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Clément Faugeras

Publications and source records attributed to Clément Faugeras.

At least 19 recordsLinked to original sources

Layer-Dependent Phonons, Excitons, and Magneto-Optical Phenomena in CrSBr: A Mini Review

Two-dimensional layered magnetic materials offer a versatile platform for exploring low-dimensional magnetism and coupled many-body interactions in these materials. Chromium sulfur bromide (CrSBr) is a promising candidate for advanced spintronic and optoelectronic applications because of its intrinsic air stability, semiconducting nature, strong in-plane anisotropy, and A-type antiferromagnetic ordering. This review summarizes recent advances in the understanding of the layer-dependent vibrational and excitonic properties of CrSBr, as well as its magneto-optical response, from bulk crystals to the monolayer limit. We examined its crystal structure, magnetic anisotropy, and interlayer spin reorientation, followed by insights into vibrational dynamics and spin-phonon coupling. Particular emphasis is placed on the excitonic landscape, including magnetic-field-sensitive photoluminescence, localized excitonic states, and the coexistence of Frenkel- and Wannier-Mott excitons in the bandgap. Finally, we discuss the challenges and prospects of harnessing the unique layer-dependent properties of CrSBr in spintronic, magneto-optical, and quantum photonic technologies.

cond-mat.mes-hall↗

Room-temperature antiferromagnetic resonance in NaMnAs

We report on antiferromagnetic resonance experiments in bulk tetragonal NaMnAs -- a room-temperature antiferromagnetic semiconductor. Our results corroborate previous ab initio studies, which propose that NaMnAs is an easy-axis antiferromagnet with the Néel vector oriented along the tetragonal axis. At $ B = 0 $, we find a single antiferromagnetic resonance line at 7 meV and associate it with a doubly degenerate ($ k = 0 $) magnon mode. Its energy softens considerably with increasing $ T $, but remains clearly visible in the data up to room temperature. From the experimental data, we estimate the single-ion anisotropy of the Mn ions in NaMnAs in the range 0.1-0.2 meV, a value that is relatively large compared to other manganese-based antiferromagnets.

cond-mat.mtrl-sci↗

Colloquium: A critique on van der Waals and two-dimensional magnets

Magnetic two-dimensional (2D) crystals were isolated about a decade ago, triggering a tremendous research activity worldwide. This colloquium raises a stiff question: what is really new about them? At first sight, they seem to be purer implementations of 2D spin models than traditional systems such as ultra-thin films. Yet, they partly realized their promises so far, and whether they give fresh perspectives on long-standing predictions in statistical physics is still an open question. Undoubtedly, they are uniquely amenable to electric-field effect, susceptible to mechanical deformation, and sensitive to moirés, for example. They represent interesting platforms for exploring, challenging, or simply revisiting a wide range of phenomena in condensed matter magnetism. This colloquium intends to offer a critical, yet not necessarily skeptical, overview of the field, clarifying what we believe could be unique with 2D magnets, related quasi-2D van der Waals magnets, and their heterostructures.

cond-mat.mtrl-sci↗

Multilayer Crystal Field states from locally broken centrosymmetry

Local charge, spin, or orbital degrees of freedom with intersite interactions are oftentimes sufficient to construct most quantum orders. This is conventionally true for f-electron systems, where the extent of the f-electrons and their associated crystal-electric-field (CEF) states are strongly localized. Here, polarized Raman spectroscopy measurements of a locally non-centrosymmetric compound, CeCoSi, unveil more CEF excitations than expected in the local model. We interpret this as experimental evidence for the entanglement of CEF states between cerium layers. This composite sublattice, spin, and orbital degree of freedom provides an unconsidered means to form novel orders, not only in this system, but in any system exhibiting globally preserved yet locally broken centrosymmetry.

cond-mat.str-el↗

Laser patterning of the room temperature van der Waals ferromagnet 1$T$-CrTe$_2$

Lamellar crystalline materials, whose layers are bond by van der Waals forces, can be stacked to form ultrathin artificial heterostructures, and in particular vertical magnetic junctions when some of the stacked materials are (ferro)magnetic. Here, using the room temperature van der Waals ferromagnet 1$T$-CrTe$_2$, we report a method for patterning lateral magnetic junctions. Exploiting the heat-induced phase transformation of the material into Cr$_x$Te$_y$ compounds ($x/y>1/2$), we use local laser heating to imprint patterns at the micron-scale. Optimizing laser heat dissipation, we further demonstrate the crucial role of the substrate to control the phase transformation. If plain, unstructured poorly heat-conducting substrates allow for direct writing of magnetic patterns, structured $h$-BN layers can serve as heat stencils to draw potentially thinner patterns. Besides, $h$-BN encapsulation turns out to be heat-protective (in addition from protecting against oxidation as it is generally used for), allowing the demonstration of room temperature ferromagnetism in $<$7~nm-thick 1$T$-CrTe$_2$.

