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Title: Precision Plasmonics with Monomers and Dimers of Spherical Gold Nanoparticles: Nonequilibrium Dynamics at the Time and Space Limits

Abstract

Monomers and dimers of spherical gold nanoparticles (NPs) exhibit highly uniform plasmonic properties at the single-particle level due to their high structural homogeneity (precision plasmonics). Recent investigations in precision plasmonics have largely focused on static properties using conventional techniques such as transmission electron microscopy and optical dark-field microscopy. Here in this Feature Article, we first highlight the application of femtosecond time-resolved electron diffraction for monitoring the nonequilibrium dynamics of spherical gold NPs after ultrafast optical excitation. The analysis of the transient diffraction patterns allows us to directly obtain quantitative information on the incoherent excitation of the lattice, that is, heating upon electron–lattice equilibration, as well as on the development of strain due to lattice expansion on picosecond time scales. The controlled assembly of two spherical gold NPs into a dimer with a few nanometers gap leads to unique optical properties. Specifically, extremely high electric fields (hot spot) in the gap are generated upon resonant optical excitation. Conventional optical microscopy cannot spatially resolve this unique hot spot due to the optical diffraction limit. We therefore employed nonlinear photoemission electron microscopy to visualize hot spots in single dimers of spherical gold NPs. A quantitative comparison of different single dimers confirms the homogeneitymore » of the hot spots on the single-particle level. Finally, overall, these initial results are highly encouraging because they pave the way to investigate nonequilibrium dynamics in highly uniform plasmonic nanostructures at the time and space limits.« less

Authors:
 [1];  [1];  [2];  [2]; ORCiD logo [2];  [2];  [3];  [3];  [3];  [3];  [3];  [3];  [3]; ORCiD logo [2];  [2]; ORCiD logo [1]
  1. Univ. of Duisburg-Essen, Essen (Germany). Dept. of Chemistry and Center for Nanointegration Duisburg-Essen (CENIDE)
  2. Univ. of Duisburg-Essen, Duisburg (Germany). Dept. of Physics and Center for Nanointegration Duisburg-Essen (CENIDE)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1532483
Grant/Contract Number:  
AC02-76SF00515; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 123; Journal Issue: 21; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 70 PLASMA PHYSICS AND FUSION TECHNOLOGY

Citation Formats

Schumacher, L., Jose, J., Janoschka, D., Dreher, P., Davis, T. J., Ligges, M., Li, R., Mo, M., Park, S., Shen, X., Weathersby, S., Yang, J., Wang, X., Meyer zu Heringdorf, F., Sokolowski-Tinten, K., and Schlücker, S. Precision Plasmonics with Monomers and Dimers of Spherical Gold Nanoparticles: Nonequilibrium Dynamics at the Time and Space Limits. United States: N. p., 2019. Web. doi:10.1021/acs.jpcc.9b01007.
Schumacher, L., Jose, J., Janoschka, D., Dreher, P., Davis, T. J., Ligges, M., Li, R., Mo, M., Park, S., Shen, X., Weathersby, S., Yang, J., Wang, X., Meyer zu Heringdorf, F., Sokolowski-Tinten, K., & Schlücker, S. Precision Plasmonics with Monomers and Dimers of Spherical Gold Nanoparticles: Nonequilibrium Dynamics at the Time and Space Limits. United States. https://doi.org/10.1021/acs.jpcc.9b01007
Schumacher, L., Jose, J., Janoschka, D., Dreher, P., Davis, T. J., Ligges, M., Li, R., Mo, M., Park, S., Shen, X., Weathersby, S., Yang, J., Wang, X., Meyer zu Heringdorf, F., Sokolowski-Tinten, K., and Schlücker, S. Wed . "Precision Plasmonics with Monomers and Dimers of Spherical Gold Nanoparticles: Nonequilibrium Dynamics at the Time and Space Limits". United States. https://doi.org/10.1021/acs.jpcc.9b01007. https://www.osti.gov/servlets/purl/1532483.
@article{osti_1532483,
title = {Precision Plasmonics with Monomers and Dimers of Spherical Gold Nanoparticles: Nonequilibrium Dynamics at the Time and Space Limits},
author = {Schumacher, L. and Jose, J. and Janoschka, D. and Dreher, P. and Davis, T. J. and Ligges, M. and Li, R. and Mo, M. and Park, S. and Shen, X. and Weathersby, S. and Yang, J. and Wang, X. and Meyer zu Heringdorf, F. and Sokolowski-Tinten, K. and Schlücker, S.},
abstractNote = {Monomers and dimers of spherical gold nanoparticles (NPs) exhibit highly uniform plasmonic properties at the single-particle level due to their high structural homogeneity (precision plasmonics). Recent investigations in precision plasmonics have largely focused on static properties using conventional techniques such as transmission electron microscopy and optical dark-field microscopy. Here in this Feature Article, we first highlight the application of femtosecond time-resolved electron diffraction for monitoring the nonequilibrium dynamics of spherical gold NPs after ultrafast optical excitation. The analysis of the transient diffraction patterns allows us to directly obtain quantitative information on the incoherent excitation of the lattice, that is, heating upon electron–lattice equilibration, as well as on the development of strain due to lattice expansion on picosecond time scales. The controlled assembly of two spherical gold NPs into a dimer with a few nanometers gap leads to unique optical properties. Specifically, extremely high electric fields (hot spot) in the gap are generated upon resonant optical excitation. Conventional optical microscopy cannot spatially resolve this unique hot spot due to the optical diffraction limit. We therefore employed nonlinear photoemission electron microscopy to visualize hot spots in single dimers of spherical gold NPs. A quantitative comparison of different single dimers confirms the homogeneity of the hot spots on the single-particle level. Finally, overall, these initial results are highly encouraging because they pave the way to investigate nonequilibrium dynamics in highly uniform plasmonic nanostructures at the time and space limits.},
doi = {10.1021/acs.jpcc.9b01007},
journal = {Journal of Physical Chemistry. C},
number = 21,
volume = 123,
place = {United States},
year = {Wed Apr 17 00:00:00 EDT 2019},
month = {Wed Apr 17 00:00:00 EDT 2019}
}

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