Kuis, RobinsonGougousi, TheodosiaBasaldua, IsaacBurkins, PaulKropp, Jaron A.Johnson, Anthony M.2019-12-172019-12-172019-10-17Kuis, Robinson; Gougousi, Theodosia; Basaldua, Isaac; Burkins, Paul; Kropp, Jaron A.; Johnson, Anthony M.; Engineering of Large Third-Order Nonlinearities in Atomic Layer Deposition Grown Nitrogen-Enriched TiO₂; ACS Photonics 6, 11, 2966-2973 (2019); https://pubs.acs.org/doi/full/10.1021/acsphotonics.9b01176https://doi.org/10.1021/acsphotonics.9b01176http://hdl.handle.net/11603/16718The third-order nonlinear optical properties of Nitrogen-enriched TiO₂ films deposited by Atomic Layer Deposition (ALD) at a temperature between 100 – 300°C on quartz substrates were studied using thermally managed Z-scan technique. TiO₂ oxide films prepared by Physical Vapor Deposition (PVD) at room temperature were used as control samples. The as-grown ALD films deposited at 150 – 300°C exhibited values for the nonlinear index of refraction, n₂, between 0.6x10ˉ¹¹ and 1x10ˉ⁹ cm²/W, which is 4–6 order larger than previously reported. Annealing the films, for 3 hours at 450°C in air, reduced the nonlinearities below the detection limit of the experimental setup. Similarly, as-grown 100°C ALD and PVD films did not produce a discernible Zscan trace. Composition analysis performed by x-ray photoelectrons spectroscopy (XPS) reveals the presence of Ti-O-N metallic bonds in the films that showed high nonlinear optical response. The presence of the metallic bonding gives the films deposited on Si (100) a golden color. These results demonstrate the possibility of a new class of thin-film nonlinear materials that their properties can be tailored by controlling the film composition.2 filesen-USThis item is likely protected under Title 17 of the U.S. Copyright Law. Unless on a Creative Commons license, for uses protected by Copyright Law, contact the copyright holder or the author.This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Photonics, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acsphotonics.9b01176.Access to this item will begin on 2020-10-17nanophotonicsnonlinear opticsthermally managed Z-scanTiO₂ filmatomic layer depositionCMOS compatible filmsText