Resolving plasmon-mediated high-order multiphoton excitation pathways in dolmen nanostructures using ultrafast nonlinear optical interferometry

Author:

Zhao Tian1ORCID,Liu Xiaoying2ORCID,Nepal Dhriti3ORCID,Park Kyoungyeon3ORCID,Vaia Richard3ORCID,Nealey Paul2ORCID,Knappenberger Kenneth L.1ORCID

Affiliation:

1. Department of Chemistry, Pennsylvania State University 1 , University Park, Pennsylvania 16802, USA

2. Pritzker School of Molecular Engineering, University of Chicago 2 , Chicago, Illinois 60637, USA

3. Air Force Research Laboratory 3 , 2491 Hobson Way, Wright Patterson Air Force Base, Dayton, Ohio 45433, USA

Abstract

The multiphoton excitation pathways of plasmonic nanorod assemblies are described. By using dolmen structures formed from the directed assembly of three gold nanorods, plasmon-mediated three-photon excitation is resolved. These high-order multiphoton excitation channels were accessed by resonantly exciting a hybrid mode of the dolmen structure that was resonant with the 800-nm carrier wavelength of an ultrafast laser system. Rotation of the exciting field polarization to a non-resonant configuration did not generate third-order responses. Hence, the multiphoton excitation and resultant non-equilibrium electron distributions were generated by structure- and mode-selective excitation. Correlation between high-order and resonant plasmon excitation was achieved through sub-cycle time-resolved interferometric detection of incoherent nonlinear emission signals. The results illustrate the advantages of nonlinear optical interferometry and Fourier analysis for distinguishing plasmon-mediated processes from those that do not require plasmon excitation.

Funder

Air Force Office of Scientific Research

Publisher

AIP Publishing

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