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Register a new userExciton Radiative Lifetime in Transition Metal Dichalcogenide Monolayers
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We have investigated the exciton dynamics in transition metal dichalcogenide mono-layers using time-resolved photoluminescence experiments performed with optimized time-resolution. For MoSe2 monolayers, we measure $tau_{rad}=1.8pm0.2$ ps that we interpret as the intrinsic radiative recombination time. Similar values are found for WSe2 mono-layers. Our detailed analysis suggests the following scenario: at low temperature (T $leq$ 50 K), the exciton oscillator strength is so large that the entire light can be emitted before the time required for the establishment of a thermalized exciton distribution. For higher lattice temperatures, the photoluminescence dynamics is characterized by two regimes with very different characteristic times. First the PL intensity drops drastically with a decay time in the range of the picosecond driven by the escape of excitons from the radiative window due to exciton- phonon interactions. Following this first non-thermal regime, a thermalized exciton population is established gradually yielding longer photoluminescence decay times in the nanosecond range. Both the exciton effective radiative recombination and non-radiative recombination channels including exciton-exciton annihilation control the latter. Finally the temperature dependence of the measured exciton and trion dynamics indicates that the two populations are not in thermodynamical equilibrium.
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We study theoretically the Coulomb interaction between excitons in transition metal dichalcogenide (TMD) monolayers. We calculate direct and exchange interaction for both ground and excited states of excitons. The screening of the Coulomb interaction, specific to monolayer structures, leads to the unique behavior of the exciton-exciton scattering for excited states, characterized by the non-monotonic dependence of the interaction as function of the transferred momentum. We find that the nontrivial screening enables the description of TMD exciton interaction strength by approximate formula which includes exciton binding parameters. The influence of screening and dielectric environment on the exciton-exciton interaction was studied, showing qualitatively different behavior for ground state and excited states of excitons. Furthermore, we consider exciton-electron interaction, which for the excited states is governed by the dominant attractive contribution of the exchange component, which increases with the excitation number. The results provide a quantitative description of the exciton-exciton and exciton-electron scattering in transition metal dichalcogenides, and are of interest for the design of perspective nonlinear optical devices based on TMD monolayers.
Due to a strong Coulomb interaction, excitons dominate the excitation kinetics in 2D materials. While Coulomb-scattering between electrons has been well studied, the interaction of excitons is more challenging and remains to be explored. As neutral composite bosons consisting of electrons and holes, excitons show a non-trivial scattering dynamics. Here, we study on microscopic footing exciton-exciton interaction in transition-metal dichalcogenides and related van der Waals heterostructures. We demonstrate that the crucial criterion for efficient scattering is a large electron/hole mass asymmetry giving rise to internal charge inhomogeneities of excitons and emphasizing their cobosonic substructure. Furthermore, both exchange and direct exciton-exciton interactions are boosted by enhanced exciton Bohr radii. We also predict an unexpected temperature dependence that is usually associated to phonon-driven scattering and we reveal an orders of magnitude stronger interaction of interlayer excitons due to their permanent dipole moment. The developed approach can be generalized to arbitrary material systems and will help to study strongly correlated exciton systems, such as moire super lattices.
The intricate interplay between optically dark and bright excitons governs the light-matter interaction in transition metal dichalcogenide monolayers. We have performed a detailed investigation of the spin-forbidden dark excitons in WSe2 monolayers by optical spectroscopy in an out-of-plane magnetic field Bz. In agreement with the theoretical predictions deduced from group theory analysis, magneto-photoluminescence experiments reveal a zero field splitting $delta=0.6 pm 0.1$ meV between two dark exciton states. The low energy state being strictly dipole forbidden (perfectly dark) at Bz=0 while the upper state is partially coupled to light with z polarization (grey exciton). The first determination of the dark neutral exciton lifetime $tau_D$ in a transition metal dichalcogenide monolayer is obtained by time-resolved photoluminescence. We measure $tau_D sim 110 pm 10$ ps for the grey exciton state, i.e. two orders of magnitude longer than the radiative lifetime of the bright neutral exciton at T=12 K.
The direct gap interband transitions in transition metal dichalcogenides monolayers are governed by chiral optical selection rules. Determined by laser helicity, optical transitions in either the $K^+$ or $K^-$ valley in momentum space are induced. Linearly polarized laser excitation prepares a coherent superposition of valley states. Here we demonstrate the control of the exciton valley coherence in monolayer WSe2 by tuning the applied magnetic field perpendicular to the monolayer plane. We show rotation of this coherent superposition of valley states by angles as large as 30 degrees in applied fields up to 9 T. This exciton valley coherence control on ps time scale could be an important step towards complete control of qubits based on the valley degree of freedom.
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.
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