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Giant paramagnetism induced valley polarization of electrons in charge-tunable monolayer MoSe2

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 Added by Atac Imamoglu
 Publication date 2017
  fields Physics
and research's language is English




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For applications exploiting the valley pseudospin degree of freedom in transition metal dichalcogenide monolayers, efficient preparation of electrons or holes in a single valley is essential. Here, we show that a magnetic field of 7 Tesla leads to a near-complete valley polarization of electrons in MoSe2 monolayer with a density 1.6x10^{12} cm^{-2}; in the absence of exchange interactions favoring single-valley occupancy, a similar degree of valley polarization would have required a pseudospin g-factor exceeding 40. To investigate the magnetic response, we use polarization resolved photoluminescence as well as resonant reflection measurements. In the latter, we observe gate voltage dependent transfer of oscillator strength from the exciton to the attractive-Fermi-polaron: stark differences in the spectrum of the two light helicities provide a confirmation of valley polarization. Our findings suggest an interaction induced giant paramagnetic response of MoSe2, which paves the way for valleytronics applications.

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Modern electronic devices heavily rely on the accurate control of charge and spin of electrons. The emergence of controllable valley degree of freedom brings new possibilities and presents a promising prospect towards valleytronics. Recently, valley excitation selected by chiral optical pumping has been observed in monolayer MoS2. In this work, we report polarized photoluminescence (PL) measurements for monolayer MoSe2, another member of the family of transition-metal-dichalcogenides (MX2), and observe drastic difference from the outcomes of MoS2. In particular, we identify a valley polarization (VP) up to 70% for B exciton, while that for A exciton is less than 3%. Besides, we also find a small but finite negative VP for A- trion. These results reveal several new intra- and inter-valley scattering processes which significantly affect valley polarization, hence provide new insights into exciton physics in monolayer MX2 and possible valleytronic applications.
We have measured circularly polarized photoluminescence in monolayer MoSe2 under perpendicular magnetic fields up to 10 T. At low doping densities, the neutral and charged excitons shift linearly with field strength at a rate of $mp$ 0.12 meV/T for emission arising, respectively, from the K and K valleys. The opposite sign for emission from different valleys demonstrates lifting of the valley degeneracy. The magnitude of the Zeeman shift agrees with predicted magnetic moments for carriers in the conduction and valence bands. The relative intensity of neutral and charged exciton emission is modified by the magnetic field, reflecting the creation of field-induced valley polarization. At high doping levels, the Zeeman shift of the charged exciton increases to $mp$ 0.18 meV/T. This enhancement is attributed to many-body effects on the binding energy of the charged excitons.
69 - M. Krol , K. Lekenta , R. Mirek 2018
Monolayer transition metal dichalcogenides, known for exhibiting strong excitonic resonances, constitute a very interesting and versatile platform for investigation of light-matter interactions. In this work we report on a strong coupling regime between excitons in monolayer WSe2 and photons confined in an open, voltage-tunable dielectric microcavity. The tunability of our system allows us to extend the exciton-polariton state over a wide energy range and, in particular, to bring the excitonic component of the lower polariton mode into resonance with other excitonic transitions in monolayer WSe2. With selective excitation of spin-polarized exciton-polaritons we demonstrate the valley polarization when the polaritons from the lower branch come into resonance with a bright trion state in monolayer WSe2 and valley depolarization when they are in resonance with a dark trion state.
The strong excitonic effect in monolayer transition metal dichalcogenide (TMD) semiconductors has enabled many fascinating light-matter interaction phenomena. Examples include strongly coupled exciton-polaritons and nearly perfect atomic monolayer mirrors. The strong light-matter interaction also opens the door for dynamical control of mechanical motion through the exciton resonance of monolayer TMDs. Here we report the observation of exciton-optomechanical coupling in a suspended monolayer MoSe2 mechanical resonator. By moderate optical pumping near the MoSe2 exciton resonance, we have observed optical damping and anti-damping of mechanical vibrations as well as the optical spring effect. The exciton-optomechanical coupling strength is also gate-tunable. Our observations can be understood in a model based on photothermal backaction and gate-induced mirror symmetry breaking in the device structure. The observation of gate-tunable exciton-optomechanical coupling in a monolayer semiconductor may find applications in nanoelectromechanical systems (NEMS) and in exciton-optomechanics.
Atomically thin crystals of transition metal dichalcogenides are ideally suited to study the interplay of light-matter coupling, polarization and magnetic field effects. In this work, we investiagte the formation of exciton-polaritons in a MoSe2 monolayer, which is integrated in a fully-grown, monolithic microcavity. Due to the narrow linewidth of the polaritonic resonances, we are able to directly investigate the emerging valley Zeeman splitting of the hybrid light-matter resonances in the presence of a magnetic field. At a detuning of -54.5 meV (13.5 % matter constituent of the lower polariton branch), we find a Zeeman splitting of the lower polariton branch of 0.36 meV, which can be directly associated with an excitonic g factor of 3.94pm0.13. Remarkably, we find that a magnetic field of 6T is sufficient to induce a notable valley polarization of 15 % in our polariton system, which approaches 30% at 9T. Strikingly, this circular polarization degree of the polariton (ground) state exceeds the polarization of the exciton reservoir for equal magnetic field magnitudes by approximately 50%, as a consequence of enhanced relaxation of bosons in our monolayer-based system.
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