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.
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Optical field tuning of localized plasmon modes in Ag microcrystals at the nanofemto scale
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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
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Maciej Dąbrowski;
Maciej Dąbrowski
2
Department of Physics and Astronomy, University of Exeter
, Exeter EX4 4QL, United Kingdom
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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: petek@pitt.edu
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a)Author to whom correspondence should be addressed: petek@pitt.edu
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
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