cond-mat.mtrl-sci↗

Resonant X-ray spectroscopies on Chromium $3\textit{d}$ orbitals in CrSBr

We investigate the Cr electronic structure and excitations in CrSBr, a layered magnetic semiconductor, using a combination of resonant x-ray spectroscopic techniques. X-ray absorption spectroscopy (XAS) and resonant inelastic x-ray scattering (RIXS) spectra collected at the Cr $L_{2,3}$ edges reveal significant linear dichroism, which arises from the distorted octahedral environment surrounding the Cr$^{3+}$ ions. The origin of the bright excitons observed in this compound is examined through a comparison of the d-d excitations identified in the RIXS spectra, the x-ray excited optical luminescence (XEOL) spectra, and previously reported optical spectroscopic and theoretical studies. To further understand these phenomena, we develop a multiplet model based on a crystal electric field (CEF) approach that accounts for the local environment of Cr ions. This model successfully reproduces several experimental features, while also suggesting strong hybridization effects between Cr $3\textit{d}$ orbitals and ligands that are not fully captured by the present framework. These findings advance our understanding of the electronic structure and excitonic behavior in CrSBr and provide a foundation for future $\textit{in-situ}$ and $\textit{operando}$ studies of CrSBr-based devices for spintronic and optoelectronic applications.

cond-mat.mtrl-sci↗

Rydberg series of intralayer K-excitons in WSe$_2$ multilayers

Semiconducting transition metal dichalcogenides of group VI are well-known for their prominent excitonic effects and the transition from an indirect to a direct band gap when reduced to monolayers. While considerable efforts have elucidated the Rydberg series of excitons in monolayers, understanding their properties in multilayers remains incomplete. In these structures, despite an indirect band gap, momentum-direct excitons largely shape the optical response. In this work, we combine magneto-reflectance experiments with theoretical modeling based on the $\mathbf {k\cdot p}$ approach to investigate the origin of excitonic resonances in WSe$_2$ bi-, tri-, and quadlayers. For all investigated thicknesses, we observe a series of excitonic resonances in the reflectance spectra, initiated by a ground state with an amplitude comparable to the ground state of the 1$s$ exciton in the monolayer. Higher energy states exhibit a decrease in intensity with increasing energy, as expected for the excited states of the Rydberg series, although a significant increase in the diamagnetic shift is missing in tri- and quadlayers. By comparing the experimental observations with theoretical predictions, we discover that the excitonic resonances observed in trilayers originate from two Rydberg series, while quadlayers exhibit four such series, and bilayers host a single Rydberg series similar to that found in monolayers.

cond-mat.mes-hall↗

Spin-defect characteristics of single sulfur vacancies in monolayer $\text{MoS}_2$

Single spin defects in 2D transition-metal dichalcogenides are natural spin-photon interfaces for quantum applications. Here we report high-field magneto-photoluminescence spectroscopy from three emission lines (Q1, Q2 and Q*) of He-ion induced sulfur vacancies in monolayer $\text{MoS}_2$. Analysis of the asymmetric PL lineshapes in combination with the diamagnetic shift of Q1 and Q2 yields a consistent picture of localized emitters with a wavefunction extent of $\sim$ 3.5 nm. The distinct valley-Zeeman splitting in out-of-plane $B$-fields and the brightening of dark states through in-plane $B$-fields necessitates spin-valley selectivity of the defect states and lifted spin-degeneracy at zero field. Comparing our results to ab-initio calculations identifies the nature of Q1 and Q2 and suggests that Q* is the emission from a chemically functionalized defect. Analysis of the optical degree of circular polarization reveals that the Fermi level is a parameter that enables the tunability of the emitter. These results show that defects in 2D semiconductors may be utilized for quantum technologies.

cond-mat.mes-hall↗

Trions in MoS$_2$ are quantum superpositions of intra- and intervalley spin states

