arXiv subjects

L. Lombez

Publications and source records attributed to L. Lombez.

14 recordsLinked to original sources

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↗

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↗

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 $Δ$ between the bright and dark exciton has been measured by photoluminescence spectroscopy. We demonstrate that $Δ$ 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

Valley polarization fluctuations, bistability, and switching in two-dimensional semiconductors

We study theoretically nonlinear valley polarization dynamics of excitons in atom-thin semiconductors. The presence of significant polarization slows down valley relaxation due to an effective magnetic field resulting from exciton-exciton interactions. We address temporal dynamics of valley polarized excitons and study the steady states of the polarized exciton gas. We demonstrate bistability of the valley polarization where two steady states with low and high valley polarization are formed. We study the effects of fluctuations and noise in such system. We evaluate valley polarization autocorrelation functions and demonstrate that for a high-polarization regime the fluctuations are characterized by high amplitude and long relaxation time. We study the switching between the low- and high-valley polarized states caused by the noise in the system and demonstrate that the state with high valley polarization is preferential in a wide range of pumping rates.

cond-mat.mes-hall↗

arXiv2011

Wide range electrical tunability of single photon emission from chromium-based colour centres in diamond

We demonstrate electrical control of the single photon emission spectrum from chromium-based colour centres implanted in monolithic diamond. Under an external electric field the tunability range is typically three orders of magnitude larger than the radiative linewidth and at least one order of magnitude larger than the observed linewidth. The electric and magnetic field dependence of luminescence gives indications on the inherent symmetry and we propose Cr-X or X-Cr-Y type noncentrosymmetric atomic configurations as most probable candidates for these centres.

cond-mat.mes-hall↗

arXiv2010

Hot Carrier Solar Cells : In the Making ?

Hot carrier solar cells allow potential efficiency close to the thermodynamical limit in ideal conditions. However, the feasability of such devices has not been clearly stated so far and only ideal cells were considered in previous studies. Here we develop a model with realistic energy selective contacts, carrier thermalization and absorptivity. The requirements in term of contact selectivity is investigated, showing that semi-selective contacts are not incompatible with high efficiencies. Candidates for absorbing material were synthesized and the required thermalization properties are obtained. Specific structures were designed to enhance absorption of concentrated sunlight in a small material thickness, allowing high carrier density in the absorber.

cond-mat.mtrl-sci↗

arXiv2009

Low temperature optical characterization of near infrared single photon emitters in nanodiamonds

In this paper, we study the optical properties of single defects emitting in the near infrared in nanodiamonds at liquid helium temperature. The nanodiamonds are synthesized using a microwave chemical vapor deposition method followed by nickel implantation and annealing. We show that single defects exhibit several striking features at cryogenic temperature: the photoluminescence is strongly concentrated into a sharp zero-phonon line in the near infrared, the radiative lifetime is in the nanosecond range and the emission is perfectly linearly polarized. The spectral stability of the defects is then investigated. An optical resonance linewidth of 4 GHz is measured using resonant excitation on the zero-phonon line. Although Fourier-transform limited emission is not achieved, our results show that it might be possible to use consecutive photons emitted in the near infrared by single defects in diamond nanocrystals to perform two photon interference experiments, which are at the heart of linear quantum computing protocols.

quant-ph↗

arXiv2007

Electron spin quantum beats in positively charged quantum dots: nuclear field effects

We have studied the electron spin coherence in an ensemble of positively charged InAs/GaAs quantum dots. In a transverse magnetic field, we show that two main contributions must be taken into account to explain the damping of the circular polarization oscillations. The first one is due to the nuclear field fluctuations from dot to dot experienced by the electron spin. The second one is due to the dispersion of the transverse electron Lande g-factor, due to the inherent inhomogeneity of the system, and leads to a field dependent contribution to the damping. We have developed a model taking into account both contributions, which is in good agreement with the experimental data. This enables us to extract the pure contribution to dephasing due to the nuclei.

cond-mat.mtrl-sci↗

arXiv2007

Electrical spin injection into p-doped quantum dots through a tunnel barrier

We have demonstrated by electroluminescence the injection of spin polarized electrons through Co/Al2O3/GaAs tunnel barrier into p-doped InAs/GaAs quantum dots embedded in a PIN GaAs light emitting diode. The spin relaxation processes in the p-doped quantum dots are characterized independently by optical measurements (time and polarization resolved photoluminescence). The measured electroluminescence circular polarization is about 15 % at low temperature in a 2T magnetic field, leading to an estimation of the electrical spin injection yield of 35%. Moreover, this electroluminescence circular polarization is stable up to 70 K.

cond-mat.other↗

arXiv2006

Spin-dependent electron dynamics and recombination in GaAs(1-x)N(x) alloys at room temperature

We report on both experimental and theoretical study of conduction-electron spin polarization dynamics achieved by pulsed optical pumping at room temperature in GaAs(1-x)N(x) alloys with a small nitrogen content (x = 2.1, 2.7, 3.4%). It is found that the photoluminescence circular polarization determined by the mean spin of free electrons reaches 40-45% and this giant value persists within 2 ns. Simultaneously, the total free-electron spin decays rapidly with the characteristic time ~150 ps. The results are explained by spin-dependent capture of free conduction electrons on deep paramagnetic centers resulting in dynamical polarization of bound electrons. We have developed a nonlinear theory of spin dynamics in the coupled system of spin-polarized free and localized carriers which describes the experimental dependencies, in particular, electron spin quantum beats observed in a transverse magnetic field.

cond-mat.mtrl-sci↗