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X. Marie

Publications and source records attributed to X. Marie.

At least 37 records · Page 2Linked to original sources

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↗

Spin dependent charge transfer in MoSe2/hBN/Ni hybrid structures

We present magneto-photoluminescence measurements in a hybrid 2D semiconductor/ferromagnetic structure consisting of MoSe2/hBN/Ni. When the Nickel layer is magnetized, we observe circularly polarized photoluminescence of the trion peak in MoSe2 monolayer under linearly polarized excitation. This build-up of circular polarization can reach a measured value of about 4% when the magnetization of Ni is saturated perpendicularly to the sample plane, and changes its sign when the magnetization is reversed. The circular polarization decreases when the hBN barrier thickness increases. These results are interpreted in terms of a spin-dependent charge transfer between the MoSe2 monolayer and the Nickel film. The build-up of circular polarization is observed up to 120 K, mainly limited by the trion emission that vanishes with temperature.

cond-mat.mtrl-sci↗

Machine learning assisted GaAsN circular polarimeter

We demonstrate the application of a two stage machine learning algorithm that enables to correlate the electrical signals from a GaAs$_x$N$_{1-x}$ circular polarimeter with the intensity, degree of circular polarization and handedness of an incident light beam. Specifically, we employ a multimodal logistic regression to discriminate the handedness of light and a 6-layer neural network to establish the relationship between the input voltages, the intensity and degree of circular polarization. We have developed a particular neural network training strategy that substantially improves the accuracy of the device. The algorithm was trained and tested on theoretically generated photoconductivity and on photoluminescence experimental results. Even for a small training experimental dataset (70 instances), it is shown that the proposed algorithm correctly predicts linear, right and left circularly polarized light misclassifying less than $1.5\%$ of the cases and attains an accuracy larger than $97\%$ in the vast majority of the predictions ($92\%$) for intensity and degree of circular polarization. These numbers are significantly improved for the larger theoretically generated datasets (4851 instances). The algorithm is versatile enough that it can be easily adjusted to other device configurations where a map needs to be established between the input parameters and the device response. Training and testing data files as well as the algorithm are provided as supplementary material.

cond-mat.other↗

Chiral photodetector based on GaAsN

The detection of light helicity is key to several research and industrial applications from drugs production to optical communications. However, the direct measurement of the light helicity is inherently impossible with conventional photodetectors based on III-V or IV-VI semiconductors, being naturally non-chiral. The prior polarization analysis of the light by a series of often moving optical elements is necessary before light is sent to the detector. A method is here presented to effectively give to the conventional dilute nitride GaAs-based semiconductor epilayer a chiral photoconductivity in paramagnetic-defect-engineered samples. The detection scheme relies on the giant spin-dependent recombination of conduction electrons and the accompanying spin polarization of the engineered defects to control the conduction band population via the electrons' spin polarization. As the conduction electron spin polarization is, in turn, intimately linked to the excitation light polarization, the light polarization state can be determined by a simple conductivity measurement. This effectively gives the GaAsN epilayer a chiral photoconductivity capable of discriminating the handedness of an incident excitation light in addition to its intensity. This approach, removing the need of any optical elements in front of a non-chiral detector, could offer easier integration and miniaturisation. This new chiral photodetector could potentially operate in a spectral range from the visible to the infra-red using (In)(Al)GaAsN alloys or ion-implanted nitrogen-free III-V compounds.

physics.app-ph↗

Polarization sensitive photodectector based on GaAsN

We propose and numerically simulate an optoelectronic compact circular polarimeter. It allows to electrically measure the degree of circular polarization and light intensity at room temperature for a wide range of incidence angles in a single shot. The device, being based on GaAsN, is easy to integrate into standard electronics and does not require bulky movable parts nor extra detectors. Its operation hinges mainly on two phenomena: the spin dependent capture of electrons and the hyperfine interaction between bound electrons and nuclei on Ga$^{2+}$ paramagnetic centers in GaAsN. The first phenomenon confers the device with sensitivity to the degree of circular polarization and the latter allows to discriminate the handedness of the incident light.

cond-mat.mes-hall↗

Control of the exciton valley dynamics in van der Waals heterostructures

The exciton valley dynamics in van der Waals heterostructures with transition metal dichalcogenides monolayers is driven by the long-range exchange interaction between the electron and the hole in the exciton. It couples the states active in the opposite circular polarizations resulting in the longitudinal-transverse splitting of excitons propagating in the monolayer plane. Here we study theoretically the effect of the dielectric environment on the long-range exchange interaction and demonstrate how the encapsulation in the hexagonal boron nitride modifies the exciton longitudinal-transverse splitting. We calculate the exciton spin/valley polarization relaxation due to the long-range exchange interaction and demonstrate that the variation of the monolayer environment results in significant, up to five-fold, enhancement of the exciton valley polarization lifetime.

