Unexpected Near-Infrared to Visible Non-linear Optical Properties from Two-Dimensional 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 10nm/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 ), 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 , persisted in separate micron-scale terraces to generate distinct harmonic polarizations. This strong atomic-level structure-property interplay suggests metal photonic properties can be controlled with atomic precision.
Keywords
Cite
@article{arxiv.2004.01809,
title = {Unexpected Near-Infrared to Visible Non-linear Optical Properties from Two-Dimensional Polar Metals},
author = {Megan A. Steves and Yuanxi Wang and Natalie Briggs and Tian Zhao and Hesham El-Sherif and Brian Bersch and Shruti Subramanian and Chengye Dong and Timothy Bowen and Ana De La Fuente Duran and Katharina Nisi and Margaux Lassaunière and Ursula Wurstbauer and Nabil Bassim and Jose J. Fonseca and Jeremy T. Robinson and Vincent Crespi and Joshua Robinson and Kenneth L. Knappenberger},
journal= {arXiv preprint arXiv:2004.01809},
year = {2020}
}