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Laurent Cario

Publications and source records attributed to Laurent Cario.

At least 19 recordsLinked to original sources
arXiv2026

Multigap superconductivity in Ising superconductors: The case of (LaSe)1.14(NbSe2)m misfit layer compounds

Strong spin-orbit coupling and broken inversion symmetry in transition metal dichalcogenides give rise to Ising superconductivity, a spin-protected pairing state first identified in monolayer NbSe$_2$ through in-plane critical fields far exceeding the Pauli limit. More recently, Ising superconductivity has been proposed as a potential route to unconventional and even topological superconductivity in bulk misfit compounds. Here, we investigate the superconducting order parameter of layered misfit compounds composed of alternating transition metal dichalcogenide and rocksalt layers, which host extremely doped, electronically decoupled NbSe$_2$ sheets within a three-dimensional crystal. Using directional scanning tunneling spectroscopy on the misfit superconductors (LaSe)$_{1.14}$(NbSe$_2$) and (LaSe)$_{1.14}$(NbSe$_2$)$_2$, we uncover a strongly anisotropic multigap superconducting state: a fragile gap on the $Γ$-centered Fermi-surface pocket coexists with a robust, intrinsic gap on the K and K$'$ pockets. These features are in quantitative agreement with momentum-resolved gaps $Δ(\mathbf{k})$ obtained from anisotropic Migdal-Eliashberg calculations. The marked fragility of the $Γ$-centered gap, combined with the strong sensitivity of the critical temperature to non-magnetic disorder, points to pairing beyond conventional $s$-wave symmetry, potentially involving a topological order parameter. These results establish NbSe$_2$-based misfit compounds as a tunable bulk platform for multigap, unconventional superconductivity, with Ising protection offering a promising route toward topological pairing.

cond-mat.supr-con↗
arXiv2026

Doping-controlled topological superconducting transition in misfit layer compounds

Achieving topological superconductivity is a key goal in quantum physics, offering a path to fault-tolerant quantum computers. A central challenge in this field is to continuously drive a material through a topological quantum phase transition to directly observe the evolution from trivial to topological superconductivity. However, finding a robust platform that allows such extreme and precise tuning remains a challenge. Here, we demonstrate a doping-controlled phase transition from a conventional to a topological superconducting state in the bulk misfit layer compound (LaxPb1-xSe)1.14(NbSe2)2. We reveal a non-monotonic phase diagram characterized by two distinct superconducting regimes separated by a non-superconducting phase at a precise doping. In the highly doped regime, the superconducting phase becomes remarkably sensitive to non-magnetic disorder, and orientation-selective in-gap modes emerge at atomic step edges. Supported by Bogoliubov-de Gennes calculations, these emergent spatial signatures are consistent with a time-reversal-symmetric crystalline-topological order parameter. Our results establish misfit compounds as a platform to engineering topological superconductivity.

cond-mat.supr-con↗
arXiv2026

Doping tunable charge density waves in misfit layer compounds

The ability to tune charge density waves (CDWs) through external control knobs, such as doping, pressure or strain is crucial for exploring the phase diagram of two dimensional (2D) or quasi-2D materials. Yet, controlling CDWs critical temperature and ordering vector remains a challenge for current experimental techniques. In this work, we establish misfit layer compound heterostructures as a reliable platform to manipulate CDWs in transition metal dichalcogenides. By combining ab initio calculations with low-temperature scanning tunneling microscopy, we show how to achieve doping tunable control over NbSe2 CDW by chemically alloying in the rocksalt subunit. Crucially, we prove that tuning the La Pb ratio in the misfit family (LaxPb1xSe)1.14(NbSe2)2 enables stabilization of different CDW orders, such as 2x2 or 3x3 patterns, and even coexisting phases. This work paves the way for engineering transition metal dichalcogenides with tailored charge density waves within misfit heterostructures.

cond-mat.mtrl-sci↗
arXiv2026

Tuning the Charge Transfer of Transition Metal Dichalcogenides via Misfit Layer Compounds

