No Arabic abstract
The coupled spin and valley degrees of freedom in transition metal dichalcogenides (TMDs) are considered a promising platform for information processing. Here, we use a TMD heterostructure ${text{MoS}_{2}-text{MoSe}_{2}}$ to study optical pumping of spin/valley polarized carriers across the interface and to elucidate the mechanisms governing their subsequent relaxation. By applying time-resolved Kerr and reflectivity spectroscopies, we find that the photoexcited carriers conserve their spin for both tunneling directions across the interface. Following this, we measure dramatically different spin/valley depolarization rates for electrons and holes, $sim 30,{text{ns}}^{-1}$ and $< 1,{text{ns}}^{-1}$, respectively and show that this difference relates to the disparity in the spin-orbit splitting in conduction and valence bands of TMDs. Our work provides insights into the spin/valley dynamics of free carriers unaffected by complex excitonic processes and establishes TMD heterostructures as generators of spin currents in spin/valleytronic devices.
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.
Non-equilibrium dynamics of strongly correlated systems constitutes a fascinating problem of condensed matter physics with many open questions. Here we investigate the relaxation dynamics of Landau-quantized electron system into spin-valley polarized ground state in a gate-tunable MoSe$_2$ monolayer subjected to a strong magnetic field. The system is driven out of equilibrium with optically injected excitons that depolarize the electron spins and the subsequent electron spin-valley relaxation is probed in time-resolved experiments. We demonstrate that the relaxation rate at millikelvin temperatures sensitively depends on the Landau level filling factor: it becomes faster whenever the electrons form an integer quantum Hall liquid and slows down appreciably at non-integer fillings. Our findings evidence that valley relaxation dynamics may be used as a tool to investigate the interplay between the effects of disorder and strong interactions in the electronic ground state.
Magneto transmission spectroscopy was employed to study the valley Zeeman effect in large-area monolayer MoS$_{2}$ and MoSe$_{2}$. The extracted values of the valley g-factors for both A- and B-exciton were found be similar with $g_v simeq -4.5$. The samples are expected to be strained due to the CVD growth on sapphire at high temperature ($700^circ$C). However, the estimated strain, which is maximum at low temperature, is only $simeq 0.2%$. Theoretical considerations suggest that the strain is too small to significantly influence the electronic properties. This is confirmed by the measured value of valley g-factor, and the measured temperature dependence of the band gap, which are almost identical for CVD and mechanically exfoliated MoS$_2$.
The valley dependent optical selection rules in recently discovered monolayer group-VI transition metal dichalcogenides (TMDs) make possible optical control of valley polarization, a crucial step towards valleytronic applications. However, in presence of Landaul level(LL) quantization such selection rules are taken over by selection rules between the LLs, which are not necessarily valley contrasting. Using MoS$_{2}$ as an example we show that the spatial inversion-symmetry breaking results in unusual valley dependent inter-LL selection rules, which directly locks polarization to valley. We find a systematic valley splitting for all Landau levels (LLs) in the quantum Hall regime, whose magnitude is linearly proportional to the magnetic field and in comparable with the LL spacing. Consequently, unique plateau structures are found in the optical Hall conductivity, which can be measured by the magneto-optical Faraday rotations.
Atomically thin semiconductors have dimensions that are commensurate with critical feature sizes of future optoelectronic devices defined using electron/ion beam lithography. Robustness of their emergent optical and valleytronic properties is essential for typical exposure doses used during fabrication. Here, we explore how focused helium ion bombardment affects the intrinsic vibrational, luminescence and valleytronic properties of atomically thin MoS$_{2}$. By probing the disorder dependent vibrational response we deduce the interdefect distance by applying a phonon confinement model. We show that the increasing interdefect distance correlates with disorder-related luminescence arising 180 meV below the neutral exciton emission. We perform ab-initio density functional theory of a variety of defect related morphologies, which yield first indications on the origin of the observed additional luminescence. Remarkably, no significant reduction of free exciton valley polarization is observed until the interdefect distance approaches a few nanometers, namely the size of the free exciton Bohr radius. Our findings pave the way for direct writing of sub-10 nm nanoscale valleytronic devices and circuits using focused helium ions.