Giant Nonlinear Optical Response via Coherent Stacking of In-Plane Ferroelectric Layers

Nannan Mao; Yue Luo; Ming-Hui Chiu; Chuqiao Shi; Xiang Ji; Tymofii S Pieshkov; Yuxuan Lin; Hao-Lin Tang; Austin J Akey; Jules A Gardener; Ji-Hoon Park; Vincent Tung; Xi Ling; Xiaofeng Qian; William L Wilson; Yimo Han; William A Tisdale; Jing Kong

doi:10.1002/adma.202210894

Giant Nonlinear Optical Response via Coherent Stacking of In-Plane Ferroelectric Layers

Adv Mater. 2023 Jun;35(26):e2210894. doi: 10.1002/adma.202210894. Epub 2023 May 12.

Authors

Nannan Mao^{1

2}, Yue Luo^{3

4}, Ming-Hui Chiu^{1

5}, Chuqiao Shi⁶, Xiang Ji^{1

5}, Tymofii S Pieshkov⁶, Yuxuan Lin⁷, Hao-Lin Tang^{1

5}, Austin J Akey³, Jules A Gardener³, Ji-Hoon Park¹, Vincent Tung⁵, Xi Ling⁸, Xiaofeng Qian⁹, William L Wilson³, Yimo Han⁶, William A Tisdale², Jing Kong¹

Affiliations

¹ Department of Electrical Engineering and Computer Science, Massachusetts Institute of Technology, Cambridge, MA, 02139, USA.
² Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, MA, 02139, USA.
³ Center for Nanoscale Systems, Harvard University, Cambridge, MA, 02138, USA.
⁴ Department of Physics, Harvard University, Cambridge, MA, 02138, USA.
⁵ Material Science and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900, Saudi Arabia.
⁶ Department of Materials Science and NanoEngineering, Rice University, Houston, TX, 77005, USA.
⁷ Department of Electrical Engineering and Computer Sciences, University of California, Berkeley, CA, USA.
⁸ Department of Chemistry and Division of Materials Science and Engineering, Boston University, Boston, MA, 02215, USA.
⁹ Department of Materials Science and Engineering, Department of Electrical and Computer Engineering, Texas A&M University, College Station, Texas, 77843, USA.

PMID: 36959753
DOI: 10.1002/adma.202210894

Abstract

Thin ferroelectric materials hold great promise for compact nonvolatile memory and nonlinear optical and optoelectronic devices. Herein, an ultrathin in-plane ferroelectric material that exhibits a giant nonlinear optical effect, group-IV monochalcogenide SnSe, is reported. Nanometer-scale ferroelectric domains with ≈90°/270° twin boundaries or ≈180° domain walls are revealed in physical-vapor-deposited SnSe by lateral piezoresponse force microscopy. Atomic structure characterization reveals both parallel and antiparallel stacking of neighboring van der Waals ferroelectric layers, leading to ferroelectric or antiferroelectric ordering. Ferroelectric domains exhibit giant nonlinear optical activity due to coherent enhancement of second-harmonic fields and the as-resulted second-harmonic generation was observed to be 100 times more intense than monolayer WS₂ . This work demonstrates in-plane ferroelectric ordering and giant nonlinear optical activity in SnSe, which paves the way for applications in on-chip nonlinear optical components and nonvolatile memory devices.

Keywords: SnSe; ferroelectric domains; ferroelectric stacking; group-IV monochalcogenides; in-plane ferroelectric materials; physical vapor deposition; second-harmonic generation.

Abstract

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