Misfit layer compounds (MLCs) are a versatile platform for exploring the electronic phase diagram of two dimensional (2D) materials beyond the limits of conventional gating techniques. This work demonstrates the precise tunability of electron doping in NbSe2 monolayers through chemical alloying within the rocksalt layer of (LaxPb1xSe)1.14(NbSe2)2 heterostructures. By combining first principles density functional theory (DFT) calculations with angle resolved photoemission spectroscopy (ARPES), we prove that the rocksalt unit acts as an universal electron donor. We show that varying the La Pb ratio results in a rigid Fermi level shift, still preserving the NbSe2 electronic structure. Crucially, photon energy dependent ARPES confirms that the NbSe2 layers nearly maintain their intrinsic 2D character and orbital identity within the three dimensional misfit. This study establishes MLCs as a reliable platform for engineering emergent states in 2D transition metal dichalcogenides through precise stoichiometric control.

cond-mat.mtrl-sci↗
arXiv2026

Two pathways to break the insulating state in a correlated transition metal oxide

Correlated transition metal oxides present exciting prospects as switches or memory and storage devices owing to the possibility to control electronic properties using various external stimuli. While their complex behaviour is known to stem from interplay between electronic correlations, atomic structure and orbital physics, they remain poorly understood on the microscopic level. Here, we investigate such origins as a function of temperature and pressure in the transition metal oxide Ti3O5. We find that the insulating room-temperature phase is characterized by one-dimensional zig-zag chains composed by two types of titanium dimers forming orbital selective valence bonds. At the thermal phase transition, one type of titanium dimer breaks up, resulting in an insulator to metal transition with a large orbital repopulation between the two states. Moreover, optical spectroscopy reveals that an additional pressure-driven insulator to metal transition occurs in Ti3O5 at room temperature. The phenomenology of this novel pressure-induced metallic transition is completely different from the insofar studied transitions and results from a competition between intra- and inter-dimer hopping. Our combined results suggest that Ti3O5 is a prototypical correlated transition metal oxide, where both correlations as well as orbital interactions need to be considered to fully understand the evolution of the electronic states.

cond-mat.str-el↗
arXiv2025

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↗
arXiv2024

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↗
arXiv2023

Dynamics of electronic states in the insulating Intermediate surface phase of 1T-TaS$_2$

This article reports a comparative study of bulk and surface properties in the transition metal dichalcogenide 1T-TaS$_2$. When heating the sample, the surface displays an intermediate insulating phase that persists for $\sim 10$ K on top of a metallic bulk. The weaker screening of Coulomb repulsion and stiffer Charge Density Wave (CDW) explain such resilience of a correlated insulator in the topmost layers. Both time resolved ARPES and transient reflectivity are employed to investigate the dynamics of electrons and CDW collective motion. It follows that the amplitude mode is always stiffer at the surface and displays variable coupling to the Mott-Peierls band, stronger in the low temperature phase and weaker in the intermediate one.

cond-mat.str-el↗
arXiv2023

Electronic dispersion, correlations and stacking in the photoexcited state of 1T-TaS$_2$

Here we perform angle and time-resolved photoelectron spectroscopy on the commensurate Charge Density Wave (CDW) phase of 1T-TaS$_2$. Data with different probe pulse polarization are employed to map the dispersion of electronic states below and above the chemical potential. Upon photoexcitation, the fluctuations of CDW order erase the band dispersion near to the chemical potential and halve the charge gap size. This transient phase sets within half a period of the coherent lattice motion and is favored by strong electronic correlations. The experimental results are compared to Density-Functional Theory (DFT) calculations with a self-consistent evaluation of the Coulomb repulsion. Our simulations indicate that the screening of Coulomb repulsion depends on the stacking order of the TaS$_2$ layers. The entanglement of such degrees of freedom suggest that both the structural order and electronic repulsion are locally modified by the photoinduced CDW fluctuations.

cond-mat.str-el↗
arXiv2023

Protection of Ising spin-orbit coupling in bulk misfit superconductors

Low-dimensional materials have remarkable properties that are distinct from their bulk counterparts. A paradigmatic example is Ising superconductivity that occurs in monolayer materials such as NbSe2 which show a strong violation of the Pauli limit. In monolayers, this occurs due to a combination of broken inversion symmetry and spin-orbit coupling that locks the spins of the electrons out-of-plane. Bulk NbSe2 is centrosymmetric and is therefore not an Ising superconductor. We show that bulk misfit compound superconductors, (LaSe)1.14(NbSe2) and (LaSe)1.14(NbSe2)2, comprised of monolayers and bilayers of NbSe2, exhibit unexpected Ising protection with a Pauli-limit violation comparable to monolayer NbSe2, despite formally having inversion symmetry. We study these misfit compounds using complementary experimental methods in combination with first-principles calculations. We propose theoretical mechanisms of how the Ising protection can survive in bulk materials. We show how some of these mechanisms operate in these bulk compounds due to a concerted effect of charge-transfer, defects, reduction of interlayer hopping, and stacking. This highlights how Ising superconductivity can, unexpectedly, arise in bulk materials, and possibly enable the design of bulk superconductors that are resilient to magnetic fields.

