arXiv subjects

Xavier Marie

Publications and source records attributed to Xavier Marie.

69 records · Page 4Linked to original sources

arXiv2017

Identifying optical signatures of momentum-dark excitons in transition metal dichalcogenide monolayers

Transition metal dichalcogenide (TMD) monolayers (MLs) exhibit rich photoluminescence spectra associated with interband optical transitions of direct-gap semiconductors. Upon absorption of photons, direct excitons with zero center-of-mass momentum are formed by photo-excited electrons in the conduction band and the respective unoccupied states in the valence band of the same valley. Different spin configurations of such momentum-direct excitons as well as their charged counterparts provide a powerful platform for spin-valley and microcavity physics in two-dimensional materials. The corresponding spectral signatures, however, are insufficient to explain the main characteristic peaks observed in the photoluminescence spectra of ML TMDs on the basis of momentum-\textit{direct} excitons alone. Here, we show that the notion of momentum-\textit{indirect} excitons is important for the understanding of the versatile photoluminescence features. Taking into account phonon-assisted radiative recombination pathways for electrons and holes from dissimilar valleys, we interpret unidentified peaks in the emission spectra as acoustic and optical phonon sidebands of momentum-dark excitons. Our approach will facilitate the interpretation of optical, valley and spin phenomena in TMDs arising from bright and dark exciton manifolds.

cond-mat.mes-hall↗

arXiv2017

Carrier and Spin Coherent Dynamics in Strained Germanium-Tin Semiconductor on Silicon

Germanium-Tin is emerging as a material exhibiting excellent photonic properties. Here we demonstrate optical initialization and readout of spins in this intriguing group IV semiconductor alloy and report on spin quantum beats between Zeeman-split levels under an external magnetic field. Our optical experiments reveal robust spin orientation in a wide temperature range and a persistent spin lifetime that approaches the ns regime at room temperature. Besides important insights into nonradiative recombination pathways, our findings disclose a rich spin physics in novel epitaxial structures directly grown on a conventional Si substrate. This introduces a viable route towards the synergic enrichment of the group IV semiconductor toolbox with advanced spintronics and photonic capabilities.

cond-mat.mtrl-sci↗

arXiv2017

Synthesis of Highly Anisotropic Semiconducting GaTe Nanomaterials and Emerging Properties Enabled by Epitaxy

Pseudo-one dimensional (pseudo-1D) materials are a new-class of materials where atoms are arranged in chain like structures in two-dimensions (2D). Examples include recently discovered black phosphorus, ReS2 and ReSe2 from transition metal dichalcogenides, TiS3 and ZrS3 from transition metal trichalcogenides and most recently GaTe. The presence of structural anisotropy impacts their physical properties and leads to direction dependent light-matter interactions, dichroic optical responses, high mobility channels, and anisotropic thermal conduction. Despite the numerous reports on the vapor phase growth of isotropic TMDCs and post transition metal chalcogenides such as MoS2 and GaSe, the synthesis of pseudo-1D materials is particularly difficult due to the anisotropy in interfacial energy, which stabilizes dendritic growth rather than single crystalline growth with well-defined orientation. The growth of monoclinic GaTe has been demonstrated on flexible mica substrates with superior photodetecting performance. In this work, we demonstrate that pseudo-1D monoclinic GaTe layers can be synthesized on a variety of other substrates including GaAs (111), Si (111) and c-cut sapphire by physical vapor transport techniques. High resolution transmission electron microscopy (HRTEM) measurements, together with angle resolved micro-PL and micro-Raman techniques, provide for the very first time atomic scale resolution experiments on pseudo-1D structures in monoclinic GaTe and anisotropic properties. Interestingly, GaTe nanomaterials grown on sapphire exhibit highly efficient and narrow localized emission peaks below the band gap energy, which are found to be related to select types of line and point defects as evidenced by PL and Raman mapping scans. It makes the samples grown on sapphire more prominent than those grown on GaAs and Si, which demonstrate more regular properties.

cond-mat.mtrl-sci↗

arXiv2016

Ultra-low power threshold for laser induced changes in optical properties of 2D Molybdenum dichalcogenides

The optical response of traditional semiconductors depends on the laser excitation power used in experiments. For two-dimensional (2D) semiconductors, laser excitation effects are anticipated to be vastly different due to complexity added by their ultimate thinness, high surface to volume ratio, and laser-membrane interaction effects. We show in this article that under laser excitation the optical properties of 2D materials undergo irreversible changes. Most surprisingly these effects take place even at low steady state excitation, which is commonly thought to be non-intrusive. In low temperature photoluminescence (PL) we show for monolayer (ML) MoSe2 samples grown by different techniques that laser treatment increases significantly the trion (i.e. charged exciton) contribution to the emission compared to the neutral exciton emission. Comparison between samples exfoliated onto different substrates shows that laser induced doping is more efficient for ML MoSe2 on SiO2/Si compared to h-BN and gold. For ML MoS2 we show that exposure to laser radiation with an average power in the $μ$W/$μ$m$^2$ range does not just increase the trion-to-exciton PL emission ratio, but may result in the irreversible disappearance of the neutral exciton PL emission and a shift of the main PL peak to lower energy.

