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

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

doi:10.1002/adma.202210894

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

Journal Article · Thu Mar 23 00:00:00 EDT 2023 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202210894· OSTI ID:2421111

^[1]; Luo, Yue ^[2]; Chiu, Ming‐Hui ^[3]; Shi, Chuqiao ^[4]; Ji, Xiang ^[3]; Pieshkov, Tymofii S. ^[4]; Lin, Yuxuan ^[5]; Tang, Hao‐Lin ^[3]; Akey, Austin J. ^[2]; Gardener, Jules A. ^[2]; Park, Ji‐Hoon ^[6]; Tung, Vincent ^[7]; Ling, Xi ^[8]; Qian, Xiaofeng ^[9]; Wilson, William L. ^[2]; Han, Yimo ^[4]; Tisdale, William A. ^[6]; ^[6]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); OSTI
Harvard Univ., Cambridge, MA (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); King Abdullah University of Science and Technology (KAUST), Thuwal (Saudi Arabia)
Rice Univ., Houston, TX (United States)
University of California, Berkeley, CA (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
King Abdullah University of Science and Technology (KAUST), Thuwal (Saudi Arabia)
Boston Univ., MA (United States)
Texas A & M Univ., College Station, TX (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Harvard Univ., Cambridge, MA (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019300; SC0019345; SC0020042

OSTI ID:: 2421111

Alternate ID(s):: OSTI ID: 1973522

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 26 Vol. 35; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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