cond-mat.mes-hall↗

Electrical spin injection into InGaAs/GaAs quantum wells: a comparison between MgO tunnel barriers grown by sputtering and molecular beam epitaxy methods

An efficient electrical spin injection into an InGaAs/GaAs quantum well light emitting diode is demonstrated thanks to a CoFeB/MgO spin injector. The textured MgO tunnel barrier is fabricated by two different techniques: sputtering and molecular beam epitaxy (MBE). The maximal spin injection efficiency is comparable for both methods. Additionally, the effect of annealing is also investigated for the two types of samples. Both samples show the same trend: an increase of the electroluminescence circular polarization (Pc) with the increase of annealing temperature, followed by a saturation of Pc beyond 350°C annealing. Since the increase of Pc starts well below the crystallization temperature of the full CoFeB bulk layer, this trend could be mainly due to an improvement of chemical structure at the top CoFeB/MgO interface. This study reveals that the control of CoFeB/MgO interface is essential important for an optimal spin injection into semiconductor.

cond-mat.mtrl-sci↗

Measurement of the Spin-Forbidden Dark Excitons in MoS2 and MoSe2 monolayers

Excitons with binding energies of a few hundreds of meV control the optical properties of transition metal dichalcogenide monolayers. Knowledge of the fine structure of these excitons is therefore essential to understand the optoelectronic properties of these 2D materials. Here we measure the exciton fine structure of MoS2 and MoSe2 monolayers encapsulated in boron nitride by magneto-photoluminescence spectroscopy in magnetic fields up to 30 T. The experiments performed in transverse magnetic field reveal a brightening of the spin-forbidden dark excitons in MoS2 monolayer: we find that the dark excitons appear at 14 meV below the bright ones. Measurements performed in tilted magnetic field provide a conceivable description of the neutral exciton fine structure. The experimental results are in agreement with a model taking into account the effect of the exchange interaction on both the bright and dark exciton states as well as the interaction with the magnetic field.

cond-mat.mtrl-sci↗

Electron-nucleus spin correlation conservation of the spin dependent recombination in Ga$^{2+}$ centers

Spin dependent recombination in GaAsN offers many interesting possibilities in the design of spintronic devices mostly due to its astounding capability to reach conduction band electron spin polarizations close to 100% at room temperature. The mechanism behind the spin selective capture of electrons in Ga$^{2+}$ paramagnetic centers is revisited in this paper to address inconsistencies common to most previously presented models. Primarily, these errors manifest themselves as major disagreements with the experimental observations of two key characteristics of this phenomenon: the effective Overhauser-like magnetic field and the width of the photoluminescence Lorentzian-like curves as a function of the illumination power. These features are not only essential to understand the spin dependent recombination in GaAsN, but are also key to the design of novel spintronic devices. Here we demonstrate that the particular structure of the electron capture expressions introduces spurious electron-nucleus correlations that artificially alter the balance between the hyperfine and the Zeeman contributions. This imbalance strongly distorts the effective magnetic field and width characteristics. In this work we propose an alternative recombination mechanism that preserves the electron-nucleus correlations and, at the same time, keeps the essential properties of the spin selective capture of electrons. This mechanism yields a significant improvement to the agreement between experimental and theoretical results. In particular, our model gives results in very good accord with the experimental effective Overhauser-like magnetic field and width data, and with the degree of circular polarization under oblique magnetic fields.

cond-mat.mes-hall↗

Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields

In semiconductor physics, many essential optoelectronic material parameters can be experimentally revealed via optical spectroscopy in sufficiently large magnetic fields. For monolayer transition-metal dichalcogenide semiconductors, this field scale is substantial --tens of teslas or more-- due to heavy carrier masses and huge exciton binding energies. Here we report absorption spectroscopy of monolayer MoS$_2$, MoSe$_2$, MoTe$_2$, and WS$_2$ in very high magnetic fields to 91~T. We follow the diamagnetic shifts and valley Zeeman splittings of not only the exciton's $1s$ ground state but also its excited $2s$, $3s$, ..., $ns$ Rydberg states. This provides a direct experimental measure of the effective (reduced) exciton masses and dielectric properties. Exciton binding energies, exciton radii, and free-particle bandgaps are also determined. The measured exciton masses are heavier than theoretically predicted, especially for Mo-based monolayers. These results provide essential and quantitative parameters for the rational design of opto-electronic van der Waals heterostructures incorporating 2D semiconductors.

