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Thibault Charpentier

Publications and source records attributed to Thibault Charpentier.

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Quantum critical collapse of a pinned vortex glass

The interplay between disorder and vortex--vortex interactions in strongly disordered superconductors in a magnetic field can stabilize a vortex-glass state, characterized by strong pinning and the absence of positional order. Yet its role in the destruction of superconductivity at the field-driven superconductor--insulator transition has remained unresolved. Here we use plasmonic microwave spectroscopy of superconducting resonators patterned from amorphous indium oxide thin films to directly track the superfluid density up to the critical field $B_c$. We find an unexpected resilience of the superfluid density, which decreases only logarithmically over nearly three orders of magnitude in field, in stark contrast to the rapid power-law suppression expected for vortex lattices. We attribute this anomalously slow decay to a collective vortex-pinning mechanism counterintuitively enhanced by vortex--vortex interactions. The superfluid density then vanishes linearly at $B_c$, where independent magnetoresistance measurements identify a continuous quantum critical point, unlike the abrupt transition observed at zero field. We further uncover an exceptionally large nonlinear electromagnetic response of the vortex glass, manifested as a pronounced positive-Kerr effect with potential for quantum sensing. These results show how disorder controls the critical magnetic field and identify the vortex glass as the key intermediate state governing the magnetic-field-induced superconductor--insulator transition.

cond-mat.supr-con

Cryogenic shock exfoliation for ultrahigh mobility rhombohedral graphite nanoelectronics

Rhombohedral multilayer graphene (RMG) offers a highly tunable platform for correlated electron physics, featuring field-effect control of magnetic, superconducting, and topological phases[1-24]. The promise of these materials has been held back by the limited abundance of rhombohedral stacking in natural graphite, which constrains both sample yield and useful area. Here we introduce 'cryogenic shock exfoliation' to produce large area rhombohedral graphene flakes which, combined with a low-pressure van der Waals assembly technique that preserves stacking order, enable highly uniform devices exceeding 1300 $\mu m^2$ with fabrication yields of 90%. Using scanning nanoSQUID-on-tip imaging, we demonstrate uniform spin magnetism over the full central 10 times 10 $\mu m^2$ area of our devices. Transverse magnetic focusing reveals a disorder mean free path exceeding 200 $\mu m$ at low temperatures. Within the flat surface bands of RMG[20], we observe a size-driven crossover from Poiseuille to porous electron flow in the intermediate-temperature regime of strong electron-electron hydrodynamics[16, 25], providing a further signature of ultrahigh device quality. Our approach overcomes a key materials bottleneck in the fabrication of mesoscopic rhombohedral graphene devices, paving the way for incorporating strongly correlated phases into two-dimensional nanoelectronics.

cond-mat.mes-hall

Flat band surface state superconductivity in thick rhombohedral graphene

Rhombohedral multilayer graphene has recently emerged as a rich platform for studying correlation driven magnetic, topological and superconducting states. While most experimental efforts have focused on devices with N$\leq 9$ layers, the electronic structure of thick rhombohedral graphene features flat-band surface states even in the infinite layer limit. Here, we use layer resolved capacitance measurements to directly detect these surface states for $N\approx 13$ layer rhombohedral graphene devices. Using electronic transport and local magnetometry, we find that the surface states host a variety of ferromagnetic phases, including both valley imbalanced quarter metals and broad regimes of density in which the system spontaneously spin polarizes. We observe several superconducting states localized to a single surface state. These superconductors appear on the unpolarized side of the density-tuned spin transitions, and show strong violations of the Pauli limit consistent with a dominant attractive interaction in the spin-triplet, valley-singlet pairing channel. In contrast to previous studies of rhombohedral multilayers, however, we find that superconductivity can persist to zero displacement field where the system is inversion symmetric. Energetic considerations suggest that superconductivity in this regime is described by the existence of two independent surface superconductors coupled via tunneling through the insulating single crystal graphite bulk.