We report magneto-photoluminescence spectroscopy of gated MoS$_2$ monolayers in high magnetic fields to 28 T. At B = 0T and electron density $n_s\sim 10^{12}cm^-2$, we observe three trion resonances that cannot be explained within a single-particle picture. Employing ab initio calculations that take into account three-particle correlation effects as well as local and non-local electron-hole exchange interaction, we identify those features as quantum superpositions of inter- and intravalley spin states. We experimentally investigate the mixed character of the trion wave function via the filling factor dependent valley Zeeman shift in positive and negative magnetic fields. Our results highlight the importance of exchange interactions for exciton physics in monolayer MoS$_2$ and provide new insights into the microscopic understanding of trion physics in 2D multi-valley semiconductors for low excess carrier densities.

cond-mat.mes-hall↗

Controlling exciton many-body states by the electric-field effect in monolayer MoS$_2$

We report magneto-optical spectroscopy of gated monolayer MoS$_2$ in high magnetic fields up to 28T and obtain new insights on the many-body interaction of neutral and charged excitons with the resident charges of distinct spin and valley texture. For neutral excitons at low electron doping, we observe a nonlinear valley Zeeman shift due to dipolar spin-interactions that depends sensitively on the local carrier concentration. As the Fermi energy increases to dominate over the other relevant energy scales in the system, the magneto-optical response depends on the occupation of the fully spin-polarized Landau levels in both $K/K^{\prime}$ valleys. This manifests itself in a many-body state. Our experiments demonstrate that the exciton in monolayer semiconductors is only a single particle boson close to charge neutrality. We find that away from charge neutrality it smoothly transitions into polaronic states with a distinct spin-valley flavour that is defined by the Landau level quantized spin and valley texture.

cond-mat.mes-hall↗

Evidence for nesting driven charge density waves instabilities in a quasi-two-dimensional material: LaAgSb2

Since their theoretical prediction by Peierls in the 30s, charge density waves (CDW) have been one of the most commonly encountered electronic phases in low dimensional metallic systems. The instability mechanism originally proposed combines Fermi surface nesting and electron-phonon coupling but is, strictly speaking, only valid in one dimension. In higher dimensions, its relevance is questionable as sharp maxima in the static electronic susceptibility χ(q) are smeared out, and are, in many cases, unable to account for the periodicity of the observed charge modulations. Here, we investigate the quasi twodimensional LaAgSb2, which exhibits two CDW transitions, by a combination of diffuse xray scattering, inelastic x-ray scattering and ab initio calculations. We demonstrate that the CDW formation is driven by phonons softening. The corresponding Kohn anomalies are visualized in 3D through the momentum distribution of the x-ray diffuse scattering intensity. We show that they can be quantitatively accounted for by considering the electronic susceptibility calculated from a Dirac-like band, weighted by anisotropic electron-phonon coupling. This remarkable agreement sheds new light on the importance of Fermi surface nesting in CDW formation.

cond-mat.str-el↗

Landau level spectroscopy of PbSnSe topological crystalline insulator

We report on an infrared magneto-spectroscopy study of Pb$_{1-x}$Sn$_x$Se, a topological crystalline insulator. We have examined a set of samples, all in the inverted regime of electronic bands, with the tin composition varying from $x=0.2$ to $0.33$. Our analysis shows that the observed response, composed of a series of interband inter-Landau level excitations, can be interpreted and modelled using the relativistic-like Hamiltonian for three-dimensional massive Dirac electrons, expanded to include diagonal quadratic terms that impose band inversion. In our data, we have not found any clear signature of massless electron states that are present on the surface of Pb$_{1-x}$Sn$_x$Se crystals in the inverted regime. Reasons for this unexpected result are discussed.

cond-mat.mes-hall↗

Rydberg series of dark excitons and the conduction band spin-orbit splitting in monolayer WSe$_2$

Strong Coulomb correlations together with multi-valley electronic bands in the presence of spin-orbit interaction and possible new optoelectronic applications are at the heart of studies of the rich physics of excitons in semiconductor structures made of monolayers of transition metal dichalcogenides (TMD). In intrinsic TMD monolayers the basic, intravalley excitons are formed by a hole from the top of the valence band and an electron either from the lower or upper spin-orbit-split conduction band subbands: one of these excitons is optically active, the second one is "dark", although possibly observed under special conditions. Here we demonstrate the s-series of Rydberg dark exciton states in monolayer WSe$_2$, which appears in addition to a conventional bright exciton series in photoluminescence spectra measured in high in-plane magnetic fields. The comparison of energy ladders of bright and dark Rydberg excitons is shown to be a method to experimentally evaluate one of the missing band parameters in TMD monolayers: the amplitude of the spin-orbit splitting of the conduction band.

cond-mat.mes-hall↗

Magnetic proximity effect on excitonic spin states in Mn-doped layered hybrid perovskites