cond-mat.supr-con↗
arXiv2021

Coherent and incoherent tunneling into YSR states revealed by atomic scale shot-noise spectroscopy

The pair breaking potential of individual magnetic impurities in s-wave superconductors generates localized states inside the superconducting gap commonly referred to as Yu- Shiba-Rusinov (YSR) states whose isolated nature makes them ideal building blocks for artificial structures that may host Majorana fermions. One of the challenges in this endeavor is to understand their intrinsic lifetime, $\hbar/Λ$, which is expected to be limited by the inelastic coupling with the continuum thus leading to decoherence. Here we use shot-noise scanning tunneling microscopy to reveal that electron tunnelling into superconducting 2H-NbSe$_2$ mediated by YSR states is ordered as function of time, as evidenced by a reduction of the noise. Moreover, our data show the concomitant transfer of charges e and 2e, indicating that incoherent single particle and coherent Andreev processes operate simultaneously. From the quantitative agreement between experiment and theory we obtain $Λ$ = 1 $μ$eV $\ll$ $k_BT$ demonstrating that shot-noise can probe energy- and time scales inaccessible by conventional spectroscopy whose resolution is thermally limited.

cond-mat.supr-con↗
arXiv2020

Misfit layer compounds: a platform for heavily-doped two-dimensional transition metal dichalcogenides

Transition metal dichalcogenides (TMDs) display a rich variety of instabilities such as spin and charge orders, Ising superconductivity and topological properties. Their physical properties can be controlled by doping in electric double-layer field-effect transistors (FET). However, for the case of single layer NbSe$_2$, FET doping is limited to $\approx 1\times 10^{14}$ cm$^{-2}$, while a somewhat larger charge injection can be obtained via deposition of K atoms. Here, by performing ARPES, STM, quasiparticle interference measurements, and first principles calculations we show that a misfit compound formed by sandwiching NbSe$_2$ and LaSe layers behaves as a NbSe$_2$ single layer with a rigid doping of $0.55-0.6$ electrons per Nb atom or $\approx 6\times 10^{14}$ cm$^{-2}$. Due to this huge doping, the $3\times3$ charge density wave is replaced by a $2\times2$ order with very short coherence length. As a tremendous number of different misfit compounds can be obtained by sandwiching TMDs layers with rock salt or other layers, our work paves the way to the exploration of heavily doped 2D TMDs over an unprecedented wide range of doping.

cond-mat.mtrl-sci↗
arXiv2020

Novel $J_{\rm{eff}}$=3/2 Metallic Phase and Unconventional Superconductivity in GaTa$_4$Se$_8$

By means of density functional theory plus dynamical mean-field theory (DFT+DMFT) calculations and resonant inelastic x-ray scattering (RIXS) experiments, we investigate the high-pressure phases of the spin-orbit-coupled $J_{\rm{eff}}=3/2$ insulator GaTa$_4$Se$_8$. Its metallic phase, derived from the Mott state by applying pressure, is found to carry $J_{\rm{eff}}=3/2$ moments. The characteristic excitation peak in the RIXS spectrum maintains its destructive quantum interference of $J_{\rm{eff}}$ at the Ta $L_2$-edge up to 10.4 GPa. Our exact diagonalization based DFT+DMFT calculations including spin-orbit coupling also reveal that the $J_{\rm{eff}}=3/2$ character can be clearly identified under high pressure. These results establish the intriguing nature of the correlated metallic magnetic phase, which represents the first confirmed example of $J_{\rm{eff}}$=3/2 moments residing in a metal. They also indicate that the pressure-induced superconductivity is likely unconventional and influenced by these $J_{\rm{eff}}=3/2$ moments. Based on a self-energy analysis, we furthermore propose the possibility of doping-induced superconductivity related to a spin-freezing crossover.

cond-mat.str-el↗
arXiv2019

Unexplored reactivity of (Sn)2- Oligomers with transition metals in low-temperature solid-state reactions

