Unexpected Near-Infrared to Visible Nonlinear Optical Properties from 2-D Polar Metals

Megan A. Steves; Yuanxi Wang; Natalie Briggs; Tian Zhao; Hesham El-Sherif; Brian M. Bersch; Shruti Subramanian; Chengye Dong; Timothy Bowen; Ana De La Fuente Duran; Katharina Nisi; Margaux Lassaunière; Ursula Wurstbauer; Nabil D. Bassim; Jose Fonseca; Jeremy T. Robinson; Vincent H. Crespi; Joshua Robinson; Kenneth L. Knappenberger

doi:10.1021/acs.nanolett.0c03481

Unexpected Near-Infrared to Visible Nonlinear Optical Properties from 2-D Polar Metals

Megan A. Steves, Yuanxi Wang, Natalie Briggs, Tian Zhao, Hesham El-Sherif, Brian M. Bersch, Shruti Subramanian, Chengye Dong, Timothy Bowen, Ana De La Fuente Duran, Katharina Nisi, Margaux Lassaunière, Ursula Wurstbauer, Nabil D. Bassim, Jose Fonseca, Jeremy T. Robinson, Vincent H. Crespi, Joshua Robinson, Kenneth L. Knappenberger

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23 Scopus citations

Abstract

Near-infrared-to-visible second harmonic generation from air-stable two-dimensional polar gallium and indium metals is described. The photonic properties of 2D metals, including the largest second-order susceptibilities reported for metals (approaching 10 nm/V), are determined by the atomic-level structure and bonding of two-to-three-atom-thick crystalline films. The bond character evolved from covalent to metallic over a few atomic layers, changing the out-of-plane metal-metal bond distances by approximately ten percent (0.2 Å), resulting in symmetry breaking and an axial electrostatic dipole that mediated the large nonlinear response. Two different orientations of the crystalline metal atoms, corresponding to lateral displacements <2 Å, persisted in separate micrometer-scale terraces to generate distinct harmonic polarizations. This strong atomic-level structure-property interplay suggests metal photonic properties can be controlled with atomic precision.

Original language	English (US)
Pages (from-to)	8312-8318
Number of pages	7
Journal	Nano letters
Volume	20
Issue number	11
DOIs	https://doi.org/10.1021/acs.nanolett.0c03481
State	Published - Nov 11 2020

All Science Journal Classification (ASJC) codes

Bioengineering
General Chemistry
General Materials Science
Condensed Matter Physics
Mechanical Engineering

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10.1021/acs.nanolett.0c03481

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Steves, M. A., Wang, Y., Briggs, N., Zhao, T., El-Sherif, H., Bersch, B. M., Subramanian, S., Dong, C., Bowen, T., Fuente Duran, A. D. L., Nisi, K., Lassaunière, M., Wurstbauer, U., Bassim, N. D., Fonseca, J., Robinson, J. T., Crespi, V. H., Robinson, J., & Knappenberger, K. L. (2020). Unexpected Near-Infrared to Visible Nonlinear Optical Properties from 2-D Polar Metals. Nano letters, 20(11), 8312-8318. https://doi.org/10.1021/acs.nanolett.0c03481

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title = "Unexpected Near-Infrared to Visible Nonlinear Optical Properties from 2-D Polar Metals",

abstract = "Near-infrared-to-visible second harmonic generation from air-stable two-dimensional polar gallium and indium metals is described. The photonic properties of 2D metals, including the largest second-order susceptibilities reported for metals (approaching 10 nm/V), are determined by the atomic-level structure and bonding of two-to-three-atom-thick crystalline films. The bond character evolved from covalent to metallic over a few atomic layers, changing the out-of-plane metal-metal bond distances by approximately ten percent (0.2 {\AA}), resulting in symmetry breaking and an axial electrostatic dipole that mediated the large nonlinear response. Two different orientations of the crystalline metal atoms, corresponding to lateral displacements <2 {\AA}, persisted in separate micrometer-scale terraces to generate distinct harmonic polarizations. This strong atomic-level structure-property interplay suggests metal photonic properties can be controlled with atomic precision.",

