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Continuous angular control over anisotropic photoemission from isotropic gold nanoshells.

Jacob Pettine¹, Andrea Marton Menendez¹, David J Nesbitt¹

¹National Institute of Standards and Technology, JILA, University of Colorado Boulder, Boulder, Colorado 80309, USA.

The Journal of Chemical Physics

|September 16, 2020

Summary

Linear laser polarization controls hot electron emission from gold nanoshells. This breakthrough enables precise ultrafast spatiotemporal control over hot carrier dynamics in nanoplasmonic systems.

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Area of Science:

Plasmonics
Nanophotonics
Materials Science

Background:

Hot carriers in metal nanoparticles are crucial for applications like catalysis and optoelectronics.
Understanding and controlling hot carrier dynamics is key to optimizing these processes.
Current methods often rely on particle geometry to tune optical control, limiting flexibility.

Purpose of the Study:

To introduce a novel method for continuously controlling hot electron excitation and emission distributions.
To investigate the role of linear laser polarization in breaking azimuthal symmetry in gold nanoshells.
To demonstrate ultrafast spatiotemporal control over hot carrier dynamics.

Main Methods:

Utilizing angle-resolved photoelectron velocity map imaging to analyze hot electron emission.

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Employing simulations of plasmonic electric field distributions.

Conducting ballistic Monte Carlo modeling of hot electron dynamics.

Main Results:

Hot electrons are predominantly emitted orthogonal to the laser-defined plasmon resonance axis in gold nanoshells.
Anisotropic emission was observed in nanoshells but not in solid nanospheres.
Simulations accurately recapitulated the experimental observations.

Conclusions:

Linear laser polarization offers a powerful tool for controlling hot carrier emission in nanoplasmonics.
Gold nanoshells exhibit unique anisotropic hot electron emission properties.
The findings provide a predictive understanding for ultrafast spatiotemporal control of hot carriers.