cond-mat.mtrl-sci↗

arXiv2016

Well separated trion and neutral excitons on superacid treated MoS2 monolayers

Developments in optoelectronics and spin-optronics based on transition metal dichalcogenide monolayers (MLs) need materials with efficient optical emission and well-defined transition energies. In as-exfoliated MoS2 MLs the photoluminescence (PL) spectra even at low temperature consists typically of broad, overlapping contributions from neutral, charged excitons (trions) and localized states. Here we show that in superacid treated MoS2 MLs the PL intensity increases by up to 60 times at room temperature. The neutral and charged exciton transitions are spectrally well separated in PL and reflectivity at T=4 K, with linewidth for the neutral exciton of 15 meV, but with similar intensities compared to the ones in as-exfoliated MLs at the same temperature. Time resolved experiments uncover picoseconds recombination dynamics analyzed separately for charged and neutral exciton emission. Using the chiral interband selection rules, we demonstrate optically induced valley polarization for both complexes and valley coherence for only the neutral exciton.

cond-mat.mtrl-sci↗

arXiv2016

Discrete quantum dot like emitters in monolayer MoSe2: Spatial mapping, Magneto-optics and Charge tuning

Transition metal dichalcogenide monolayers such as MoSe2,MoS2 and WSe2 are direct bandgap semiconductors with original optoelectronic and spin-valley properties. Here we report spectrally sharp, spatially localized emission in monolayer MoSe2. We find this quantum dot like emission in samples exfoliated onto gold substrates and also suspended flakes. Spatial mapping shows a correlation between the location of emitters and the existence of wrinkles (strained regions) in the flake. We tune the emission properties in magnetic and electric fields applied perpendicular to the monolayer plane. We extract an exciton g-factor of the discrete emitters close to -4, as for 2D excitons in this material. In a charge tunable sample we record discrete jumps on the meV scale as charges are added to the emitter when changing the applied voltage. The control of the emission properties of these quantum dot like emitters paves the way for further engineering of the light matter interaction in these atomically thin materials.

cond-mat.mtrl-sci↗

arXiv2015

Spin-orbit engineering in transition metal dichalcogenide alloy monolayers

Transition metal dichalcogenide (TMDC) monolayers are newly discovered semiconductors for a wide range of applications in electronics and optoelectronics. Most studies have focused on binary monolayers that share common properties: direct optical bandgap, spin-orbit (SO) splittings of hundreds of meV, light-matter interaction dominated by robust excitons and coupled spin-valley states of electrons. Studies on alloy-based monolayers are more recent, yet they may not only extend the possibilities for TMDC applications through specific engineering but also help understanding the differences between each binary material. Here, we synthesized highly crystalline Mo$_{(1-x)}$W$_{x}$Se$_2$ to show engineering of the direct optical bandgap and the SO coupling in ternary alloy monolayers. We investigate the impact of the tuning of the SO spin splitting on the optical and polarization properties. We show a non-linear increase of the optically generated valley polarization as a function of tungsten concentration, where 40% tungsten incorporation is sufficient to achieve valley polarization as high as in binary WSe2. We also probe the impact of the tuning of the conduction band SO spin splitting on the bright versus dark state population i.e. PL emission intensity. We show that the MoSe2 PL intensity decreases as a function of temperature by an order of magnitude, whereas for WSe2 we measure surprisingly an order of magnitude increase over the same temperature range (T=4-300K). The ternary material shows a trend between these two extreme behaviors. These results show the strong potential of SO engineering in ternary TMDC alloys for optoelectronics and applications based on electron spin- and valley-control.

cond-mat.mtrl-sci↗

arXiv2015

Optical orientation of electron spins and valence band spectroscopy in germanium

We have investigated optical orientation in the vicinity of the direct gap of bulk germanium. The electron spin polarization is studied via polarization-resolved photoluminescence excitation spectroscopy unfolding the interplay between doping and ultrafast electron transfer from the center of the Brillouin zone towards its edge. As a result, the direct-gap photoluminescence circular polarisation can vary from 30% to -60% when the excitation laser energy increases. This study provides also simultaneous access to the resonant electronic Raman scattering due to inter-valence band excitations of spin-polarized holes, yielding a fast and versatile spectroscopic approach for the determination of the energy spectrum of holes in semiconducting materials.

cond-mat.mes-hall↗

arXiv2014

Investigation of the anisotropic electron g factor as a probe of the electronic structure of GaBi$_{x}$As$_{1-x}$/GaAs epilayers

