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

Research output: Contribution to journalArticlepeer-review

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 languageEnglish (US)
Pages (from-to)8312-8318
Number of pages7
JournalNano letters
Volume20
Issue number11
DOIs
StatePublished - Nov 11 2020

All Science Journal Classification (ASJC) codes

  • Bioengineering
  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanical Engineering

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