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Van der Waals (Vdw) heterostructures constructed from TMDCs provide an ideal platform for exploring various quasiparticle behaviors, with trion-composed of neutral exciton and charged carrier-being a notable example. There are typically three methods to generate trion: electrical doping, chemical doping, and direct optical doping. The first two methods generate static trion, while the last gives rise to transient trion. Here, we present an indirect optical doping approach to generate transient trion via ultrafast charge transfer (CT) and achieve control over the trion-to-exciton ratio by adjusting CT in Gr/MoS2 heterostructure. Furthermore, we demonstrated that dynamics of the transient trion generated with this method, which shows slightly longer lifetime than that of exciton accounted for the Coulomb interactions between trion and charged defect. This study provides fresh perspectives on the construction of new quasiparticles, dynamical characterization and the control of the many-body interaction in two-dimensional structure., Comment: 16 pages, 4 figures

Mixing the fundamental ($\omega$) and the second harmonic (2$\omega$) waves in gas phase is a widely employed technique for emitting terahertz (THz) pulses. The THz generation driven by bi-chromatic fields can be described by the photocurrent model, where the THz generation is attributed to free electrons ionized by the $\omega$ field, and the 2$\omega$ field provides a perturbation to break the symmetry of the asymptotic momentum of free electrons. However, we find that the THz radiation is amplified by one order of magnitude when driven by bi-focal bi-chromatic fields, contradicting the common understanding of the photocurrent model. Meanwhile, present measurements demonstrate that the THz radiation mainly originates from the plasma created by the 2$\omega$ pulses instead of the $\omega$ pulses. Energy transfer from the 2$\omega$ beam to the THz beam during the THz generation has been observed, validating the major contribution of the 2$\omega$ beam. Furthermore, the THz bandwidth has been observed to extensively exceed the bandwidth of the pump pulse, not be explained by the photocurrent model as well. These counterintuitive results indicate that undiscovered physical mechanisms are involved in bi-chromatic THz generation in plasma, presenting a significant challenge for understanding strong-field nonlinear optics and simultaneously expanding various applications.

Vertical van der Waals (vdW) heterostructures consisting of graphene (Gr) and transition metal dichalcogenides (TMDs) have created a fascinating platform for exploring optical and electronic properties in the two-dimensional limit. Previous study has revealed the ultrafast formation of interfacial excitons and the exciton dynamics in the Gr/MoS2 heterostructure. However, a fully understanding of interfacial charge separation and the subsequent dynamics in graphene-based heterostructures remains elusive. Here, we investigate the carrier dynamics of Gr-MoS2 (including Gr/MoS2 and MoS2/Gr stacking sequences) heterostructures under different photoexcitation energies and stacking sequences by comprehensive ultrafast means, including time-resolved terahertz spectroscopy (TRTS), terahertz emission spectroscopy (TES) and transient absorption spectroscopy (TAS). We demonstrate that the Gr/MoS2 heterostructure generates hot electron injection from graphene into the MoS2 layer with photoexcitation of sub-A-exciton of MoS2, while the interfacial charge separation in the MoS2/Gr could be partially blocked by the electric field of substrate. Charge transfer (CT) occurs in same directions for the Gr-MoS2 heterostructures with opposite stacking order, resulting in the opposite orientations of the interfacial photocurrent, as directly demonstrated by the terahertz (THz) emission. Moreover, we demonstrate that the recombination time of interfacial charges after CT is on a timescale of 18 ps to 1 ns, depending on the density of defect states in MoS2 layer. This work provides a comprehensive and unambiguous picture of the interfacial charge dynamics of graphene-based heterostructures, which is essential for developing Gr/TMDs based optoelectronic devices., Comment: 23 pages, 5 Figures

In this study,we combined time-resolved terahertz spectroscopy along with transient absorption spectroscopy to revisit the interlayer non-equilibrium carrier dynamics in largely lateral size Gr/MoS2 heterostructure fabricated with chemical vapor deposition method. Our experimental results reveal that, with photon-energy below the A-exciton of MoS2 monolayer, hot electrons transfer from graphene to MoS2 takes place in time scale of less than 0.5 ps, resulting in ultrafast formation of interfacial exciton in the heterostructure, subsequently, recombination relaxation of the interfacial exciton occurs in time scale of ~18 ps. A new model considering carrier heating and photogating effect in graphene is proposed to estimate the amount of carrier transfer in the heterostructure, which shows a good agreement with experimental result. Moreover, when the photon-energy is on-resonance with the A-exciton of MoS2, photogenerated holes in MoS2 are transferred to graphene layer within 0.5 ps, leading to the formation of interfacial exciton, the subsequent photoconductivity (PC) relaxation of graphene and bleaching recovery of A-exciton in MoS2 take place around ~10 ps time scale, ascribing to the interfacial exciton recombination. The faster recombination time of interfacial exciton with on-resonance excitation could come from the reduced interface barrier caused by bandgap renormalization effect. Our study provides deep insight into the understanding of interfacial charge transfer as well as the relaxation dynamics in graphene-based heterostructures, which are promising for the applications of graphene-based optoelectronic devices., Comment: 24 pages, 4 figures