cond-mat.supr-con

Universal bound on microwave dissipation in superconducting circuits

Improving the coherence of superconducting qubits is essential for advancing quantum technologies. While superconductors are theoretically perfect conductors, they consistently exhibit residual energy dissipation when driven by microwave currents, limiting coherence times. Here, we report an empirical scaling relation between microwave dissipation and the superfluid density, a bulk property of superconductors related to charge carrier density and disorder. Our analysis spans a wide range of superconducting materials and device geometries, from highly disordered amorphous films to ultra-clean systems with record-high quality factors, including resonators, 3D cavities, and transmon qubits. This scaling reveals an intrinsic bulk dissipation channel, independent of surface dielectric losses, which we attribute to nonequilibrium quasiparticles trapped within disorder-induced spatial variations of the superconducting gap, with a density set by a universal material parameter. Our findings identify an empirical coherence limit associated with intrinsic material properties and provide a data-driven basis for materials selection in future superconducting quantum circuits.

cond-mat.mes-hall

First-order quantum breakdown of superconductivity in amorphous superconductors

Continuous quantum phase transitions are widely assumed and frequently observed in various systems of quantum particles or spins. Their characteristic trait involves scaling laws governing a second-order, gradual suppression of the order parameter as the quantum critical point is approached. The localization of Cooper pairs in disordered superconductors and the resulting breakdown of superconductivity have long stood as a prototypical example. Here, we show a departure from this paradigm, showcasing that amorphous superconducting films of indium oxide undergo a distinctive, discontinuous first-order quantum phase transition tuned by disorder. Through systematic measurements of the plasmon spectrum in superconducting microwave resonators, we provide evidence for a marked jump of both the zero-temperature superfluid stiffness and the transition temperature at the critical disorder. This discontinuous transition sheds light on the previously overlooked role of repulsive interactions between Cooper pairs and the subsequent competition between superconductivity and insulating Cooper-pair glass. Furthermore, our investigation shows that the critical temperature of the films no longer relates to the pairing amplitude but aligns with the superfluid stiffness, consistent with the pseudogap regime of preformed Cooper pairs. Our findings raise fundamental new questions into the role of disorder in quantum phase transitions and carry implications for superinductances in quantum circuits.

cond-mat.mes-hall

Near-power-law temperature dependence of the superfluid stiffness in strongly disordered superconductors

In BCS superconductors, the superfluid stiffness is virtually constant at low temperature and only slightly affected by the exponentially low density of thermal quasiparticles. Here, we present an experimental and theoretical study on the temperature dependence of superfluid stiffness $Θ\left(T\right)$ in a strongly disordered pseudo-gaped superconductor, amorphous $\text{InO}_{x}$, which exhibits non-BCS behavior. Experimentally, we report an unusual power-law suppression of the superfluid stiffness $δΘ\left(T\right)\propto T^{b}$ at $T\ll T_{c}$, with $b\sim1.6$, which we measured via the frequency shift of microwave resonators. Theoretically, by combining analytical and numerical methods to a model of a disordered superconductor with pseudogap and spatial inhomogeneities of the superconducting order parameter, we found a qualitatively similar low-temperature power-law behavior with exponent $b\sim1.6-3$ being disorder-dependent. This power-law suppression of the superfluid density occurs mainly due to the broad distribution of the superconducting order parameter that is known to exist in such superconductors [arXiv:1012.3630], even moderately far from the superconductor-insulator transition. The presence of the power-law dependence $δΘ\left(T\right)\propto T^{b}$ at low $T\ll T_{c}$ demonstrates the existence of low-energy collective excitations; in turn, it implies the presence of a new channel of dissipation in inhomogeneous superconductors caused by sub-gap excitations that are not quasiparticles. Our findings have implications for the use of strongly disordered superconductors as superinductance in quantum circuits.

cond-mat.supr-con

Structure and properties of lead silicate glasses

The original electronic structure of the Pb$^{2+}$ ion explains its particular structural role in crystalline phases and silicate glasses. After a description of the structural role of lead in crystalline phases (PbO, silicates), this chapter presents a summary of the main structural studies carried out on glasses from the SiO$_2$-PbO, SiO$_2$-PbO-R$_2$O (R: alkaline) and SiO$_2$-PbO-Al$_2$O$_3$ systems, using various spectroscopic and simulation techniques.

