arXiv subjects

X. Marie

Publications and source records attributed to X. Marie.

At least 19 recordsLinked to original sources

arXiv2026

Spin-Valley Relaxation of Rydberg Excitons

Rydberg excitons, characterized by large spatial extension and reduced electron-hole overlap, must have a spin-valley dynamics different from that of ground state excitons. Here we report a direct measurement of spin relaxation of Rydberg excitons in high-quality WSe2 monolayer using continuous-wave and time-resolved optical orientation experiments. Excited excitonic states exhibit exceptionally large photoluminescence circular polarization, approaching 90% for the 3s state. Time-resolved measurements reveal a strong increase of the spin relaxation time with the principal quantum number, from ~2 ps for the 1s exciton to ~75 ps for the 3s exciton. A microscopic model based on electron-hole exchange-driven spin relaxation quantitatively reproduces the observed trend, demonstrating that Rydberg excitons enable tunable spin-valley dynamics in two-dimensional semiconductors.

cond-mat.other↗

arXiv2025

2D Excitonics with Atomically Thin Lateral Heterostructures

Semiconducting transition metal dichalcogenides (TMDs), such as MoSe$_2$ and WSe$_2$, exhibit unique optical and electronic properties. Vertical stacking of layers of one or more TMDs, to create heterostructures, has expanded the fields of moir\'e physics and twistronics. Bottom-up fabrication techniques, such as chemical vapor deposition, have advanced the creation of heterostructures beyond what was possible with mechanical exfoliation and stacking. These techniques now enable the fabrication of lateral heterostructures, where two or more monolayers are covalently bonded in the plane of their atoms. At their atomically sharp interfaces, lateral heterostructures exhibit additional phenomena, such as the formation of charge-transfer excitons, in which the electron and hole reside on opposite sides of the interface. Due to the energy landscape created by differences in the band structures of the constituent materials, unique effects such as unidirectional exciton transport and excitonic lensing can be observed in lateral heterostructures. This review outlines recent progress in exciton dynamics and spectroscopy of TMD-based lateral heterostructures and offers an outlook on future developments in excitonics in this promising system.

cond-mat.mtrl-sci↗

arXiv2025

Exciton Formation in Two-Dimensional Semiconductors

The optical properties of atomically thin semiconductors are dominated by excitons, tightly bound electron-hole pairs, which give rise to particularly rich and remarkable physics. Despite their importance, the microscopic formation mechanisms of excitons remain very poorly understood due to the complex interplay of concurrent phenomena occurring on an ultrafast timescale. Here, we investigate the exciton formation processes in 2D materials based on transition metal dichalcogenide (TMD) monolayers using a technique based on the control of excitation light polarization. It allows us to distinguish between the two competing models of exciton formation: geminate and bimolecular formation. The geminate process is the direct formation of the exciton from the initially photogenerated electron hole pair before the loss of correlation between them, whereas the bimolecular process corresponds to the random binding of free electron hole-pairs from the initially photogenerated plasma. These processes control the exciton formation time. Our findings reveal that the luminescence intensity is higher by up to 40% for circularly polarized excitation compared to linearly polarized excitation for laser energy above the free carrier gap. We show that this spin-dependent exciton emission is a fingerprint of the bimolecular formation process. Importantly, we observe that exciton linear polarization (valley coherence) persists even for laser excitation energies exceeding the gap. We demonstrate that it is the result of a fraction of excitons formed by a geminate process. This shows that two formation processes coexist for excitation energies above the gap, where both mechanisms operate concurrently.

cond-mat.mtrl-sci↗

arXiv2025

Interlayer Coupling and Exciton Dynamics in 2D Hybrid Structures based on an InGaN Quantum Well coupled to a MoSe2 Monolayer