Chalcogenides (Q = S, Se, Te), one of the most important family of materials in solid-state chemistry, differ from oxides by their ability to form covalently-bonded (Qn)2- oligomers. Each chalcogen atom within such entity fulfills the octet rule by sharing electrons with other chalcogen atoms but some antibonding levels are vacant. This makes these oligomers particularly suited for redox reactions in solid state, namely towards elemental metals with a low redox potential that may be oxidized. We recently used this strategy to design, at low temperature and in an orientated manner, materials with 2D infinite layers through the topochemical insertion of copper into preformed precursors containing (S2)2- and/or (Se2)2- dimers (i.e. La2O2S2, Ba2F2S2 and LaSe2). Herein we extend the validity of the concept to the redox activity of (S2)2- and (S3)2- oligomers towards 3d transition metal elements (Cu, Ni, Fe) and highlight the strong relationship between the structures of the precursors, BaS2 and BaS3, and the products, BaCu2S2, BaCu4S3, BaNiS2 and BaFe2S3. Clearly, beyond the natural interest for the chemical reactivity of oligomers to generate compounds, this soft chemistry route may conduct to the rational conception of materials with a predicted crystal structure.

cond-mat.mtrl-sci↗
arXiv2018

Traces of Charge Density Waves in NbS$_2$

Among Transition Metal Dichalcogenides (TMD), NbS$_2$ is often considered as the archetypal compound that does not have a Charge Density Wave (CDW) in any of its polytypes. By comparison, close iso-electronic compounds such as NbSe$_2$, TaS$_2$ and TaSe$_2$ all have CDW in at least one polytype. Here, we report traces of CDW in the 2H polytype of NbS$_2$, using diffuse x-ray scattering measurements at 77\,K and room temperature. We observe 12 extremely weak satellite peaks located at $\pm$13$^\mathrm{o}$ 54' from $\vec{a}^*$ and $\vec{b}^*$ around each Bragg peaks in the $(h,k,0)$ plane. These satellite peaks are commensurate with the lattice via $3\vec{q}-\vec{q}\,'=\vec{a}^*$, where $\vec{q}\,'$ is the 120$^{\circ}$ rotation of $\vec{q}$, and define two chiral $\sqrt{13}\,a\times\sqrt{13}\,a$ superlattices in real space. These commensurate wavevectors and tilt angle are identical to those of the CDW observed in the 1T polytype of TaS$_2$ and TaSe$_2$. To understand this similarity and the faintness of the peaks, we discuss possible sources of local 1T polytype environment in bulk 2H-NbS$_2$ crystals.

cond-mat.str-el↗
arXiv2017

Relaxation of a Mott-neuron

We consider the phenomenon of electric Mott transition (EMT), which is an electric induced insulator to metal transition. Experimentally, it is observed that depending on the magnitude of the electric excitation the final state may show a short lived or a long lived resistance change. We extend a previous model for the EMT to include the effect of local structural distortions through an elastic energy term. We find that by strong electric pulsing the induced metastable phase may become further stabilized by the electro-elastic effect. We present a systematic study of the model by numerical simulations and compare the results to new experiments in Mott insulators of the AM4Q8 family. Our work significantly extends the scope of our recently introduced leaky-integrate-and-fire Mott-neuron [P. Stoliar Adv Mat 2017] to bring new insight on the physical mechanism of its relaxation. This is a key feature for future neuromorphic circuit implementations.

cond-mat.mtrl-sci↗
arXiv2017

Direct experimental observation of the molecular Jeff=3/2 ground state in the lacunar spinel GaTa4Se8

Strong spin-orbit coupling lifts the degeneracy of t2g orbitals in 5d transition-metal systems, leaving a Kramers doublet and quartet with effective angular momentum of Jeff = 1/2 and 3/2, respectively. These spin-orbit entangled states can host exotic quantum phases such as topological Mott state, unconventional superconductivity, and quantum spin liquid. The lacunar spinel GaTa4Se8 was theoretically predicted to form the molecular Jeff = 3/2 ground state. Experimental verification of its existence is an important first step to exploring the consequences of the Jeff = 3/2 state. Here, we report direct experimental evidence of the Jeff = 3/2 state in GaTa4Se8 by means of excitation spectra of resonant inelastic x-rays scattering at the Ta L3 and L2 edges. We found that the excitations involving the Jeff = 1/2 molecular orbital were suppressed only at the Ta L2 edge, manifesting the realization of the molecular Jeff = 3/2 ground state in GaTa4Se8.

cond-mat.str-el↗