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Register a new userAnomalous valley polarization in monolayer MoSe2
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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.
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Single layers of transition metal dichalcogenides (TMDs) are direct gap semiconductors with nondegenerate valley indices. An intriguing possibility for these materials is the use of their valley index as an alternate state variable. Several limitations to such a utility include strong, phonon-enabled intervalley scattering, as well as multiparticle interactions leading to multiple emission channels. We prepare single-layer WS$_{2}$ such that the photoluminescence is from either the neutral or charged exciton (trion). After excitation with circularly polarized light, the neutral exciton emission has zero polarization, however, the trion emission has a large polarization (28%) at room temperature. The trion emission also has a unique, non-monotonic temperature dependence that we show is a consequence of the multiparticle nature of the trion. This temperature dependence enables us to determine that coulomb assisted intervalley scattering, electron-hole radiative recombination, and a 3-particle Auger process are the dominant mechanisms at work in this system. Because this dependence involves trion systems, one can use gate voltages to modulate the polarization (or intensity) emitted from TMD structures.
In monolayer semiconductor transition metal dichalcogenides, the exciton-phonon interaction is expected to strongly affect the photocarrier dynamics. Here, we report on an unusual oscillatory enhancement of the neutral exciton photoluminescence with the excitation laser frequency in monolayer MoSe2. The frequency of oscillation matches that of the M-point longitudinal acoustic phonon, LA(M). Oscillatory behavior is also observed in the steady-state emission linewidth and in timeresolved photoluminescence excitation data, which reveals variation with excitation energy in the exciton lifetime. These results clearly expose the key role played by phonons in the exciton formation and relaxation dynamics of two-dimensional van der Waals semiconductors.
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.
Valleytronics is rapidly emerging as an exciting area of basic and applied research. In two dimensional systems, valley polarisation can dramatically modify physical properties through electron-electron interactions as demonstrated by such phenomena as the fractional quantum Hall effect and the metal-insulator transition. Here, we address the electrons spin alignment in a magnetic field in silicon-on-insulator quantum wells under valley polarisation. In stark contrast to expectations from a non-interacting model, we show experimentally that less magnetic field can be required to fully spin polarise a valley-polarised system than a valley-degenerate one. Furthermore, we show that these observations are quantitatively described by parameter free ab initio quantum Monte Carlo simulations. We interpret the results as a manifestation of the greater stability of the spin and valley degenerate system against ferromagnetic instability and Wigner crystalisation which in turn suggests the existence of a new strongly correlated electron liquid at low electron densities.
Valleytronics targets the exploitation of the additional degrees of freedom in materials where the energy of the carriers may assume several equal minimum values (valleys) at non-equivalent points of the reciprocal space. In single layers of transition metal dichalcogenides (TMDs) the lack of inversion symmetry, combined with a large spin-orbit interaction, leads to a conduction (valence) band with different spin-polarized minima (maxima) having equal energies. This offers the opportunity to manipulate information at the level of the charge (electrons or holes), spin (up or down) and crystal momentum (valley). Any implementation of these concepts, however, needs to consider the robustness of such degrees of freedom, which are deeply intertwined. Here we address the spin and valley relaxation dynamics of both electrons and holes with a combination of ultrafast optical spectroscopy techniques, and determine the individual characteristic relaxation times of charge, spin and valley in a MoS$_{2}$ monolayer. These results lay the foundations for understanding the mechanisms of spin and valley polarization loss in two-dimensional TMDs: spin/valley polarizations survive almost two-orders of magnitude longer for holes, where spin and valley dynamics are interlocked, than for electrons, where these degrees of freedom are decoupled. This may lead to novel approaches for the integration of materials with large spin-orbit in robust spintronic/valleytronic platforms.
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