Hybrid structures incorpora1ng both III-nitride and Transi1on Metal Dichalcogenide (TMD) semiconductors have strong applica1on poten1al for light harves1ng and optoelectronics. Here we have inves1gated the proper1es of hybrid structures based on a MoSe2 monolayer coupled to an InGaN quantum well (QW). The coupling efficiency is controlled by a thin GaN barrier of variable thickness located between them. Time-integrated and 1me-resolved micro-photoluminescence experiments show a quenching of the InGaN QW exciton emission which increases with the decrease of the GaN barrier thickness d: the PL intensity is reduced by a factor 3 for d=1 nm as a consequence of carrier transfer to the MoSe2 monolayer. This interplay between the two semiconductors is confirmed by 1meresolved photoluminescence spectroscopy highligh1ng a clear reduc1on of the QW exciton life1me in the presence of the monolayer. Interes1ngly the coupling between the QW and the TMD monolayer is also demonstrated by measuring op1cally the excitonic transport proper1es in the quantum well: the exciton diffusion length decreases in the presence of the MoSe2 monolayer. The measured dependences as a func1on of temperature highlight the role played by localiza1on effects in the QW. All these results can be well interpreted by a type II band alignment between the InGaN QW and the MoSe2 monolayer and a tunneling process between the two semiconductors.

cond-mat.mtrl-sci↗

arXiv2025

Spin-valley polarization control in WSe$_2$ monolayers using photochemical doping

We report on the influence of a photochemical doping method on the spin-valley polarization degree ($P_{c}$) of excitons in WSe$_2$ monolayers. By varying the carrier density and transitioning from an excess of electrons (n-type) to an excess of holes (p-type), we observe a non-monotonic dependence of $P_{c}$ on the doping level. Using controlled, single-shot photochlorination steps, we unveil this non-monotonic behavior, with $P_{c}$ reaching a minimum value of less than 10$\%$ at 78 K near the charge neutrality point, while increasing by a factor of three at a hole density of $5 \times 10^{11} \,\mathrm{cm^{-2}}$. The impact of the doping on $P_{c}$ is explained using a phenomenological model that accounts for various mechanisms influencing exciton polarization dynamics, including exciton-carrier scattering processes and exciton-to-trion conversion rates. Among these, exciton-carrier collisions emerge as the dominant mechanism driving the observed variations in $P_{c}$, while the exciton effective lifetime remains nearly independent of doping. These findings highlight the potential of photochemical methods for investigating valley physics and for effectively tuning the exciton polarization degree in transition metal dichalcogenide monolayers.

cond-mat.mes-hall↗

arXiv2025

Magnetic imaging under high pressure with a spin-based quantum sensor integrated in a van der Waals heterostructure

Pressure is a powerful thermodynamic parameter for tuning the magnetic properties of van der Waals magnets owing to their weak interlayer bonding. However, local magnetometry measurements under high pressure still remain elusive for this important class of emerging materials. Here we introduce a method enabling in situ magnetic imaging of van der Waals magnets under high pressure with sub-micron spatial resolution. Our approach relies on a quantum sensing platform based on boron-vacancy (V$_\text{B}^-$) centers in hexagonal boron nitride (hBN), which can be placed in atomic contact of any type of two-dimensional (2D) material within a van der Waals heterostructure. We first show that the V$_\text{B}^-$ center can be used as a magnetic field sensor up to pressures of a few GPa, a pressure range for which the properties of a wide variety of van der Waals magnets are efficiently altered. We then use V$_\text{B}^-$ centers in a thin hBN layer to perform magnetic imaging of a van der Waals magnet under pressure. As a proof of concept, we study the pressure-dependent magnetization in micrometer-sized flakes of $1T$-CrTe$_2$, whose evolution is explained by a shift of the Curie temperature. Besides providing a new path for studying pressure-induced phase transitions in van der Waals magnets, this work also opens up interesting perspectives for exploring the physics of 2D superconductors under pressure via local measurements of the Meissner effect.

cond-mat.mtrl-sci↗

arXiv2024

Enhanced optical properties of MoSe$_2$ grown by molecular beam epitaxy on hexagonal boron nitride

