1.School of Electrical and Electronic Engineering, Nanyang Technological University, 639798 Singapore, Singapore
2.School of Material Science and Engineering, Nanyang Technological University, 639798 Singapore, Singapore
3.CINTRA CNRS/NTU/THALES, UMI 3288, Research Techno Plaza, Nanyang Technological University, 637371 Singapore, Singapore
4.School of Materials Science and Engineering, Harbin Institute of Technology, 150001 Harbin, China
5.Department of Chemistry, National University of Singapore, 117543 Singapore, Singapore
6.GPL Photonics Lab, State Key Laboratory of Applied Optics, Changchun Institute of Optics, Fine Mechanics and Physics, Chinese Academy of Sciences, 130033 Changchun, China
7.School of Electronics and Information Engineering, Sichuan University, 610064 Chengdu, Sichuan, China
8.School of Physical and Mathematical Sciences, Nanyang Technological University, 637371 Singapore, Singapore
9.Departments of Electrical and Computer Engineering, Physics and Astronomy, and Materials Science and NanoEngineering, Rice University, Houston, TX, USA
Xingji Li (lxj0218@hit.edu.cn)
Zheng Liu (z.liu@ntu.edu.sg)
Qi Jie Wang (qjwang@ntu.edu.sg)
Published:31 August 2024,
Published Online:27 May 2024,
Received:14 January 2024,
Revised:03 May 2024,
Accepted:09 May 2024
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Zhu, S. et al. Strong nonlinear optical processes with extraordinary polarization anisotropy in inversion-symmetry broken two-dimensional PdPSe. Light: Science & Applications, 13, 1524-1533 (2024).
Zhu, S. et al. Strong nonlinear optical processes with extraordinary polarization anisotropy in inversion-symmetry broken two-dimensional PdPSe. Light: Science & Applications, 13, 1524-1533 (2024). DOI: 10.1038/s41377-024-01474-6.
Nonlinear optical activities
especially second harmonic generation (SHG)
are key phenomena in inversion-symmetry-broken two-dimensional (2D) transition metal dichalcogenides (TMDCs). On the other hand
anisotropic nonlinear optical processes are important for unique applications in nano-nonlinear photonic devices with polarization functions
having become one of focused research topics in the field of nonlinear photonics. However
the strong nonlinearity and strong optical anisotropy do not exist simultaneously in common 2D materials. Here
we demonstrate strong second-order and third-order susceptibilities of 64 pm/V and 6.2×10
−19
m
2
/V
2
respectively
in the even-layer PdPSe
which has not been discovered in other common TMDCs (e.g.
MoS
2
). Strikingly
it also simultaneously exhibited strong SHG anisotropy with an anisotropic ratio of ~45
which is the largest reported among all 2D materials to date
to the best of our knowledge. In addition
the SHG anisotropy ratio can be harnessed from 0.12 to 45 (375 times) by varying the excitation wavelength due to the dispersion of
$$ {\chi }^{(2)} $$
values. As an illustrative example
we further demonstrate polarized SHG imaging for potential applications in crystal orientation identification and polarization-dependent spatial encoding. These findings in 2D PdPSe are promising for nonlinear nanophotonic and optoelectronic applications.
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