of a single effective electron temperature. The present work demonstrates the ability of Time-Resolved Raman scattering to selectively probe out-of-equilibrium pathways of different electronic sub-degrees of freedom during a photoinduced phase transition.

cond-mat.supr-con↗

arXiv2022

Disentangling lattice and electronic instabilities in the excitonic insulator candidate Ta$_2$NiSe$_5$ by nonequilibrium spectroscopy

Ta$_2$NiSe$_5$ is an excitonic insulator candidate showing the semiconductor/semimetal-to-insulator (SI) transition below $T_{\text{c}}$ = 326 K. However, since a structural transition accompanies the SI transition, deciphering the role of electronic and lattice degrees of freedom in driving the SI transition has remained controversial. Here, we investigate the photoexcited nonequilibrium state in Ta$_2$NiSe$_5$ using pump-probe Raman and photoluminescence (PL) spectroscopies. The combined nonequilibrium spectroscopic measurements of the lattice and electronic states reveal the presence of a photoexcited metastable state where the insulating gap is suppressed, but the low-temperature structural distortion is preserved. We conclude that electron correlations play a vital role in the SI transition of Ta$_2$NiSe$_5$.

cond-mat.str-el↗

arXiv2021

Elastic and magnetoelastic properties of TbMnO3 single crystal by nanosecond time resolved acoustics and first-principles calculations

Time resolved pump and probe acoustics and first-principles calculations were employed to assess elastic properties of the TbMnO3 perovskite manganite having orthorhombic symmetry. Measuring sound velocities of bulk longitudinal and shear acoustic waves propagating along at least two different directions in the high symmetry planes (100), (010) and (001), provided a powerful mean to selectively determine the six diagonal elastic constants C11= 227 GPa, C22= 349 GPa, C33= 274 GPa, C44= 71 GPa, C55= 57 GPa, C66= 62 GPa. Among the three remaining off-diagonal ones, C23= 103 GPa was determined with a bissectrice direction. Density functional theory calculations with colinear spin-polarized provided complementary insights on their optical, elastic and magnetoelastic properties.

cond-mat.str-el↗

arXiv2021

Exploration of the Hg-based cuprate superconductors by Raman spectroscopy under hydrostatic pressure

The superconducting phase of the $\mathrm{HgBa}_2\mathrm{CuO}_{4+\delta}$ (Hg-1201) and $\mathrm{HgBa}_2\mathrm{Ca}_2\mathrm{Cu}_3\mathrm{O}_{8+\delta}$ (Hg-1223) cuprates has been investigated by Raman spectroscopy under hydrostatic pressure. Our analysis reveals that the increase of $T_c$ with pressure is slower in Hg-1223 cuprate compared to the Hg-1201 due to a charge carrier concentration imbalance (accentuated by pressure) between the $\mathrm{CuO}_2$ layers of Hg-1223. We find that the energy variation under pressure of the apical oxygen mode from which the charge carriers are transferred to the $\mathrm{CuO}_2$ layers, is the same for both the Hg-1223 and Hg-1223 cuprates and it is controlled by the inter-layer compressibility. At last, we show that the binding energy of the Cooper pairs related to the maximum amplitude of the $d-$ wave superconducting gap at the anti-nodes, does not follow $T_c$ with pressure. It decreases while $T_c$ increases. In the particular case of Hg-1201, the binding energy collapses from 10 to 2 $K_B T_c$ as the pressure increases up to 10 GPa. These direct spectroscopic observations joined to the fact that the binding energy of the Cooper pairs at the anti-nodes does not follow $T_c$ either with doping, raises the question of its link with the pseudogap energy scale which follows the same trend with doping.

cond-mat.supr-con↗

arXiv2021

Elastic properties assessment in the multiferroic BiFeO3 by pump and probe method

We have performed elasticity measurements in the bulk multiferroic BiFeO3 (BFO) using acoustical pump and probe spectroscopy. The sound velocities of the (quasi)-longitudinal and of the two (quasi)-transverse acoustic waves along three independent directions of the (110) surface have been measured. Moreover, one surface wave and one longitudinal wave propagating perpendicular to the surface have been detected. Based on initial input values of the six independent Cij elastic constants determined by our density functional theory calculations and our eleven experimental velocities, the numerical resolution of the acoustic equations allows to determine all the Cij elastic constants of BFO. The propagation direction dependence of volume and surface waves phase velocities allows the unambiguously assignment of the waves, hence the polarization of phonons.