cond-mat.mtrl-sci

Reducing the impact of radioactivity on quantum circuits in a deep-underground facility

As quantum coherence times of superconducting circuits have increased from nanoseconds to hundreds of microseconds, they are currently one of the leading platforms for quantum information processing. However, coherence needs to further improve by orders of magnitude to reduce the prohibitive hardware overhead of current error correction schemes. Reaching this goal hinges on reducing the density of broken Cooper pairs, so-called quasiparticles. Here, we show that environmental radioactivity is a significant source of nonequilibrium quasiparticles. Moreover, ionizing radiation introduces time-correlated quasiparticle bursts in resonators on the same chip, further complicating quantum error correction. Operating in a deep-underground lead-shielded cryostat decreases the quasiparticle burst rate by a factor fifty and reduces dissipation up to a factor four, showcasing the importance of radiation abatement in future solid-state quantum hardware.

cond-mat.supr-con

Phonon traps reduce the quasiparticle density in superconducting circuits

Out of equilibrium quasiparticles (QPs) are one of the main sources of decoherence in superconducting quantum circuits, and are particularly detrimental in devices with high kinetic inductance, such as high impedance resonators, qubits, and detectors. Despite significant progress in the understanding of QP dynamics, pinpointing their origin and decreasing their density remain outstanding tasks. The cyclic process of recombination and generation of QPs implies the exchange of phonons between the superconducting thin film and the underlying substrate. Reducing the number of substrate phonons with frequencies exceeding the spectral gap of the superconductor should result in a reduction of QPs. Indeed, we demonstrate that surrounding high impedance resonators made of granular aluminum (grAl) with lower gapped thin film aluminum islands increases the internal quality factors of the resonators in the single photon regime, suppresses the noise, and reduces the rate of observed QP bursts. The aluminum islands are positioned far enough from the resonators to be electromagnetically decoupled, thus not changing the resonator frequency, nor the loading. We therefore attribute the improvements observed in grAl resonators to phonon trapping at frequencies close to the spectral gap of aluminum, well below the grAl gap.

cond-mat.supr-con

Extended Czjzek model applied to NMR parameter distributions in sodium metaphosphate glass

The Extended Czjzek Model (ECM) is applied to the distribution of NMR parameters of a simple glass model (sodium metaphosphate, $\mathrm{NaPO_3}$) obtained by Molecular Dynamics (MD) simulations. Accurate NMR tensors, Electric Field Gradient (EFG) and Chemical Shift Anisotropy (CSA), are calculated from Density Functional Theory (DFT) within the well-established PAW/GIPAW framework. Theoretical results are compared to experimental high-resolution solid-state NMR data and are used to validate the considered structural model. The distributions of the calculated coupling constant $C_Q\propto |V_{zz}|$ and of the asymmetry parameter $η_Q$ that characterize the quadrupolar interaction are discussed in terms of structural considerations with the help of a simple point charge model. Finally, the ECM analysis is shown to be relevant for studying the distribution of CSA tensor parameters and gives new insight into the structural characterization of disordered systems by solid-state NMR.

cond-mat.dis-nn

Effect of changing the rare earth cation type on the structure and crystallization behavior of an aluminoborosilicate glass

An aluminoborosilicate glass, containing high amount of rare earth (RE) accordingly to the following composition 50.68 SiO2 - 4.25 Al2O3 - 8.50 B2O3 - 12.19 Na2O - 4.84 CaO - 3.19 ZrO2 - 16.35 RE2O3 (wt.%), is currently under study for the immobilization of nuclear waste solutions. In this work, we wanted to investigate the effect of changing the RE cation type on the glass structure and on its crystallization behavior. For this purpose, a glass series was elaborated in which the nature of the RE is varying from lanthanum to lutetium. In this glass series, only little effect was observed on the glass structure. On the contrary, a strong impact was put in evidence on the crystallization behavior through different heat treatments. A slow cooling of the melt at 1^/circC/min, revealed significant crystallization of apatite Ca2RE8(SiO4)6O2 in sample containing rare earths with ionic radii close to that of calcium. Another heat treatment consisting of successive nucleation and growth stages, performed to force the crystallization in the bulk and reduce any surface crystallization effect, put in evidence the existence of a strongly heterogeneous second rare earth rich silicate phase for samples containing RE with low ionic radius (from Y to Lu).