Transition metal dichalcogenides (TMD) like MoSe$_2$ exhibit remarkable optical properties such as intense photoluminescence (PL) in the monolayer form. To date, narrow-linewidth PL is only achieved in micrometer-sized exfoliated TMD flakes encapsulated in hexagonal boron nitride (hBN). In this work, we develop a growth strategy to prepare monolayer MoSe$_2$ on hBN flakes by molecular beam epitaxy in the van der Waals regime. It constitutes the first step towards the development of large area single crystalline TMDs encapsulated in hBN for potential integration in electronic or opto-electronic devices. For this purpose, we define a two-step growth strategy to achieve monolayer-thick MoSe$_2$ grains on hBN flakes. The high quality of MoSe$_2$ allows us to detect very narrow PL linewidth down to 5.5 meV at 13 K, comparable to the one of encapsulated exfoliated MoSe$_2$ flakes. Moreover, sizeable PL can be detected at room temperature as well as clear reflectivity signatures of A, B and charged excitons.

cond-mat.mtrl-sci↗

arXiv2024

Efficient Electron Spin Relaxation by Chiral Phonons in WSe$_2$ Monolayers

In transition metal dichalcogenide semiconductor monolayers the spin dynamics of electrons is controlled by the original spin-valley locking effect resulting from the interplay between spin-orbit interaction and inversion asymmetry. As a consequence, for electrons occupying bottom conduction bands, a carrier spin flip occurs only if there is a simultaneous change of valley. However, very little is known about the intra-valley spin relaxation processes. In this work we have performed stationary and time-resolved photoluminescence measurements in high quality WSe$_2$ monolayers. Our experiments highlight an efficient relaxation from bright to dark excitons, due to a fast intra-valley electron transfer from the top to the bottom conduction band with opposite spins. A combination of experiments and theoretical analysis allows us to infer a spin relaxation time of about $\tau_s\sim10~$ps, driven by the interplay between $\Gamma$-valley chiral phonons and spin-orbit mixing.

cond-mat.mes-hall↗

arXiv2024

Brightened emission of dark trions in transition-metal dichalcogenide monolayers

The optical emission spectra of semiconducting transition-metal dichalcogenide monolayers highlight fascinating recombination processes of charged excitons (trions). When charge tunable WSe$_2$ monolayers are moderately doped with electrons, a strong luminescence peak emerges just below the well-understood spectral lines associated with the recombination of negatively charged bright and dark trions. Despite previous investigations, its origin remains elusive. Here, we demonstrate that this luminescence peak is the result of electron-electron assisted recombination that brightens the dark trion emission. Supporting evidence for this second-order recombination process comes from identifying the brightened emission of positively charged dark trions when the monolayer is electrostatically doped with holes. Remarkably, the discovered hole-hole assisted luminescence peak emerges in the near infrared, about 500 meV below the well-studied spectral region of excitons and trions. In magneto-photoluminescence experiments we find that the $g$-factor of this new transition ($g$ = +4) has an opposite sign compared to the well-known $g$-factor of neutral or charged excitons. This allows us to propose a mechanism of brightening of the positively charged dark trion involving the $\Gamma$ valence band.

cond-mat.mes-hall↗

arXiv2024

Spin-dependent photodynamics of boron-vacancy centers in hexagonal boron nitride

The negatively-charged boron vacancy (V$_\text{B}^-$) center in hexagonal boron nitride (hBN) is currently garnering considerable attention for the design of two-dimensional (2D) quantum sensing units. Such developments require a precise understanding of the spin-dependent optical response of V$_\text{B}^-$ centers, which still remains poorly documented despite its key role for sensing applications. Here we investigate the spin-dependent photodynamics of V$_\text{B}^-$ centers in hBN by a series of time-resolved photoluminescence (PL) measurements. We first introduce a robust all-optical method to infer the spin-dependent lifetime of the excited states and the electron spin polarization of V$_\text{B}^-$ centers under optical pumping. Using these results, we then analyze PL time traces recorded at different optical excitation powers with a seven-level model of the V$_\text{B}^-$ center and we extract all the rates involved in the spin-dependent optical cycles, both under ambient conditions and at liquid helium temperature. These findings are finally used to study the impact of a vector magnetic field on the optical response. More precisely, we analyze PL quenching effects resulting from electron spin mixing induced by the magnetic field component perpendicular to the V$_\text{B}^-$ quantization axis. All experimental results are well reproduced by the seven-level model, illustrating its robustness to describe the spin-dependent photodymanics of V$_\text{B}^-$ centers. This work provides important insights into the properties of V$_\text{B}^-$ centers in hBN, which are valuable for future developments of 2D quantum sensing units.

