Nanoscale plasmonic field enhancement at sub-wavelength metallic particles is crucial for surface sensitive spectroscopy, ultrafast microscopy, and nanoscale energy transduction. Here, we demonstrate control of the spatial distribution of localized surface plasmon modes at sub-optical-wavelength crystalline silver (Ag) micropyramids grown on a Si(001) surface. We employ multiphoton photoemission electron microscopy (mP-PEEM) to image how the plasmonic field distributions vary with the photon energy, light polarization, and phase in coherent two-pulse excitation. For photon energy hυ > 2.0 eV, the mP-PEEM images show single photoemission locus, which splits into a dipolar pattern that straddles the Ag crystal at a lower energy. We attribute the variation to the migration of plasmon resonances from the Ag/vacuum to the Ag/Si interfaces by choice of the photon energy. Furthermore, the dipolar response of the Ag/Si interface follows the polarization state of light: for linearly polarized excitations, the plasmon dipole follows the in-plane electric field vector, while for circularly polarized excitations, it tilts in the direction of the handedness due to the conversion of spin angular momentum of light into orbital angular momentum of the plasmons excited in the sample. Finally, we show the coherent control of the spatial plasmon distribution by exciting the sample with two identical circularly polarized light pulses with delay defined with attosecond precision. The near field distribution wobbles at the pyramid base as the pump–probe delay is advanced due to interferences among the contributing fields. We illustrate how the frequency, polarization, and pulse structure can be used to design and control plasmon fields on the nanofemto scale for applications in chemistry and physics.
Skip Nav Destination
Optical field tuning of localized plasmon modes in Ag microcrystals at the nanofemto scale
Article navigation
7 February 2020
Research Article|
February 03 2020
Optical field tuning of localized plasmon modes in Ag microcrystals at the nanofemto scale
Special Collection:
Emerging Directions in Plasmonics
Yanan Dai;
Yanan Dai
1
Department of Physics and Astronomy and Pittsburgh Quantum Institute, University of Pittsburgh
, Pittsburgh, Pennsylvania 15260, USA
Search for other works by this author on:
Maciej Dąbrowski;
Maciej Dąbrowski
2
Department of Physics and Astronomy, University of Exeter
, Exeter EX4 4QL, United Kingdom
Search for other works by this author on:
Hrvoje Petek
Hrvoje Petek
a)
1
Department of Physics and Astronomy and Pittsburgh Quantum Institute, University of Pittsburgh
, Pittsburgh, Pennsylvania 15260, USA
a)Author to whom correspondence should be addressed: [email protected]
Search for other works by this author on:
1
Department of Physics and Astronomy and Pittsburgh Quantum Institute, University of Pittsburgh
, Pittsburgh, Pennsylvania 15260, USA
2
Department of Physics and Astronomy, University of Exeter
, Exeter EX4 4QL, United Kingdom
a)Author to whom correspondence should be addressed: [email protected]
Note: This paper is part of the JCP Special Topic on Emerging Directions in Plasmonics.
J. Chem. Phys. 152, 054201 (2020)
Article history
Received:
November 22 2019
Accepted:
January 09 2020
Citation
Yanan Dai, Maciej Dąbrowski, Hrvoje Petek; Optical field tuning of localized plasmon modes in Ag microcrystals at the nanofemto scale. J. Chem. Phys. 7 February 2020; 152 (5): 054201. https://doi.org/10.1063/1.5139543
Download citation file:
Pay-Per-View Access
$40.00
Sign In
You could not be signed in. Please check your credentials and make sure you have an active account and try again.
Citing articles via
DeePMD-kit v2: A software package for deep potential models
Jinzhe Zeng, Duo Zhang, et al.
CREST—A program for the exploration of low-energy molecular chemical space
Philipp Pracht, Stefan Grimme, et al.
Related Content
A topological lattice of plasmonic merons
Appl. Phys. Rev. (December 2021)
Ultrafast microscopy of a twisted plasmonic spin skyrmion
Appl. Phys. Rev. (March 2022)
Optical properties of metal nanoparticles as probed by photoemission electron microscopy
J. Appl. Phys. (April 2007)
Plasmon-induced optical field enhancement studied by correlated scanning and photoemission electron microscopy
J. Chem. Phys. (April 2013)
Nanofabrication of plasmon-tunable nanoantennas for tip-enhanced Raman spectroscopy
J. Chem. Phys. (September 2020)