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Tailoring MoS2 Valley-Polarized Photoluminescence with Super Chiral Near-Field

Ziwei Li, Changxu Liu, Xin Rong, Yang Luo, Haotian Cheng, Liheng Zheng, Feng Lin, Bo Shen, Yongji Gong, Shuang Zhang,* and Zheyu Fang*


Abstract:Transition metal dichalcogenides with intrinsic spin–valley degrees of freedom hold great potentials for applications in spintronic and val-leytronic devices. MoS2 monolayer possesses two inequivalent valleys in the Brillouin zone, with each valley coupling selectively with circularly polarized photons. The degree of valley polarization (DVP) is a parameter to characterize the purity of valley-polarized photoluminescence (PL) of MoS2 monolayer. Usually, the detected values of DVP in MoS2 monolayer show achiral property under optical excitation of opposite helicities due to reciprocal phonon-assisted intervalley scattering process. Here, it is reported that valley-polarized PL of MoS2 can be tailored through near-field interaction with plasmonic chiral metasurface. The resonant field of the chiral metasurface couples with valley-polarized excitons, and tailors the measured PL spectra in the far-field, resulting in observation of chiral DVP of MoS2-metasurface under opposite helicities excitations. Valley-contrast PL in the chiral heterostructure is also observed when illuminated by linearly polarized light. The manipulation of valley-polarized PL in 2D materials using chiral metasurface represents a viable route toward valley-polaritonic devices.


Advanced Materials, 2018. 30(34). Advanced Materials - 2018 - Li.pdf