cond-mat.mtrl-sci↗

arXiv2023

Biaxial strain tuning of exciton energy and polarization in monolayer WS2

We perform micro-photoluminescence and Raman experiments to examine the impact of biaxial tensile strain on the optical properties of WS2 monolayers. A strong shift on the order of -130 meV per % of strain is observed in the neutral exciton emission at room temperature. Under near-resonant excitation we measure a monotonic decrease in the circular polarization degree under applied strain. We experimentally separate the effect of the strain-induced energy detuning and evaluate the pure effect coming from biaxial strain. The analysis shows that the suppression of the circular polarization degree under biaxial strain is related to an interplay of energy and polarization relaxation channels as well as to variations in the exciton oscillator strength affecting the long-range exchange interaction.

cond-mat.mtrl-sci↗

arXiv2023

Isotopic control of the boron-vacancy spin defect in hexagonal boron nitride

We report on electron spin resonance (ESR) spectroscopy of boron-vacancy (V$_\text{B}^-$) centers hosted in isotopically-engineered hexagonal boron nitride (hBN) crystals. We first show that isotopic purification of hBN with $^{15}$N yields a simplified and well-resolved hyperfine structure of V$_\text{B}^-$ centers, while purification with $^{10}$B leads to narrower ESR linewidths. These results establish isotopically-purified h$^{10}$B$^{15}$N crystals as the optimal host material for future use of V$_\text{B}^-$ spin defects in quantum technologies. Capitalizing on these findings, we then demonstrate optically-induced polarization of $^{15}$N nuclei in h$^{10}$B$^{15}$N, whose mechanism relies on electron-nuclear spin mixing in the V$_\text{B}^-$ ground state. This work opens up new prospects for future developments of spin-based quantum sensors and simulators on a two-dimensional material platform.

quant-ph↗

arXiv2023

Electrostatic modulation of excitonic fluid in GaN/AlGaN quantum wells by deposition of few-layered graphene and nickel/gold films

Excitons hosted by GaN/(Al,Ga)N quantum wells (QWs) are spatially indirect due to the giant built-in electric field that separates electrons and holes along the growth direction. This electric field, and thus exciton energy, can be reduced by depositing metallic layers on the sample surface. Using spatially-resolved micro-photoluminescence spectroscopy we compare the effects of two different materials, Nickel/Gold (NiAu) and few-layered graphene (FLG), on the potential landscape experienced by the excitons. We are able to (i) determine the potential barriers imposed on QW excitons by deposition of FLG and NiAu to be $14$ and $82$~meV, respectively, and (ii) to evidence their impact on the exciton transport at appropriate densities. Optical losses and inhomogeneous broadening induced by deposition of NiAu and FLG layers are similar, and their joined implementation constitute a promising tool for electrostatic modulation of IX densities even in the absence of any applied electric bias.

cond-mat.quant-gas↗

arXiv2023

Optically-active spin defects in few-layer thick hexagonal boron nitride

Optically-active spin defects in hexagonal boron nitride (hBN) are promising quantum systems for the design of two-dimensional quantum sensing units offering optimal proximity to the sample being probed. In this work, we first demonstrate that the electron spin resonance frequencies of boron vacancy centres (V$_\text{B}^-$) can be detected optically in the limit of few-atomic-layer thick hBN flakes despite the nanoscale proximity of the crystal surface that often leads to a degradation of the stability of solid-state spin defects. We then analyze the variations of the electronic spin properties of V$_\text{B}^-$ centres with the hBN thickness with a focus on (i) the zero-field splitting parameters, (ii) the optically-induced spin polarization rate and (iii) the longitudinal spin relaxation time. This work provides important insights into the properties of V$_\text{B}^-$ centres embedded in ultrathin hBN flakes, which are valuable for future developments of foil-based quantum sensing technologies.