cond-mat.mes-hall↗

Control of the Exciton Radiative Lifetime in van der Waals Heterostructures

Optical properties of atomically thin transition metal dichalcogenides are controlled by robust excitons characterized by a very large oscillator strength. Encapsulation of monolayers such as MoSe$_2$ in hexagonal boron nitride (hBN) yields narrow optical transitions approaching the homogenous exciton linewidth. We demonstrate that the exciton radiative rate in these van der Waals heterostructures can be tailored by a simple change of the hBN encapsulation layer thickness as a consequence of the Purcell effect. The time-resolved photoluminescence measurements together with cw reflectivity and photoluminescence experiments show that the neutral exciton spontaneous emission time can be tuned by one order of magnitude depending on the thickness of the surrounding hBN layers. The inhibition of the radiative recombination can yield spontaneous emission time up to $10$~ps. These results are in very good agreement with the calculated recombination rate in the weak exciton-photon coupling regime. The analysis shows that we are also able to observe a sizeable enhancement of the exciton radiative decay rate. Understanding the role of these electrodynamical effects allow us to elucidate the complex dynamics of relaxation and recombination for both neutral and charged excitons.

cond-mat.mes-hall↗

Intervalley Polaron in Atomically Thin Transition Metal Dichalcogenides

We study theoretically intervalley coupling in transition-metal dichalcogenide monolayers due to electron interaction with short-wavelength phonons. We demonstrate that this intervalley polaron coupling results in (i) a renormalization of the conduction band spin splitting and (ii) an increase of the electron effective masses. We also calculate the renormalization of the cyclotron energy and the Landau level splitting in the presence of an external magnetic field. An inter-valley magneto-phonon resonance is uncovered. Similar, but much weaker effects are also expected for the valence band holes. These results might help to resolve the discrepancy between ab initio values of the electron effective masses and the ones deduced from magneto-transport measurements.

cond-mat.mes-hall↗

Exciton states in monolayer MoSe2 and MoTe2 probed by upconversion spectroscopy

Transitions metal dichalcogenides (TMDs) are direct semiconductors in the atomic monolayer (ML) limit with fascinating optical and spin-valley properties. The strong optical absorption of up to 20 % for a single ML is governed by excitons, electron-hole pairs bound by Coulomb attraction. Excited exciton states in MoSe$_2$ and MoTe$_2$ monolayers have so far been elusive due to their low oscillator strength and strong inhomogeneous broadening. Here we show that encapsulation in hexagonal boron nitride results in emission line width of the A:1$s$ exciton below 1.5 meV and 3 meV in our MoSe$_2$ and MoTe$_2$ monolayer samples, respectively. This allows us to investigate the excited exciton states by photoluminescence upconversion spectroscopy for both monolayer materials. The excitation laser is tuned into resonance with the A:1$s$ transition and we observe emission of excited exciton states up to 200 meV above the laser energy. We demonstrate bias control of the efficiency of this non-linear optical process. At the origin of upconversion our model calculations suggest an exciton-exciton (Auger) scattering mechanism specific to TMD MLs involving an excited conduction band thus generating high energy excitons with small wave-vectors. The optical transitions are further investigated by white light reflectivity, photoluminescence excitation and resonant Raman scattering confirming their origin as excited excitonic states in monolayer thin semiconductors.

cond-mat.mes-hall↗

Charged excitons in monolayer WSe$_2$: experiment and theory

Charged excitons, or X$^{\pm}$-trions, in monolayer transition metal dichalcogenides have binding energies of several tens of meV. Together with the neutral exciton X$^0$ they dominate the emission spectrum at low and elevated temperatures. We use charge tunable devices based on WSe$_2$ monolayers encapsulated in hexagonal boron nitride, to investigate the difference in binding energy between X$^+$ and X$^-$ and the X$^-$ fine structure. We find in the charge neutral regime, the X$^0$ emission accompanied at lower energy by a strong peak close to the longitudinal optical (LO) phonon energy. This peak is absent in reflectivity measurements, where only the X$^0$ and an excited state of the X$^0$ are visible. In the $n$-doped regime, we find a closer correspondence between emission and reflectivity as the trion transition with a well-resolved fine-structure splitting of 6~meV for X$^-$ is observed. We present a symmetry analysis of the different X$^+$ and X$^-$ trion states and results of the binding energy calculations. We compare the trion binding energy for the $n$-and $p$-doped regimes with our model calculations for low carrier concentrations. We demonstrate that the splitting between the X$^+$ and X$^-$ trions as well as the fine structure of the X$^-$ state can be related to the short-range Coulomb exchange interaction between the charge carriers.

