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Register a new userTrion Species-Resolved Quantum Beats in MoSe2
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Monolayer photonic materials offer a tremendous potential for on-chip optoelectronic devices. Their realization requires knowledge of optical coherence properties of excitons and trions that have so far been limited to nonlinear optical experiments carried out with strongly inhomogenously broadened material. Here we employ h-BN encapsulated and electrically gated MoSe2 to reveal coherence properties of trion-species directly in the linear optical response. Autocorrelation measurements reveal long dephasing times up to T2=1.16+-0.05 ps for positively charged excitons. Gate dependent measurements provide evidence that the positively-charged trion forms via spatially localized hole states making this trion less prone to dephasing in the presence of elevated hole carrier concentrations. Quantum beat signatures demonstrate coherent coupling between excitons and trions that have a dephasing time up to 0.6 ps, a two-fold increase over those in previous reports. A key merit of the prolonged exciton/trion coherences is that they were achieved in a linear optical experiment, and thus are directly relevant to applications in nanolasers, coherent control, and on-chip quantum information processing requiring long photon coherence.
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We present a detailed investigation of the exciton and trion dynamics in naturally doped MoSe2 and WSe2 single atomic layers as a function of temperature in the range 10-300K under above band-gap laser excitation. By combining time-integrated and time-resolved photoluminescence (PL) spectroscopy we show the importance of exciton and trion localization in both materials at low temperatures. We also reveal the transition to delocalized exciton complexes at higher temperatures where the exciton and trion thermal energy exceeds the typical localization energy. This is accompanied with strong changes in PL including suppression of the trion PL and decrease of the trion PL life-time, as well as significant changes for neutral excitons in the temperature dependence of the PL intensity and appearance of a pronounced slow PL decay component. In MoSe2 and WSe2 studied here, the temperatures where such strong changes occur are observed at around 100 and 200 K, respectively, in agreement with their inhomogeneous PL linewidth of 8 and 20 meV at T~10K. The observed behavior is a result of a complex interplay between influences of the specific energy ordering of bright and dark excitons in MoSe2 and WSe2, sample doping, trion and exciton localization and various temperature-dependent non-radiative processes.
Transition metal dichalcogenides represent an ideal testbed to study excitonic effects, spin-related phenomena and fundamental light-matter coupling in nanoscopic condensed matter systems. In particular, the valley degree of freedom, which is unique to such direct band gap monolayers with broken inversion symmetry, adds fundamental interest in these materials. Here, we implement a Tamm-plasmon structure with an embedded MoSe2 monolayer and study the formation of polaritonic quasi-particles. Strong coupling conditions between the Tamm-mode and the trion resonance of MoSe2 are established, yielding bright luminescence from the polaritonic ground state under non-resonant optical excitation. We demonstrate, that tailoring the electrodynamic environment of the monolayer results in a significantly increased valley polarization. This enhancement can be related to change in recombination dynamics shown in time-resolved photoluminescence measurements. We furthermore observe strong upconversion luminescence from resonantly excited polariton states in the lower polariton branch. This upconverted polariton luminescence is shown to preserve the valley polarization of the trion-polariton, which paves the way towards combining spin-valley physics and exciton scattering experiments.
In this paper, we experimentally demonstrate an oscillating energy shift of quantum-confined exciton levels in a semiconductor quantum well after excitation into a superposition of two quantum confined exciton states of different parity. Oscillations are observed at frequencies corresponding to the quantum beats between these states. We show that the observed effect is a manifestation of the exciton density oscillations in the real space similar to the dynamics of a Hertzian dipole. The effect is caused by the exciton-exciton exchange interaction and appears only if the excitons are in a superposition quantum state. Thus, we have found clear evidence for the incoherent exchange interaction in the coherent process of quantum beats. This effect may be harnessed for quantum technologies requiring the quantum coherence of states.
Multiple quantum beats of a system of the coherently excited quantum confined exciton states in a high-quality heterostructure with a wide InGaAs/GaAs quantum well are experimentally detected by the spectrally resolved pump-probe method for the first time. The beat signal is observed as at positive as at negative delays between the pump and probe pulses. A theoretical model is developed, which allows one to attribute the QBs at negative delay to the four-wave mixing (FWM) signal detected at the non-standard direction. The beat signal is strongly enhanced by the interference of the FWM wave with the polarization created by the probe pulse. At positive delay, the QBs are due to the mutual interference of the quantum confined exciton states. Several QB frequencies are observed in the experiments, which coincide with the interlevel spacings in the exciton system. The decay time for QBs is of order of several picoseconds at both the positive and negative delays. They are close to the relaxation time of exciton population that allows one to consider the exciton depopulation as the main mechanism of the coherence relaxation in the system under study.
In this work, we show how domain engineered lithium niobate can be used to selectively dope monolayer MoSe2 and WSe2 and demonstrate that these ferroelectric domains can significantly enhance or inhibit photoluminescence (PL) with the most dramatic modulation occurring at the heterojunction interface between two domains. A micro-PL and Raman system is used to obtain spatially resolved images of the differently doped transition metal dichalcogenides (TMDs). The domain inverted lithium niobate causes changes in the TMDs due to electrostatic doping as a result of the remnant polarization from the substrate. Moreover, the differently doped TMDs (n-type MoSe2 and p-type WSe2) exhibit opposite PL modulation. Distinct oppositely charged domains were obtained with a 9-fold PL enhancement for the same single MoSe2 sheet when adhered to the positive (P+) and negative (P-) domains. This sharp PL modulation on the ferroelectric domain results from different free electron or hole concentrations in the materials conduction band or valence band. Moreover, excitons dissociate rapidly at the interface between the P+ and P- domains due to the built-in electric field. We are able to adjust the charge on the P+ and P- domains using temperature via the pyroelectric effect and observe rapid PL quenching over a narrow temperature range illustrating the observed PL modulation is electronic in nature. This observation creates an opportunity to harness the direct bandgap TMD 2D materials as an active optical component for the lithium niobate platform using domain engineering of the lithium niobate substrate to create optically active heterostructures that could be used for photodetectors or even electrically driven optical sources on-chip.
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