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Evidence of High-Order Nonlinearities in Supercontinuum White-Light Generation from a Gold Nanofilm

Chen, Junsheng LU ; Krasavin, Alexey; Ginzburg, Pavel; Zayats, Anatoly V.; Pullerits, Tõnu LU and Karki, Khadga Jung LU (2018) In ACS Photonics 5(5). p.1927-1932
Abstract

White-light supercontinuum generation can be readily observed when gold nanostructures are irradiated with short pulses of light. It is believed that the nanostructures enhance the optical fields, which facilitates the supercontinuum white-light generation from the surrounding environment or the substrate. Here, we investigate the different nonlinear processes that contribute to the generation of the supercontinuum from plasmonic nanostructures themselves using a technique that isolates the different nonlinear contributions. By exciting a gold nanofilm with a pair of frequency shifted optical frequency combs, we demonstrate multiple modulation frequencies in the supercontinuum. Their dependence on the excitation intensity reveals that... (More)

White-light supercontinuum generation can be readily observed when gold nanostructures are irradiated with short pulses of light. It is believed that the nanostructures enhance the optical fields, which facilitates the supercontinuum white-light generation from the surrounding environment or the substrate. Here, we investigate the different nonlinear processes that contribute to the generation of the supercontinuum from plasmonic nanostructures themselves using a technique that isolates the different nonlinear contributions. By exciting a gold nanofilm with a pair of frequency shifted optical frequency combs, we demonstrate multiple modulation frequencies in the supercontinuum. Their dependence on the excitation intensity reveals that the supercontinuum originates from different orders of nonlinear light-matter interactions. This contrasts with the supercontinuum generation by a cascaded third-order optical nonlinear response in traditional dielectric-based white-light sources. The while-light emission from the gold nanofilm is efficient even under relatively weak excitation indicating that nonlocal effects in nanostructures may facilitate the supercontinuum generation by adding new pathways in the nonlinear interactions. The results provide experimental basis for the understanding of the collective nonlinear response of free-electrons in the metallic nanostructures and associated nonlinear processes, which are crucial in development of nonlinear metasurfaces and nanophotonic devices.

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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
nonlinear interactions, nonlocal response, rough metal films, white-light generation
in
ACS Photonics
volume
5
issue
5
pages
6 pages
publisher
The American Chemical Society
external identifiers
  • scopus:85047226176
ISSN
2330-4022
DOI
10.1021/acsphotonics.7b01125
language
English
LU publication?
yes
id
3c9d0ab0-8e59-4e3a-9c1d-f678d6d707e2
date added to LUP
2018-06-01 13:49:19
date last changed
2018-09-16 04:55:37
@article{3c9d0ab0-8e59-4e3a-9c1d-f678d6d707e2,
  abstract     = {<p>White-light supercontinuum generation can be readily observed when gold nanostructures are irradiated with short pulses of light. It is believed that the nanostructures enhance the optical fields, which facilitates the supercontinuum white-light generation from the surrounding environment or the substrate. Here, we investigate the different nonlinear processes that contribute to the generation of the supercontinuum from plasmonic nanostructures themselves using a technique that isolates the different nonlinear contributions. By exciting a gold nanofilm with a pair of frequency shifted optical frequency combs, we demonstrate multiple modulation frequencies in the supercontinuum. Their dependence on the excitation intensity reveals that the supercontinuum originates from different orders of nonlinear light-matter interactions. This contrasts with the supercontinuum generation by a cascaded third-order optical nonlinear response in traditional dielectric-based white-light sources. The while-light emission from the gold nanofilm is efficient even under relatively weak excitation indicating that nonlocal effects in nanostructures may facilitate the supercontinuum generation by adding new pathways in the nonlinear interactions. The results provide experimental basis for the understanding of the collective nonlinear response of free-electrons in the metallic nanostructures and associated nonlinear processes, which are crucial in development of nonlinear metasurfaces and nanophotonic devices.</p>},
  author       = {Chen, Junsheng and Krasavin, Alexey and Ginzburg, Pavel and Zayats, Anatoly V. and Pullerits, Tõnu and Karki, Khadga Jung},
  issn         = {2330-4022},
  keyword      = {nonlinear interactions,nonlocal response,rough metal films,white-light generation},
  language     = {eng},
  month        = {05},
  number       = {5},
  pages        = {1927--1932},
  publisher    = {The American Chemical Society},
  series       = {ACS Photonics},
  title        = {Evidence of High-Order Nonlinearities in Supercontinuum White-Light Generation from a Gold Nanofilm},
  url          = {http://dx.doi.org/10.1021/acsphotonics.7b01125},
  volume       = {5},
  year         = {2018},
}