cond-mat.mes-hall↗

Spectrally narrow exciton luminescence from monolayer MoS2 exfoliated onto epitaxially grown hexagonal BN

The strong light-matter interaction in transition Metal dichalcogenides (TMDs) monolayers (MLs) is governed by robust excitons. Important progress has been made to control the dielectric environment surrounding the MLs, especially through hexagonal boron nitride (hBN) encapsulation, which drastically reduces the inhomogeneous contribution to the exciton linewidth. Most studies use exfoliated hBN from high quality flakes grown under high pressure. In this work, we show that hBN grown by molecular beam epitaxy (MBE) over a large surface area substrate has a similarly positive impact on the optical emission from TMD MLs. We deposit MoS$_2$ and MoSe$_2$ MLs on ultrathin hBN films (few MLs thick) grown on Ni/MgO(111) by MBE. Then we cover them with exfoliated hBN to finally obtain an encapsulated sample : exfoliated hBN/TMD ML/MBE hBN. We observe an improved optical quality of our samples compared to TMD MLs exfoliated directly on SiO$_2$ substrates. Our results suggest that hBN grown by MBE could be used as a flat and charge free substrate for fabricating TMD-based heterostructures on a larger scale.

cond-mat.mtrl-sci↗

Exciton-phonon coupling in MoSe2 monolayers

We study experimentally and theoretically the exciton-phonon interaction in MoSe2 monolayers encapsulated in hexagonal BN, which has an important impact on both optical absorption and emission processes. The exciton transition linewidth down to 1 meV at low temperatures makes it possible to observe high energy tails in absorption and emission extending over several meV, not masked by inhomogeneous broadening. We develop an analytical theory of the exciton-phonon interaction accounting for the deformation potential induced by the longitudinal acoustic phonons, which plays an important role in exciton formation. The theory allows fitting absorption and emission spectra and permits estimating the deformation potential in MoSe2 monolayers. We underline the reasons why exciton-phonon coupling is much stronger in two-dimensional transition metal dichalcodenides as compared to conventional quantum well structures. The importance of exciton-phonon interactions is further highlighted by the observation of a multitude of Raman features in the photoluminescence excitation experiments.

cond-mat.mtrl-sci↗

Electrically tunable dynamic nuclear spin polarization in GaAs quantum dots at zero magnetic field

In III-V semiconductor nano-structures the electron and nuclear spin dynamics are strongly coupled. Both spin systems can be controlled optically. The nuclear spin dynamics is widely studied, but little is known about the initialization mechanisms. Here we investigate optical pumping of carrier and nuclear spins in charge tunable GaAs dots grown on 111A substrates. We demonstrate dynamic nuclear polarization (DNP) at zero magnetic field in a single quantum dot for the positively charged exciton X$^+$ state transition. We tune the DNP in both amplitude and sign by variation of an applied bias voltage V$_g$. Variation of $Δ$V$_g$ of the order of 100 mV changes the Overhauser splitting (nuclear spin polarization) from -30 $μ$eV (-22 %) to +10 $μ$eV (+7 %), although the X$^+$ photoluminescence polarization does not change sign over this voltage range. This indicates that absorption in the structure and energy relaxation towards the X$^+$ ground state might provide favourable scenarios for efficient electron-nuclear spin flip-flops, generating DNP during the first tens of ps of the X$^+$ lifetime which is of the order of hundreds of ps. Voltage control of DNP is further confirmed in Hanle experiments.

cond-mat.mes-hall↗

Electrical initialization of electron and nuclear spins in a single quantum dot at zero magnetic field

The emission of circularly polarized light from a single quantum dot relies on the injection of carriers with well-defined spin polarization. Here we demonstrate single dot electroluminescence (EL) with a circular polarization degree up to 35% at zero applied magnetic field. The injection of spin polarized electrons is achieved by combining ultrathin CoFeB electrodes on top of a spin-LED device with p-type InGaAs quantum dots in the active region. We measure an Overhauser shift of several $μ$eV at zero magnetic field for the positively charged exciton (trion X$^+$) EL emission, which changes sign as we reverse the injected electron spin orientation. This is a signature of dynamic polarization of the nuclear spins in the quantum dot induced by the hyperfine interaction with the electrically injected electron spin. This study paves the way for electrical control of nuclear spin polarization in a single quantum dot without any external magnetic field.

cond-mat.mes-hall↗