cond-mat.mtrl-sci

Structural characterization of SiO2-Na2O-CaO-B2O3-MoO3 glasses

Nuclear spent fuel reprocessing generates high level radioactive waste with high Mo concentration that are currently immobilized in borosilicate glass matrices containing both alkali and alkaline-earth elements [1]. Because of its high field strength, Mo6+ ion has a limited solubility in silicate and borosilicate glasses and crystallization of alkali or alkaline-earth molybdates can be observed during melt cooling or heat treatment of glasses [2-4]. Glass composition changes can significantly modify the nature and the relative proportions of molybdate crystals that may form during natural cooling of the melt. For instance, in a previous work we showed that CaMoO4 crystallization tendency increased at the expenses of Na2MoO4 when B2O3 concentration increased in a SiO2-Na2O-CaO-MoO3 glass composition [4]. In this study, we present structural results on two series (Mx, By) of quenched glass samples belonging to this system using 29Si, 11B, 23Na MAS NMR and Raman spectroscopies. The effect of MoO3 on the glassy network structure is studied and its structural role is discussed (Mx series). The evolution of the distribution of Na+ ions within the borosilicate network is followed when B2O3 concentration increased (By series) and is discussed according to the evolution of the crystallization tendency of the melt. For all glasses, ESR was used to investigate the nature and the concentration of paramagnetic species.

cond-mat.mtrl-sci

Structural study of a rare earth-rich aluminoborosilicate glass containing various alkali and alkaline-earth modifier cations

A rare-earth rich aluminoborosilicate glass of composition (given in wt.%): 50.68 SiO2 - 4.25 Al2O3 - 8.50 B2O3 - 12.19 M2O - 4.84 M'O - 3.19 ZrO2 - 16.35 Nd2O3 (where M and M' are respectively an alkali and alkaline earth cation) is currently under study as potential nuclear waste form. In this work, we were interested in the structure of this glass in relation with the modifier cation type. Two different glass series were elaborated by changing separately the nature of the alkaline (M=Li, Na, K, Rb, Cs) and the alkaline-earth (M'=Mg, Ca, Sr, Ba) ions and different structural studies were intended to elucidate the local environment of the rare-earth and the network arrangement. Only slight effect was put in evidence on the covalency degree and the length of Nd-O linkage with a change of M or M', by optical spectroscopy and EXAFS measurements. Raman and MAS NMR (29Si, 27Al, 11B) spectroscopies showed a variation of the polymerization degree of the network with the size of the modifier cation. Finally, the most important feature of this glass composition is related to the AlO4- charge compensation which was proved to be uniquely assured by alkali cations.

cond-mat.mtrl-sci

Effect of the nature of alkali and alkaline-earth oxides on the structure and crystallization of an aluminoborosilicate glass developed to immobilize highly concentrated nuclear waste solutions

A complex rare-earth rich aluminoborosilicate glass has been proved to be a good candidate for the immobilization of new high level radioactive wastes. A simplified seven-oxides composition of this glass was selected for this study. In this system, sodium and calcium cations were supposed in other works to simulate respectively all the other alkali (R+=Li+, Rb+, Cs+) and alkaline-earth (R'2+=Sr2+, Ba2+) cations present in the complex glass composition. Moreover, neodymium or lanthanum are used here to simulate all the rare-earths and actinides occurring in waste solutions. In order to study the impact of the nature of R+ and R'2+ cations on both glass structure and melt crystallization tendency during cooling, two glass series were prepared by replacing either Na+ or Ca2+ cations in the simplified glass by respectively (Li+, K+, Rb+, Cs+) or (Mg2+, Sr2+, Ba2+) cations. From these substitutions, it was established that alkali ions are preferentially involved in the charge compensation of (AlO4)- entities in the glass network comparatively to alkaline-earth ions. The glass compositions containing calcium give way to the crystallization of an apatite silicate phase bearing calcium and rare-earth ions. The melt crystallization tendency during cooling strongly varies with the nature of the alkaline-earth.

cond-mat.mtrl-sci