Abstract
Abstract Recent developments in the application of plasmonic nanoparticles have showcased the importance of understanding in detail their plasmonic resonances at the single-particle level. These resonances can be excited and probed through various methods, which can be grouped in four categories, depending on whether excitation and detection involve electrons (electron energy loss spectroscopy), photons (e.g., dark-field microscopy), or both (cathodoluminescence and photon-induced near-field electron microscopy). While both photon-based and electron-based methods have made great strides toward deepening our understanding of known plasmonic properties and discovering new ones, they have in general progressed in parallel, without much cross-pollination. This evolution can be primarily attributed to the different theoretical approaches driving these techniques, mainly dictated by the inherent different nature of electrons and photons. The discrepancies that still exist among them have hampered the development of a holistic approach to the characterization of plasmonic materials. In this review therefore, we aim to briefly present those electron-based and photon-based methods fundamental to the study of plasmonic properties at the single-particle level, with an eye to new behaviors involving multipolar, propagating, and bulk modes coexisting in colloidal nanostructures. By exploring the key fundamental discoveries in nanoparticle plasmonics achieved with these techniques, herein we assess how integrating this information could encourage the creation of a unified understanding of the various phenomena occurring in individual nanoparticles, which would benefit the plasmonics and electron microscopy communities alike.
Highlights
In this short review, we critically present and analyze key advances in electron-based [1, 2] and photon-based [3,4,5] techniques for the study of plasmonic phenomena in individual nanoparticles, with the overarching goal to encourage cross-talk between the plasmonics and electron microscopy communities, which, it is safe to say, has been rather limited so far
Driven by our extensive work on gold nanostars with high shape anisotropy [6,7,8,9], and motivated by the numerous fundamental questions that have arisen during these studies, we focus here on recapitulating the most cuttingedge investigative tools available for single-particle plasmonics, classifying them in two main classes: on one side
We report on cutting-edge plasmonic mode mapping work carried out by two different groups of scientists using two different exciting and probing with electrons (EELS) approaches
Summary
We critically present and analyze key advances in electron-based [1, 2] and photon-based [3,4,5] techniques for the study of plasmonic phenomena in individual nanoparticles, with the overarching goal to encourage cross-talk between the plasmonics and electron microscopy communities, which, it is safe to say, has been rather limited so far. Tsoulos et al.: Multipolar and bulk modes those that allow the study of the local nature of surfacelocalized and bulk plasmon resonances (electron-based methods) [9], and on the other side the ones that reveal the collective nature of plasmonic resonances (photon-based methods) In this critical review, we bring together a decades-long progress in both classes, focusing on the most important results achieved with each technique and comparatively assessing the benefits and drawbacks of each of them. We suggest that, with the recent developments in both instrumentation and synthesis, the time might be right to propose a unifying picture for single-particle plasmonics, that takes into account both electrons and photons, and can be backed up by solid theory While they might have not been until recently, our plasmonics and electron microscopy communities are equipped with the analytical, computational, and theoretical tools to achieve it
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