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Etienne Janod

Publications and source records attributed to Etienne Janod.

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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

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

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

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

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

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

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

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

Long range coherent magnetic bound states in superconductors

The quantum coherent coupling of completely different degrees of freedom is a challenging path towards creating new functionalities for quantum electronics. Usually the antagonistic coupling between spins of magnetic impurities and superconductivity leads to the destruction of the superconducting order. Here we show that a localized classical spin of an iron atom immersed in a superconducting condensate can give rise to new kind of long range coherent magnetic quantum state. In addition to the well-known Shiba bound state present on top of an impurity we reveal the existence of a star shaped pattern which extends as far as 12 nm from the impurity location. This large spatial dispersion turns out to be related, in a non-trivial way, to the superconducting coherence length. Inside star branches we observed short scale interference fringes with a particle-hole asymmetry. Our theoretical approach captures these features and relates them to the electronic band structure and the Fermi wave length of the superconductor. The discovery of a directional long range effect implies that distant magnetic atoms could coherently interact leading to new topological superconducting phases with fascinating properties.

cond-mat.supr-con

Universal electric-field-driven resistive transition in narrow-gap Mott insulators

One of today's most exciting research frontier and challenge in condensed matter physics is known as Mottronics, whose goal is to incorporate strong correlation effects into the realm of electronics. In fact, taming the Mott insulator-to-metal transition (IMT), which is driven by strong electronic correlation effects, holds the promise of a commutation speed set by a quantum transition, and with negligible power dissipation. In this context, one possible route to control the Mott transition is to electrostatically dope the systems using strong dielectrics, in FET-like devices. Another possibility is through resistive switching, that is, to induce the insulator-to-metal transition by strong electric pulsing. This action brings the correlated system far from equilibrium, rendering the exact treatment of the problem a difficult challenge. Here, we show that existing theoretical predictions of the off-equilibrium manybody problem err by orders of magnitudes, when compared to experiments that we performed on three prototypical narrow gap Mott systems V2-xCrxO3, NiS2-xSex and GaTa4Se8, and which also demonstrate a striking universality of this Mott resistive transition (MRT). We then introduce and numerically study a model based on key theoretically known physical features of the Mott phenomenon in the Hubbard model. We find that our model predictions are in very good agreement with the observed universal MRT and with a non-trivial timedelay electric pulsing experiment, which we also report. Our study demonstrates that the MRT can be associated to a dynamically directed avalanche.

cond-mat.mtrl-sci

Electric pulse induced electronic patchwork in the Mott insulator GaTa$_{4}$Se$_{8}$

Following a recent discovery of the Insulator-to-Metal Transition induced by electric field in GaTa$_{4}$Se$_{8}$, we performed a detailed Scanning Tunneling Microscopy/Spectroscopy study of both pristine (insulating) and transited (conducting) crystals of this narrow gap Mott insulator. The spectroscopic maps show that pristine samples are spatially homogeneous insulators while the transited samples reveal at nanometer scale a complex electronic pattern that consists of metallic and super-insulating patches immersed in the pristine insulating matrix. Surprisingly, both kinds of patches are accompanied by a strong local topographic inflation, thus evidencing for a strong electron-lattice coupling involved in this metal-insulator transition. Finally, using a strong electric field generated across the STM tunneling junction, we demonstrate the possibility to trig the metal-insulator transition locally even at room temperature.

cond-mat.str-el

Electric-Field-Induced Resistive Switching in a Family of Mott Insulators : towards Non-Volatile Mott-RRAM Memories

The fundamental building blocks of modern silicon-based microelectronics, such as double gate transistors in non-volatile Flash memories, are based on the control of electrical resistance by electrostatic charging. Flash memories could soon reach their miniaturization limits mostly because reliably keeping enough electrons in an always smaller cell size will become increasingly difficult . The control of electrical resistance at the nanometer scale therefore requires new concepts, and the ultimate resistance-change device is believed to exploit a purely electronic phase change such as the Mott insulator to insulator transition [2]. Here we show that application of short electric pulses allows to switch back and forth between an initial high-resistance insulating state ("0" state) and a low-resistance "metallic" state ("1" state) in the whole class of Mott Insulator compounds AM4X8 (A = Ga, Ge; M= V, Nb, Ta; X = S, Se). We found that electric fields as low as 2 kV/cm induce an electronic phase change in these compounds from a Mott insulating state to a metallic-like state. Our results suggest that this transition belongs to a new class of resistive switching and might be explained by recent theoretical works predicting that an insulator to metal transition can be achieved by a simple electric field in a Mott Insulator. This new type of resistive switching has potential to build up a new class of Resistive Random Access Memory (RRAM) with fast writing/erasing times (50 ns to 10 μs) and resistance ratios ΔR/R of the order of 25% at room temperature.

cond-mat.mtrl-sci

Resistive switching induced by electronic avalanche breakdown in GaTa$_4$Se$_{8-x}$Te$_x$ narrow gap Mott Insulators

Mott transitions induced by strong electric fields are receiving a growing interest. Recent theoretical proposals have focused on the Zener dielectric breakdown in Mott insulators, however experimental studies are still too scarce to conclude about the mechanism. Here we report a study of the dielectric breakdown in the narrow gap Mott insulators GaTa$_4$Se$_{8-x}$Te$_x$. We find that the I-V characteristics and the magnitude of the threshold electric field (E$_{th}$) do not correspond to a Zener breakdown, but rather to an avalanche breakdown. E$_{th}$ increases as a power law of the Mott Hubbard gap (E$_g$), in surprising agreement with the universal law E$_{th}$ $\propto$E$_g$$^{2.5}$ reported for avalanche breakdown in semiconductors. However, the delay time for the avalanche that we observe in Mott insulators is over three orders of magnitude longer than in conventional semiconductors. Our results suggest that the electric field induces local insulator-to-metal Mott transitions that create conductive domains which grow to form filamentary paths across the sample.

cond-mat.str-el

Magnetoelastic polarons in the hole-doped quasi-one dimensional model system Y2-xCaxBaNiO5

Charge transport in the hole-doped quasi-1D model system Y$_{2-x}$Ca$_x$BaNiO$_5$ (x $ leq$ 0.15) is investigated in the 50-300 K temperature range. The resistivity temperature dependence is characterized by a constant activation energy $E_{a}/k_{B} sim$ 1830 K at room temperature while $E_{a}$ decreases upon cooling. We suggest that $E_{a}$ measures the binding energy of the doped holes which form magneto-acoustic polarons when polarizing the neighboring Ni spins. A semi-classical model is proposed which allows to relate the electrical measurements and the bulk magnetic susceptibility. This model gives a picture of the spin-charge-lattice relation in this inhomogeneously doped quasi-1D system and explains its unusual one-particle charge excitation spectrum close to the Fermi level.

cond-mat.str-el

Crystal structure and charge order below the metal-insulator transition in the vanadium bronze $β$-SrV$_6$O$_{15}$

Single crystal X-ray diffraction measurements were performed on one-dimensional mixed valence vanadium bronze $β$-SrV$_6$O$_{15}$ in which a metal-insulator transition exists at 170 K. Above 170 K the P2$_1$/a structure with zigzag order of Sr in the tunnels of vanadium is confirmed. In the structure below 170 K, the P2$_1$/a space group is retained with a b-axis threefold increase and a charge order appears. A Bond Valence Sum analysis shows that the charge order may consist in clusters of V$^{4+}$ regularly spaced along 1D direction.

cond-mat.str-el