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Register a new userBrightening of dark excitons in monolayers of semiconducting transition metal dichalcogenides
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We present low temperature magneto-photoluminescence experiments which demonstrate the brightening of dark excitons by an in-plane magnetic field $B$ applied to monolayers of different semiconducting transition metal dichalcogenides. For both WSe$_2$ and WS$_2$ monolayers, the dark exciton emission is observed at $sim$50 meV below the bright exciton peak and displays a characteristic doublet structure which intensity is growing with $B^2$, while no magnetic field induced emission peaks appear for MoSe$_2$ monolayer. Our experiments also show that the MoS$_2$ monolayer has a dark exciton ground state with a dark-bright exciton splitting energy of $sim$100 meV.
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The photoluminescence (PL) spectrum of transition metal dichalcogenides (TMDs) shows a multitude of emission peaks below the bright exciton line and not all of them have been explained yet. Here, we study the emission traces of phonon-assisted recombinations of momentum-dark excitons. To this end, we develop a microscopic theory describing simultaneous exciton, phonon and photon interaction and including consistent many-particle dephasing. We explain the drastically different PL below the bright exciton in tungsten- and molybdenum-based materials as result of different configurations of bright and dark states. In good agreement with experiments, we show that WSe$_2$ exhibits clearly visible low-temperature PL signals stemming from the phonon-assisted recombination of momentum-dark excitons.
We theoretically study the interaction of an ultrafast intense linearly polarized optical pulse with monolayers of transition metal dichalcogenides (TMDCs). Such a strong pulse redistributes electrons between the bands and generates femtosecond currents during the pulse. Due to the large bandwidth of the incident pulse, this process is completely off-resonant. While in TMDCs the time-reversal symmetry is conserved, the inversion symmetry is broken and these monolayers have the axial symmetry along armchair direction but not along the zigzag one. Therefore, the pulse polarized along the asymmetric direction of TMDC monolayer generates both longitudinal, i.e., along the direction of polarization, and transverse, i.e., in the perpendicular direction, currents. Such currents result in charge transfer through the system. We study different TMDC materials and show how the femtosecond transport in TMDC monolayers depend on their parameters, such as lattice constant and bandgap.
A rate equation model for the dark and bright excitons kinetics is proposed which explains the wide variation in the observed degree of circular polarization of the PL emission in different TMDs monolayers. Our work suggests that the dark exciton states play an important, and previously unsuspected role in determining the degree of polarization of the PL emission. A dark exciton ground state provides a robust reservoir for valley polarization, which tries to maintain a Boltzmann distribution of the bright exciton states in the same valley via the intra valley bright dark exciton scattering mechanism. The dependence of the degree of circular polarization on the detuning energy of the excitation in MoSe$_2$ suggests that the electron-hole exchange interaction dominates over two LA phonon emission mechanism for inter valley scattering in TMDs.
The linear absorption spectra in monolayers of transition metal dichalcogenides show pronounced signatures of the exceptionally strong exciton-phonon interaction in these materials. To account for both exciton and phonon physics in such optical signals, we compare different theoretical methods to calculate the absorption spectra using the example of $mathrm{MoSe_2}$. In this paper, we derive the equations of motion for the polarization either using a correlation expansion up to 4th Born approximation or a time convolutionless master equation. We show that the Born approximation might become problematic when not treated in high enough order, especially at high temperatures. In contrast, the time convolutionless formulation gives surprisingly good results despite its simplicity when compared to higher-order corrrelation expansion and therefore provides a powerful tool to calculate the lineshape of linear absorption spectra in the very popular monolayer materials.
Current-controlled (also known as S-type) negative differential resistance (NDR) is of crucial importance to many emerging applications including neuromorphic computing and high-density memristors integration. However, the experimental realization of S-type NDR based on conventional mechanisms poses demanding requirements on materials, which greatly limits their potential applications. Here, we experimentally identify that semiconducting transition metal dichalcogenides (TMDs) can host a bipolar S-type NDR devices. Theoretical simulations indicate that the origin of the NDR in these devices arises from a thermal feedback mechanism. Furthermore, we demonstrate the potential applications of TMDs based S-type NDR device in signal processing and neuromorphic electronics.
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