The electron Landé g factor ($g^{*}$) is investigated both experimentally and theoretically in a series of GaBi$_{x}$As$_{1-x}$/GaAs strained epitaxial layers, for bismuth compositions up to $x = 3.8$%. We measure $g^{*}$ via time-resolved photoluminescence spectroscopy, which we use to analyze the spin quantum beats in the polarization of the photoluminescence in the presence of an externally applied magnetic field. The experimental measurements are compared directly to atomistic tight-binding calculations on large supercells, which allows us to explicitly account for alloy disorder effects. We demonstrate that the magnitude of $g^{*}$ increases strongly with increasing Bi composition $x$ and, based on the agreement between the theoretical calculations and experimental measurements, elucidate the underlying causes of the observed variation of $g^{*}$. By performing measurements in which the orientation of the applied magnetic field is changed, we further demonstrate that $g^{*}$ is strongly anisotropic. We quantify the observed variation of $g^{*}$ with $x$, and its anisotropy, in terms of a combination of epitaxial strain and Bi-induced hybridization of valence states due to alloy disorder, which strongly perturbs the electronic structure.

cond-mat.mtrl-sci↗

arXiv2012

Nuclear spin physics in quantum dots: an optical investigation

The mesoscopic spin system formed by the 10E4-10E6 nuclear spins in a semiconductor quantum dot offers a unique setting for the study of many-body spin physics in the condensed matter. The dynamics of this system and its coupling to electron spins is fundamentally different from its bulk counter-part as well as that of atoms due to increased fluctuations that result from reduced dimensions. In recent years, the interest in studying quantum dot nuclear spin systems and their coupling to confined electron spins has been fueled by its direct implication for possible applications of such systems in quantum information processing as well as by the fascinating nonlinear (quantum-)dynamics of the coupled electron-nuclear spin system. In this article, we review experimental work performed over the last decades in studying this mesoscopic,coupled electron-nuclear spin system and discuss how optical addressing of electron spins can be exploited to manipulate and read-out quantum dot nuclei. We discuss how such techniques have been applied in quantum dots to efficiently establish a non-zero mean nuclear spin polarization and, most recently, were used to reduce fluctuations of the average quantum dot nuclear spin orientation. Both results in turn have important implications for the preservation of electron spin coherence in quantum dots, which we discuss. We conclude by speculating how this recently gained understanding of the quantum dot nuclear spin system could in the future enable experimental observation of quantum-mechanical signatures or possible collective behavior of mesoscopic nuclear spin ensembles.

cond-mat.mes-hall↗

arXiv2010

Impact of heavy hole-light hole coupling on optical selection rules in GaAs quantum dots

We report strong heavy hole-light mixing in GaAs quantum dots grown by droplet epitaxy. Using the neutral and charged exciton emission as a monitor we observe the direct consequence of quantum dot symmetry reduction in this strain free system. By fitting the polar diagram of the emission with simple analytical expressions obtained from k$\cdot$p theory we are able to extract the mixing that arises from the heavy-light hole coupling due to the geometrical asymmetry of the quantum dot.

cond-mat.mes-hall↗

arXiv2009

Controlling the polarization eigenstate of a quantum dot exciton with light

We demonstrate optical control of the polarization eigenstates of a neutral quantum dot exciton without any external fields. By varying the excitation power of a circularly polarized laser in micro-photoluminescence experiments on individual InGaAs quantum dots we control the magnitude and direction of an effective internal magnetic field created via optical pumping of nuclear spins. The adjustable nuclear magnetic field allows us to tune the linear and circular polarization degree of the neutral exciton emission. The quantum dot can thus act as a tunable light polarization converter.

physics.optics↗

arXiv2008

Optically monitored nuclear spin dynamics in individual GaAs quantum dots grown by droplet epitaxy

We report optical orientation experiments in individual, strain free GaAs quantum dots in AlGaAs grown by droplet epitaxy. Circularly polarized optical excitation yields strong circular polarization of the resulting photoluminescence at 4K. Optical injection of spin polarized electrons into a dot gives rise to dynamical nuclear polarization that considerably changes the exciton Zeeman splitting (Overhauser shift). We show that the created nuclear polarization is bistable and present a direct measurement of the build-up time of the nuclear polarization in a single GaAs dot in the order of one second.

physics.optics↗

arXiv2007

Exciton Spin Dynamics in Semiconductor Quantum Wells

In this paper we will review Exciton Spin Dynamics in Semiconductor Quantum Wells. The spin properties of excitons in nanostructures are determined by their fine structure. We will mainly focus in this review on GaAs and InGaAs quantum wells which are model systems.

cond-mat.other↗

arXiv2005

Dynamic nuclear polarization of a single charge-tunable InAs/GaAs quantum dot

We report on the dynamic nuclear polarization of a single charge-tunable self-assembled InAs/GaAs quantum dot in a longitudinal magnetic field of $\sim$0.2T. The hyperfine interaction between the optically oriented electron and nuclei spins leads to the polarization of the quantum dot nuclei measured by the Overhauser-shift of the singly-charged excitons ($X^{+}$ and $X^{-}$). When going from $X^{+}$ to $X^{-}$, we observe a reversal of this shift which reflects the average electron spin optically written down in the quantum dot either in the $X^{+}$ state or in the final state of $X^{-}$ recombination. We discuss a theoretical model which indicates an efficient depolarization mechanism for the nuclei limiting their polarization to ~10%.

cond-mat.other↗