Predictability of Localized Plasmonic Responses in Nanoparticle Assemblies

Kevin M. Roccapriore, Maxim Ziatdinov, Shin Hum Cho, Jordan A. Hachtel, Sergei V. Kalinin

Research output: Contribution to journalArticlepeer-review

24 Scopus citations

Abstract

Design of nanoscale structures with desired optical properties is a key task for nanophotonics. Here, the correlative relationship between local nanoparticle geometries and their plasmonic responses is established using encoder-decoder neural networks. In the im2spec network, the relationship between local particle geometries and local spectra is established via encoding the observed geometries to a small number of latent variables and subsequently decoding into plasmonic spectra; in the spec2im network, the relationship is reversed. Surprisingly, these reduced descriptions allow high-veracity predictions of local responses based on geometries for fixed compositions and surface chemical states. Analysis of the latent space distributions and the corresponding decoded and closest (in latent space) encoded images yields insight into the generative mechanisms of plasmonic interactions in the nanoparticle arrays. Ultimately, this approach creates a path toward determining configurations that yield the spectrum closest to the desired one, paving the way for stochastic design of nanoplasmonic structures.

Original languageEnglish
Article number2100181
JournalSmall
Volume17
Issue number21
DOIs
StatePublished - May 27 2021

Funding

This effort (ML and STEM) is based upon work supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), Materials Sciences and Engineering Division (K.M.R., S.V.K.) and was performed and partially supported (J.A.H., M.Z.) at the Oak Ridge National Laboratory's Center for Nanophase Materials Sciences (CNMS), a U.S. Department of Energy, Office of Science User Facility. S.H.C. acknowledges (NSF, CHE‐19052631609656, CBET‐1704634, NASCENT, an NSF ERC EEC‐1160494, and CDCM, an NSF MRSEC DMR‐1720595), the Welch Foundation (F‐1848), and the Fulbright Program (IIE‐15151071). The authors thank Andrew Lupini for his fruitful discussions and valuable advice in the manuscript.

FundersFunder number
CDCMMRSEC DMR‐1720595
CNMS
NSF ERCEEC‐1160494
Oak Ridge National Laboratory
National Science FoundationCBET‐1704634, CHE‐19052631609656
U.S. Department of Energy
Welch FoundationIIE‐15151071, F‐1848
Office of Science
Basic Energy Sciences
Division of Materials Sciences and Engineering

    Keywords

    • electron energy loss spectroscopy
    • machine learning
    • nanoparticle arrays
    • nanophotonics
    • plasmonics
    • scanning transmission electron microscopy

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