author = "Steves, {Megan A.} and Yuanxi Wang and Natalie Briggs and Tian Zhao and Hesham El-Sherif and Bersch, {Brian M.} and Shruti Subramanian and Chengye Dong and Timothy Bowen and {Fuente Duran}, {Ana De La} and Katharina Nisi and Margaux Lassauni{\`e}re and Ursula Wurstbauer and Bassim, {Nabil D.} and Jose Fonseca and Robinson, {Jeremy T.} and Crespi, {Vincent H.} and Joshua Robinson and Knappenberger, {Kenneth L.}",

year = "2020",

month = nov,

day = "11",

doi = "10.1021/acs.nanolett.0c03481",

language = "English (US)",

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Steves, MA, Wang, Y, Briggs, N, Zhao, T, El-Sherif, H, Bersch, BM, Subramanian, S, Dong, C, Bowen, T, Fuente Duran, ADL, Nisi, K, Lassaunière, M, Wurstbauer, U, Bassim, ND, Fonseca, J, Robinson, JT, Crespi, VH , Robinson, J & Knappenberger, KL 2020, 'Unexpected Near-Infrared to Visible Nonlinear Optical Properties from 2-D Polar Metals', Nano letters, vol. 20, no. 11, pp. 8312-8318. https://doi.org/10.1021/acs.nanolett.0c03481

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AU - Steves, Megan A.

AU - Wang, Yuanxi

AU - Briggs, Natalie

AU - Zhao, Tian

AU - El-Sherif, Hesham

AU - Bersch, Brian M.

AU - Subramanian, Shruti

AU - Dong, Chengye

AU - Bowen, Timothy

AU - Fuente Duran, Ana De La

AU - Nisi, Katharina

AU - Lassaunière, Margaux

AU - Wurstbauer, Ursula

AU - Bassim, Nabil D.

AU - Fonseca, Jose

AU - Robinson, Jeremy T.

AU - Crespi, Vincent H.

AU - Robinson, Joshua

AU - Knappenberger, Kenneth L.

PY - 2020/11/11

Y1 - 2020/11/11

N2 - Near-infrared-to-visible second harmonic generation from air-stable two-dimensional polar gallium and indium metals is described. The photonic properties of 2D metals, including the largest second-order susceptibilities reported for metals (approaching 10 nm/V), are determined by the atomic-level structure and bonding of two-to-three-atom-thick crystalline films. The bond character evolved from covalent to metallic over a few atomic layers, changing the out-of-plane metal-metal bond distances by approximately ten percent (0.2 Å), resulting in symmetry breaking and an axial electrostatic dipole that mediated the large nonlinear response. Two different orientations of the crystalline metal atoms, corresponding to lateral displacements <2 Å, persisted in separate micrometer-scale terraces to generate distinct harmonic polarizations. This strong atomic-level structure-property interplay suggests metal photonic properties can be controlled with atomic precision.

AB - Near-infrared-to-visible second harmonic generation from air-stable two-dimensional polar gallium and indium metals is described. The photonic properties of 2D metals, including the largest second-order susceptibilities reported for metals (approaching 10 nm/V), are determined by the atomic-level structure and bonding of two-to-three-atom-thick crystalline films. The bond character evolved from covalent to metallic over a few atomic layers, changing the out-of-plane metal-metal bond distances by approximately ten percent (0.2 Å), resulting in symmetry breaking and an axial electrostatic dipole that mediated the large nonlinear response. Two different orientations of the crystalline metal atoms, corresponding to lateral displacements <2 Å, persisted in separate micrometer-scale terraces to generate distinct harmonic polarizations. This strong atomic-level structure-property interplay suggests metal photonic properties can be controlled with atomic precision.

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JO - Nano letters

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IS - 11

ER -

Unexpected Near-Infrared to Visible Nonlinear Optical Properties from 2-D Polar Metals

Abstract

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