Abstract

The near-field properties and dynamics of plasmonic nanostructures play a crucial role in several fundamental concepts in physics and chemistry, and they are widely relevant in plasmonic applications. Ultrafast photoemission electron microscopy (PEEM) is a novel approach that has been widely applied to probe plasmonic nanostructures from multiple domains. Furthermore, PEEM is the only technique that provides nanometer spatial resolution, sub-femtosecond temporal resolution, and tens to hundreds of millielectron volt energy resolution. This allows for extremely sensitive observations of plasmonic field oscillations, field dephasing, and hot electrons. This Perspective provides a brief overview of the basic principles and main applications of ultrafast PEEM. The research progress of ultrafast PEEM in plasmonics is highlighted from three points of view: near-field imaging, near-field spectroscopy, and ultrafast dynamics. Future applications of PEEM in plasmonics for the probing of plasmonic hot electron dynamics in the energy and time domains are proposed and discussed.

Highlights

  • Plasmonics is a rapidly developing field of study that is focused on the interaction between an electromagnetic field and free electrons in metals.[1]

  • Ultrafast photoemission electron microscopy (PEEM) is based on multi-photon photoemission, and it has been demonstrated to be a promising alternative for probing the near field of plasmonic nanostructures with a high spatial resolution along the order of 10 nm.[37,38,39]

  • Excitation laser conditions can be adjusted to reveal the near-field spectral properties of plasmonic nanostructures, which is useful in studying the fundamental physics behind the plasmon coupling of complex coupled plasmonics

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Summary

INTRODUCTION

Plasmonics is a rapidly developing field of study that is focused on the interaction between an electromagnetic field and free electrons in metals.[1]. Ultrafast photoemission electron microscopy (PEEM) is based on multi-photon photoemission, and it has been demonstrated to be a promising alternative for probing the near field of plasmonic nanostructures with a high spatial resolution along the order of 10 nm.[37,38,39] This approach is “photon in and electron out,” the inverse of CL. This study explores the application of PEEM to multidimensional plasmonic characterization, including real space, time space, and energy space, with a focus on LSPRs. The PEEM acquisition of near-field images and spectra for the study of plasmonic nanostructures is introduced, while the time-resolved PEEM measurement of ultrafast plasmonic mode dynamics using the interferometric two-pulse correlation technique is further discussed. Several studies have already given a thorough discussion on other plasmonic responses,[56,65] which can be investigated by PEEM

PROBING LSP
Near-field mapping in the spatial domain
Near-field spectral properties
Dynamics and coherent control by time-resolved PEEM
PLASMONIC HOT ELECTRONS AND THEIR DYNAMICS IN THE ENERGY AND TIME DOMAINS
Photoemission electron energy measurement in real-space and reciprocal-space
Plasmon hot electron dynamics in metals
Time-resolved photoemission spectroscopy measurement of hot electrons
CONCLUSION AND OUTLOOK
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