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Ye, Ziliang

Publications and source records attributed to Ye, Ziliang.

Efficient generation of neutral and charged biexcitons in encapsulated WSe2 monolayers

Abstract Higher-order correlated excitonic states arise from the mutual interactions of excitons, which generally requires a significant exciton density and therefore high excitation levels. Here, we report the emergence of two biexcitons species, one neutral and one charged, in monolayer tungsten diselenide under moderate continuous-wave excitation. The efficient formation of biexcitons is facilitated by the long lifetime of the dark exciton state associated with a spin-forbidden transition, as well as improved sample quality from encapsulation between hexagonal boron nitride layers. From studies of the polarization and magnetic field dependence of the neutral biexciton, we conclude that this species is composed of a bright and a dark excitons residing in opposite valleys in momentum space. Our observations demonstrate that the distinctive features associated with biexciton states can be accessed at low light intensities and excitation densities.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Optical manipulation of valley pseudospin

The coherent manipulation of spin and pseudospin underlies existing and emerging quantum technologies, including quantum communication and quantum computation. Valley polarization, associated with the occupancy of degenerate, but quantum mechanically distinct valleys in momentum space, closely resembles spin polarization and has been proposed as a pseudospin carrier for the future quantum electronics. Valley exciton polarization has been created in the transition metal dichalcogenide monolayers using excitation by circularly polarized light and has been detected both optically and electrically. In addition, the existence of coherence in the valley pseudospin has been identified experimentally. The manipulation of such valley coherence has, however, remained out of reach. In this paper, we demonstrate all-optical control of the valley coherence by means of the pseudomagnetic field associated with the optical Stark effect. Using below-bandgap circularly polarized light, we rotate the valley exciton pseudospin in monolayer WSe 2 on the femtosecond timescale. Both the direction and speed of the rotation can be manipulated optically by tuning the dynamic phase of excitons in opposite valleys. Finally, this study unveils the possibility of generation, manipulation, and detection of the valley pseudospin by coupling to photons.

36 MATERIALS SCIENCE↗

Atomically phase-matched second-harmonic generation in a 2D crystal

Second-harmonic generation (SHG) has found extensive applications from hand-held laser pointers to spectroscopic and microscopic techniques. Recently, some cleavable van der Waals (vdW) crystals have shown SHG arising from a single atomic layer, where the SH light elucidated important information such as the grain boundaries and electronic structure in these ultra-thin materials. However, despite the inversion asymmetry of the single layer, the typical crystal stacking restores inversion symmetry for even numbers of layers leading to an oscillatory SH response, drastically reducing the applicability of vdW crystals such as molybdenum disulfide (MoS 2 ). Here, we probe the SHG generated from the noncentrosymmetric 3R crystal phase of MoS 2 . We experimentally observed quadratic dependence of second-harmonic intensity on layer number as a result of atomically phase-matched nonlinear dipoles in layers of the 3R crystal that constructively interfere. By studying the layer evolution of the A and B excitonic transitions in 3R-MoS 2 using SHG spectroscopy, we also found distinct electronic structure differences arising from the crystal structure and the dramatic effect of symmetry and layer stacking on the nonlinear properties of these atomic crystals. The constructive nature of the SHG in this 2D crystal provides a platform to reliably develop atomically flat and controllably thin nonlinear media.

3R-MoS2↗

Nonlinear optical selection rule based on valley-exciton locking in monolayer ws 2

Optical selection rules fundamentally determine the optical transitions between energy states in a variety of physical systems, from hydrogen atoms to bulk crystals such as gallium arsenide. These rules are important for optoelectronic applications such as lasers, energy-dispersive X-ray spectroscopy, and quantum computation. Recently, single-layer transition metal dichalcogenides have been found to exhibit valleys in momentum space with nontrivial Berry curvature and excitons with large binding energy. However, there has been little study of how the unique valley degree of freedom combined with the strong excitonic effect influences the nonlinear optical excitation. Here in this paper, we report the discovery of nonlinear optical selection rules in monolayer WS 2 , an important candidate for visible 2D optoelectronics because of its high quantum yield and large direct bandgap. We experimentally demonstrated this principle for second-harmonic generation and two-photon luminescence (TPL). Moreover, the circularly polarized TPL and the study of its dynamics evince a sub-ps interexciton relaxation (2p → 1s). The discovery of this new optical selection rule in a valleytronic 2D system not only considerably enhances knowledge in this area but also establishes a foundation for the control of optical transitions that will be crucial for valley optoelectronic device applications such as 2D valley-polarized THz sources with 2p-1s transitions, optical switches, and coherent control for quantum computing.

2D materials↗