Yutian Yang, Yingying Wang, Jingsi Qiao, Weiwei Zhao, Yuanfang Yu, Shaopeng Feng, Xuhong An, Jialin Zhang, Wei Ji, Xinran Wang, Junpeng Lu & Zhenhua Ni
Abstract
The functionality of 2D molecular crystal-based devices crucially depends on their intrinsic properties, such as molecular energy levels, light absorption efficiency, and dielectric permittivity, which are highly sensitive to molecular aggregation. Here, it is demonstrated that the dielectric permittivity of the 2,7-dioctyl[1]benzothieno[3,2-b][1]benzothiophene (C8-BTBT) molecular crystals on monolayer WS2 substrates can be tuned from 4.62 in the wetting layer to 2.25 in the second layer. Its origin lies in the different molecular orientations in the wetting layer (lying-down) and in the subsequently stacked layers (standing-up), which lead to a positive Coulomb coupling (JCoup) value (H-aggregation) and a negative JCoup value (J-aggregation), respectively. Polarized optical contrast spectroscopy reveals that the permittivity of C8-BTBT is anisotropic, and its direction is related to the underlying substrate. The study offers guidelines for future manipulation of the permittivity of 2D molecular crystals, which may promote their applications toward various electronic and optoelectronic devices.
Yuan Huang, Yun-Kun Wang, Xin-Yu Huang, Guan-Hua Zhang, Xu Han, Yang Yang, Yunan Gao, Lei Meng, Yushu Wang, Guang-Zhou Geng, Li-Wei Liu, Lin Zhao, Zhi-Hai Cheng, Xin-Feng Liu, Ze-Feng Ren, Hui-Xia Yang, Yufeng Hao, Hong-Jun Gao, Xing-Jiang Zhou, Wei Ji & Ye-Liang Wang
Abstract
Two-dimensional (2D) materials are highly sensitive to substrates, interfaces, and the surrounding environments. Suspended 2D materials are free from substrate-induced effects, thus an ideal approach to study their intrinsic properties. However, it is very challenging to prepare large-area suspended 2D materials with high efficiency. Here we report a universal method, based on pretreatments of densely patterned hole array substrates with either oxygen-plasma or gold film deposition, to prepare large-area suspended mono- and few-layer 2D materials. Multiple structural, optical, and electrical characterization tools were used to fully evaluate the improved performance of various suspended 2D layers. Some of these observations reported in this study are: (1) Observation of a new Raman low frequency mode for the suspended MoS2; (2) Significantly stronger photoluminescence (PL) and second harmonic generation (SHG) signals of suspended WSe2, which enables the study of new optical transition processes; (3) The low energy electron diffraction pattern on suspended MoS2 also exhibits much sharper spots than that on the supported area; and (4) The mobility of suspended graphene device approaches 300 000 cm2 V−1 s−1, which is desirable to explore the intrinsic properties of graphene. This work provides an innovative and efficient route for fabricating suspended 2D materials, and we expect that it can be broadly used for studying intrinsic properties of 2D materials and in applications of hybrid active nanophotonic and electronic devices.
A confined electronic system can host a wide variety of fascinating electronic, magnetic, valleytronic and photonic phenomena due to its reduced symmetry and quantum confinement effect. For the recently emerging one-dimensional van der Waals (1D vdW) materials with electrons confined in 1D sub-units, an enormous variety of intriguing physical properties and functionalities can be expected. Here, we demonstrate the coexistence of giant linear/nonlinear optical anisotropy and high emission yield in fibrous red phosphorus (FRP), an exotic 1D vdW semiconductor with quasi-flat bands and a sizeable bandgap in the visible spectral range. The degree of photoluminescence (third-order nonlinear) anisotropy can reach 90% (86%), comparable to the best performance achieved so far. Meanwhile, the photoluminescence (third-harmonic generation) intensity in 1D vdW FRP is strong, with quantum efficiency (third-order susceptibility) four (three) times larger than that in the most well-known 2D vdW materials (e.g., MoS2). The concurrent realization of large linear/nonlinear optical anisotropy and emission intensity in 1D vdW FRP paves the way towards transforming the landscape of technological innovations in photonics and optoelectronics.