cond-mat.str-el↗

arXiv2020

A switchable two-dimensional electron gas based on ferroelectric Ca:SrTiO$_3$

Two-dimensional electron gases (2DEGs) can form at the surface of oxides and semiconductors or in carefully designed quantum wells and interfaces. Depending on the shape of the confining potential, 2DEGs may experience a finite electric field, which gives rise to relativistic effects such as the Rashba spin-orbit coupling. Although the amplitude of this electric field can be modulated by an external gate voltage, which in turn tunes the 2DEG carrier density, sheet resistance and other related properties, this modulation is volatile. Here, we report the design of a ''ferroelectric'' 2DEG whose transport properties can be electrostatically switched in a non-volatile way. We generate a 2DEG by depositing a thin Al layer onto a SrTiO$_3$ single crystal in which 1 percent of Sr is substituted by Ca to make it ferroelectric. Signatures of the ferroelectric phase transition at 25 K are visible in the Raman response and in the temperature dependences of the carrier density and sheet resistance that shows a hysteretic dependence on electric field as a consequence of ferroelectricity. We suggest that this behavior may be extended to other oxide 2DEGs, leading to novel types of ferromagnet-free spintronic architectures.

cond-mat.mtrl-sci↗

arXiv2020

Impact of the surface phase transition on magnon and phonon excitations in BiFeO3 nanoparticles

We have performed Raman scattering measurements on BiFeO3 nanoparticles and studied both magnetic and lattice modes. We reveal strong anomalies between 140 K and 200 K in the frequency of magnon and E(LO1), E(TO1) and A1(LO1) phonon modes. These anomalies are related to a surface expansion and are enhanced for nanoparticle sizes approaching the spin cycloidal length. These observations point out the strong interplay between the surface, the lattice, and the magnetism for sizes of BiFeO3 nanoparticles close to the cycloid periodicity.

cond-mat.str-el↗

arXiv2019

Colossal electromagnon excitation in the non-cycloidal phase of TbMnO3 under pressure

The magnetoelectric coupling, i.e., cross-correlation between electric and magnetic orders, is a very desirable property to combine functionalities of materials for next-generation switchable devices. Multiferroics with spin-driven ferroelectricity presents such a mutual interaction concomitant with magneto- and electro-active excitations called electromagnons. TbMnO3 is a paradigmatic material in which two electromagnons have been observed in the cycloidal magnetic phase. However, their observation in TbMnO3 is restricted to the cycloidal spin phase and magnetic ground states that can support the electromagnon excitation are still under debate. Here, we show by performing Raman spectroscopy measurements under pressure that the lower-energy electromagnon (4 meV) disappears when the ground state enters from a cycloidal phase to an antiferromagnetic phase (E-type). On the contrary, the magnetoelectric activity of the higher-energy electromagnon (8 meV) increases in intensity by one order of magnitude. Using microscopic model calculations, we demonstrate that the lowerenergy electromagnon, observed in the cycloidal phase, originates from a higher harmonic of the magnetic cycloid, and we determine that the symmetric exchange-striction mechanism is at the origin of the higher-energy electromagnon which survives even in the E-type phase. The colossal enhancement of the electromagnon activity in TbMnO3 paves the way to use multiferroics more efficiently for generation, conversion and control of spin waves in magnonic devices.

cond-mat.str-el↗

arXiv2018

Crystal Growth and Doping Control of HgBa2CuO4+δ, the Model Compound for High-Tc Superconductors

A new method to grow very high quality single crystals of the superconducting HgBa2CuO4+δ mercury cuprates is reported. The single crystals are platelet-shaped, with surfaces of high optical quality and good crystallographic properties. Annealing enables optimization of Tc up to Tcmax = 94 K. With adequate treatment, the doping level of the crystalline samples can be finely controlled in a wide under- and over-doped range. Complete structural characterization from single crystal X-ray diffraction data is given for the first time for different doping levels. The role of added gold on the doping is also investigated. The signature of under- and over-doping for both pure and gold-substituted crystals has been identified from micro-Raman spectroscopy measurements.

cond-mat.supr-con↗

arXiv2018

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↗

arXiv2018

Crystal Growth and Characterization of HgBa2Ca2Cu3O8+δ Superconductor with the Highest Critical Temperature at Ambient Pressure

We report an original procedure for the elaboration of very high quality single crystals of superconducting HgBa2Ca2Cu3O8+δ mercury cuprates. These single crystals are unique with very high quality surface paving the way for spectroscopic, transport and thermodynamic probes in order to understand the hole-doped cuprate phase diagram. The superconductivity transition width of about 2 K indicates they are homogeneous. Annealing allows to optimize Tc up to Tc$^{max}$ = 133 K. We show for the first time that with adequate heat treatment, Hg-1223 can be largely under-doped and its doping level controlled. Importantly, the crystal structure was studied in detail by single crystal X-ray diffraction, and we have identified the signature of the under-doping by a detailed sample characterization and micro-Raman spectroscopy measurements.

cond-mat.str-el↗

arXiv2018

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↗

arXiv2018

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↗

arXiv2017

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↗

arXiv2016

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↗