Materials combining the optoelectronic functionalities of semiconductors with control of the spin degree of freedom are highly sought after for the advancement of quantum technology devices. Here, we report the paramagnetic Ruddlesden-Popper hybrid perovskite Mn:(PEA)2PbI4 (PEA = phenethylammonium) in which the interaction of isolated Mn2+ ions with magnetically brightened excitons leads to circularly polarized photoluminescence. Using a combination of superconducting quantum interference device (SQUID) magnetometry and magneto-optical experiments, we find that the Brillouin-shaped polarization curve of the photoluminescence follows the magnetization of the material. This indicates coupling between localized manganese magnetic moments and exciton spins via a magnetic proximity effect. The saturation polarization of 15% at 4 K and 6 T indicates a highly imbalanced spin population and demonstrates that manganese doping enables efficient control of excitonic spin states in Ruddlesden-Popper perovskites. Our finding constitutes the first example of polarization control in magnetically doped hybrid perovskites and will stimulate research on this highly tuneable material platform that promises tailored interactions between magnetic moments and electronic states.

cond-mat.mtrl-sci↗

Many-body effects in suspended graphene probed through magneto-phonon resonances

We make use of micro-magneto Raman scattering spectroscopy to probe magneto-phonon resonances (MPR) in suspended mono- to penta-layer graphene. MPR correspond to avoided crossings between zone-center optical phonons (G-mode) and optically-active inter Landau level (LL) transitions and provide a tool to perform LL spectroscopy at a fixed energy ($\approx 197~\rm{meV}$) set by the G-mode phonon. Using a single-particle effective bilayer model, we readily extract the velocity parameter associated with each MPR. A single velocity parameter slightly above the bulk graphite value suffices to fit all MPR for $N\geq2$ layer systems. In contrast, in monolayer graphene, we find that the velocity parameter increases significantly from $(1.23\pm 0.01) \times 10^6~\mathrm{m.s^{-1}}$ up to $(1.45\pm0.02) \times 10^6~\mathrm{m.s^{-1}}$ as the first to third optically-active inter LL transition couple to the G-mode phonon. This result is understood as a signature of enhanced many-body effects in unscreened graphene.

cond-mat.mes-hall↗

Magnetoelastic interaction in the two-dimensional magnetic material MnPS$_3$ studied by first principles calculations and Raman experiments

We report experimental and theoretical studies on the magnetoelastic interactions in MnPS$_3$. Raman scattering response measured as a function of temperature shows a blue shift of the Raman active modes at 120.2 and 155.1 cm$^{-1}$, when the temperature is raised across the antiferromagnetic-paramagnetic transition. Density functional theory (DFT) calculations have been performed to estimate the effective exchange interactions and calculate the Raman active phonon modes. The calculations lead to the conclusion that the peculiar behavior with temperature of the two low energy phonon modes can be explained by the symmetry of their corresponding normal coordinates which involve the virtual modification of the super-exchange angles associated with the leading antiferromagnetic (AFM) interactions.

cond-mat.mes-hall↗

Time-resolved magneto-Raman study of carrier dynamics in low Landau levels of graphene

We study the relaxation dynamics of the electron system in graphene flakes under Landau quantization regime using a novel approach of time-resolved Raman scattering. The non-resonant character of the experiment allows us to analyze the field dependence of the relaxation rate. Our results clearly evidence sharp increase in the relaxation rate upon the resonance between the energy of the Landau transition and the G-band and shed new light on relaxation mechanism of the Landau-quantized electrons in graphene beyond the previously studied Auger scattering.

cond-mat.mes-hall↗

Flat Electronic Bands in Long Sequences of Rhombohedral-stacked Multilayer Graphene

The crystallographic stacking order in multilayer graphene plays an important role in determining its electronic properties. It has been predicted that a rhombohedral (ABC) stacking displays a conducting surface state with flat electronic dispersion. In such a flat band, the role of electron-electron correlation is enhanced possibly resulting in high Tc superconductivity, charge density wave or magnetic orders. Clean experimental band structure measurements of ABC stacked specimens are missing because the samples are usually too small in size. Here, we directly image the band structure of large multilayer graphene flake containing approximately 14 consecutive ABC layers. Angle-resolved photoemission spectroscopy experiments reveal the flat electronic bands near the K point extends by 0.13 Å-1 at the Fermi level at liquid nitrogen temperature. First-principle calculations identify the electronic ground state as an antiferromagnetic state with a band gap of about 40 meV.

cond-mat.mtrl-sci↗