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Matthieu Bugnet

Publications and source records attributed to Matthieu Bugnet.

6 recordsLinked to original sources

Photo-induced Wavelength-tuning of Telecom-band Quantum Dot Nanowires Embedded in a Phase Change Material

Scalable quantum-photonic technologies require spatially separated emitters to emit at the same wavelength, yet epitaxially grown quantum dots naturally exhibit emitter-to-emitter variations in their emission energies. Here, we demonstrate a contact-free post-growth tuning approach for InAs quantum dots embedded in InP nanowires using the photo-induced transformation of an amorphous Sb2S3 shell. This photoinduced effect leads to a progressive relaxation of the strain imposed on the InP core, enabling controlled spectral tuning of the quantum-dot emission. The effect is observed both at room temperature and under cryogenic conditions for quantum dots emitting in the O-band of the telecommunications spectrum. Strain-induced redshifts of approximately 7 meV at room temperature and 28 meV under cryogenic conditions are observed, respectively. The use of an amorphous chalcogenide shell therefore provides a route to achieve local wavelength tuning at the single quantum-dot-in-a-nanowire level after growth. This approach could enable spectrally matched emitters for scalable quantum-photonic architectures.

cond-mat.mes-hall

AI-Driven Phase Identification from X-ray Hyperspectral Imaging of cycled Na-ion Cathode Materials

Na-ion batteries have emerged as viable candidates for large-scale energy storage applica- tions due to resource abundance and cost advantages. The constraints imposed on their performance and durability, for instance, by complex phase transformations in positive electrode materials during electrochemical cycling, can be addressed and are thus not detrimental to their development. However, diffusion-limited Na-ion transport can drive spatially heterogeneous phase nucleation and propagation, leading to multiphase coexis- tence and locally non-uniform electrochemical activity, generating complex reaction path- ways that challenge both mechanistic understanding and predictive material optimization. These challenges can be addressed by investigating single-crystalline regions of materials, i.e. down to the scale of individual particles, although such analyses are often constrained by energetically and/or spatially sparse hyperspectral datasets. Here, we developed an AI-driven method to process hyperspectral data under sparse sampling conditions and generate multiphase maps with nanometer-scale resolution over a micrometer-scale field of view. We applied this processing on scanning transmission X-ray microscopy (STXM) data to determine the distribution and coexistence of phases in individual particles of NaxV2(PO4)2F3 cathode materials, at different states of charge. The methodology relies on a workflow which combines a Gaussian mixture variational autoencoder (GMVAE) algorithm with the Pearson corre- lation coefficient to identify the sodium content and map their spatial distribution. Our approach reveals nanoscale phase heterogeneity and evolution within individual particles, and improves the reliability of phase detection by identifying ambiguity zones, false assign- ments, and transition phases localized at grain boundaries.

cond-mat.mtrl-sci

Nanoscale Mapping of Transition Metal Ordering in Individual LiNi0.5Mn1.5O4 Particles Using 4D-STEM ACOM Technique

The electrochemical performance of the spinel LiNi0.5Mn1.5O4, a high-voltage positive electrode material for Li-ion batteries, is influenced by the transition metal arrangement in the octahedral network, leading to disordered (Fd m S.G.) and ordered3 (P4332 S.G.) structures. However, widely used techniques lack the spatial resolution necessary to elucidate the ordering phenomenon at the particle scale. Using the 4D-STEM technique, we present the first direct observation of ordering distribution in individual LiNi0.5Mn1.5O4 particles with nanometric spatial resolution. We propose a quantification method for the local degree of ordering based on the ratio of ordered to disordered spinel lattices along the particle thickness extracted from electron diffraction spot intensities. In an ordered spinel LiNi0.5Mn1.5O4, the transition metal ordering is consistently observed throughout the primary particle. However, the extent of ordering in the spinel phase depends on its distribution at the particle scale, a factor influenced by the annealing conditions. The 4D-STEM analysis elucidates the boundary between highly-ordered and low-ordered LiNi0.5Mn1.5O4 particles.

cond-mat.mtrl-sci

Reversible single-pulse laser-induced phase change of Sb$_2$S$_3$ thin films: multi-physics modeling and experimental demonstrations

Phase change materials (PCMs) have gained a tremendous interest as a means to actively tune nanophotonic devices through the large optical modulation produced by their amorphous to crystalline reversible transition. Recently, materials such as Sb$_2$S$_3$ emerged as particularly promising low loss PCMs, with both large refractive index modulations and transparency in the visible and NIR. Controlling the local and reversible phase transition in this material is of major importance for future applications, and an appealing method to do so is to exploit pulsed lasers. Yet, the physics and limits involved in the optical switching of Sb$_2$S$_3$ are not yet well understood. Here, we investigate the reversible laser-induced phase transition of Sb$_2$S$_3$, focusing specifically on the mechanisms that drive the optically induced amorphization, with multi-physics considerations including the optical and thermal properties of the PCM and its environment. We theoretically and experimentally determine the laser energy threshold for reversibly changing the phase of the PCM, not only between fully amorphous and crystalline states but also between partially recrystallized states. We then reveal the non-negligible impact of the material's polycrystallinity and anisotropy on the power thresholds for optical switching. Finally, we address the challenges related to laser amorphization of thick Sb$_2$S$_3$ layers, as well as strategies to overcome them. These results enable a qualitative and quantitative understanding of the physics behind the optically-induced reversible change of phase in Sb$_2$S$_3$ layers.

physics.app-ph

Real-space mapping of electronic orbitals

Electronic states are responsible for most material properties, including chemical bonds, electrical and thermal conductivity, as well as optical and magnetic properties. Experimentally, however, they remain mostly elusive. Here, we report the real-space mapping of selected transitions between p and d states on the {\AA}ngstr\"om scale in bulk rutile (TiO2) using electron energy-loss spectrometry (EELS), revealing information on individual bonds between atoms. On the one hand, this enables the experimental verification of theoretical predictions about electronic states. On the other hand, it paves the way for directly investigating electronic states under conditions that are at the limit of the current capabilities of numerical simulations such as, e.g., the electronic states at defects, interfaces, and quantum dots.

cond-mat.mtrl-sci

The origin of anisotropy and high density of states in the electronic structure of Cr$_2$GeC by means of polarized soft X-ray spectroscopy and ab initio calculations

The anisotropy in the electronic structure of the inherently nanolaminated ternary phase Cr$_{2}$GeC is investigated by bulk-sensitive and element selective soft x-ray absorption/emission spectroscopy. The angle-resolved absorption/emission measurements reveal differences between the in-plane and out-of-plane bonding at the (0001) interfaces of Cr$_{2}$GeC. The Cr $L_{2,3}$, C $K$, and Ge $M_{1}$, $M_{2,3}$ emission spectra are interpreted with first-principles density-functional theory (DFT) including core-to-valence dipole transition matrix elements. For the Ge $4s$ states, the x-ray emission measurements reveal two orders of magnitude higher intensity at the Fermi level than DFT within the General Gradient Approximation (GGA) predicts. We provide direct evidence of anisotropy in the electronic structure and the orbital occupation that should affect the thermal expansion coefficient and transport properties. As shown in this work, hybridization and redistribution of intensity from the shallow $3d$ core levels to the $4s$ valence band explain the large Ge density of states at the Fermi level.

cond-mat.mtrl-sci