quant-ph↗

arXiv2023

Control of the Bright-Dark Exciton Splitting using Lamb Shift in a 2D Semiconductor

We have investigated the exciton fine structure in atomically thin WSe2 -based van der Waals heterostructures where the density of optical modes at the location of the semiconductor monolayer can be tuned. The energy splitting $\Delta$ between the bright and dark exciton has been measured by photoluminescence spectroscopy. We demonstrate that $\Delta$ can be tuned by a few meV, as a result of a significant Lamb shift of the optically active exciton which arises from emission and absorption of virtual photons triggered by the vacuum fluctuations of the electromagnetic field. We also measured strong variations of the bright exciton radiative linewidth, as a result of the Purcell effect. All these experimental results illustrate the strong sensitivity of the excitons to local vacuum field. We found a very good agreement with a model that demonstrates the equivalence, for our system, of a classical electrodynamical transfer matrix formalism and quantum-electrodynamical approach. The bright-dark splitting control demonstrated here should apply to any semiconductor structures.

cond-mat.mes-hall↗

arXiv2022

Non-linear diffusion of negatively charged excitons in WSe2 monolayer

We investigate the diffusion process of negatively charged excitons (trions) in WSe2 transition metal dichalcogenide monolayer. We measure time-resolved photoluminescence spatial profiles of these excitonic complexes which exhibit a non-linear diffusion process with an effective negative diffusion behavior. Specifically, we examine the dynamics of the two negatively charged bright excitons (intervalley and intravalley trion) as well as the dark trion. The time evolution allows us to identify the interplay of different excitonic species: the trionic species appear after the neutral excitonic ones, consistent with a bimolecular formation mechanism. Using the experimental observations, we propose a phenomenological model suggesting the coexistence of two populations: a first one exhibiting a fast and efficient diffusion mechanism and a second one with a slower dynamics and a less efficient diffusion process. These two contributions could be attributed to hot and cold trion populations.

cond-mat.mtrl-sci↗

arXiv2022

Magnetic imaging with spin defects in hexagonal boron nitride

Optically-active spin defects hosted in hexagonal boron nitride (hBN) are promising candidates for the development of a two-dimensional (2D) quantum sensing unit. Here, we demonstrate quantitative magnetic imaging with hBN flakes doped with negatively-charged boron-vacancy (V$_{\rm B}^-$) centers through neutron irradiation. As a proof-of-concept, we image the magnetic field produced by CrTe$_2$, a van der Waals ferromagnet with a Curie temperature slightly above $300$ K. Compared to other quantum sensors embedded in 3D materials, the advantages of the hBN-based magnetic sensor described in this work are its ease of use, high flexibility and, more importantly, its ability to be placed in close proximity to a target sample. Such a sensing unit will likely find numerous applications in 2D materials research by offering a simple way to probe the physics of van der Waals heterostructures.

cond-mat.mtrl-sci↗

arXiv2022

Optical manipulation of the Rashba effect in germanium quantum wells

The Rashba effect in Ge/Si$_{0.15}$Ge$_{0.85}$ multiple quantum wells embedded in a p-i-n diode is studied through polarization and time-resolved photoluminescence. In addition to a sizeable redshift arising from the quantum-confined Stark effect, a threefold enhancement of the circular polarization degree of the direct transition is obtained by increasing the pump power over a 2kW/cm$^2$ range. This marked variation reflects an efficient modulation of the spin population and is further supported by dedicated investigations of the indirect gap transition. This study demonstrates a viable strategy to engineer the spin-orbit Hamiltonian through contactless optical excitation and opens the way towards the electro-optical manipulation of spins in quantum devices based on group-IV heterostructures.

cond-mat.mes-hall↗