journal article·2024-06-25

Out-of-plane Emission Dipole of Second Harmonic Generation in Odd- and Even-layered vdWs Janus Nb3SeI7

Jia-Peng Wang, Xinfeng Chen, Qiyi Zhao, Yuqiang Fang, Quan Liu, Jierui Fu, Yue Liu, Xinlong Xu, Jia Zhang, Liang Zhen, Cheng-Yan Xu, Fuqiang Huang, Alfred J. Meixner, Dai Zhang, Gaoyang Gou, Yang Li

ACS Nano· Volume 18· Issue 25
Publisher page

Abstract

Integration of atomically thin nonlinear optical (NLO) devices demands an out-of-plane (OP) emission dipole of second harmonic generation (SHG) to enhance the spontaneous emission for nanophotonics. However, the research on van der Waals (vdWs) materials with an OP emission dipole of SHG is still in its infancy. Here, by coupling back focal plane (BFP) imaging with numerical simulations and density functional theory (DFT) calculations, we demonstrate that vdWs Janus Nb 3 SeI 7, ranging from bulk to the monolayer limit, exhibits a dominant OP emission dipole of SHG owing to the breaking of the OP symmetry. Explicitly, even-layered Nb 3 SeI 7 with C 6v symmetry is predicted to exhibit a pure OP emission dipole attributed to the only second-order susceptibility coefficient χ zxx . Meanwhile, although odd-layered Nb 3 SeI 7 with C 3v symmetry has both OP and IP dipole components (χ zxx and χ yyy ), the value of χ zxx is 1 order of magnitude greater than that of χ yyy, leading to an approximate OP emission dipole of SHG. Moreover, the crystal symmetry and OP emission dipole can be preserved under hydrostatic pressure, accompanied by the enhanced χ zxx and the resulting 3-fold increase in SHG intensity. The reported stable OP dipole in 2D vdWs Nb 3 SeI 7 can facilitate the rapid development of chip-integrated NLO devices.
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Research context

OpenAlex topics: Advanced Fiber Laser Technologies · 2D Materials and Applications · Photorefractive and Nonlinear Optics

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

School of Materials Science and Engineering, Harbin Institute of Technology, Harbin 150001, China

Frontier Institute of Science and Technology & State Key Laboratory of Electrical Insulation and Power Equipment, Xi’an Jiaotong University, Xi’ an 710049, China

School of Science, Xi’an University of Posts and Telecommunications, Xi’an 710199, China

State Key Laboratory of High-Performance Ceramics and Superfine Microstructure Shanghai Institute of Ceramics Chinese Academy of Sciences, Shanghai 200050, China

Institute of Physical and Theoretical Chemistry, Eberhard Karls University Tübingen, Tübingen 72076, Germany

School of Physics, Northwest University, Xi’an 710069, China

MOE Key Laboratory of Micro-Systems and Micro-Structures Manufacturing, Harbin Institute of Technology, Harbin 150080, China

Sauvage Laboratory for Smart Materials, School of Materials Science and Engineering, Harbin Institute of Technology Shenzhen, Shenzhen 518055, China

Funding

National Key Research and Development Program of China · Key Science and Technology Program of Shaanxi Province · Deutsche Forschungsgemeinschaft · Fundamental Research Funds for the Central Universities · Alexander von Humboldt-Stiftung · National Natural Science Foundation of China · Eberhard Karls Universit?t T?bingen

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