Abstract
Spatial confinement of matter in functional nanostructures has propelled these systems to the forefront of nanoscience, both as a playground for exotic physics and quantum phenomena and in multiple applications including plasmonics, optoelectronics, and sensing. In parallel, the emergence of monochromated electron energy loss spectroscopy (EELS) has enabled exploration of local nanoplasmonic functionalities within single nanoparticles and the collective response of nanoparticle assemblies, providing deep insight into associated mechanisms. However, modern synthesis processes for plasmonic nanostructures are often limited in the types of accessible geometry, and materials and are limited to spatial precisions on the order of tens of nm, precluding the direct exploration of critical aspects of the structure-property relationships. Here, the atomic-sized probe of the scanning transmission electron microscope is used to perform precise sculpting and design nanoparticle configurations. Using low-loss EELS, dynamic analyses of the evolution of the plasmonic response are provided. It is shown that within self-assembled systems of nanoparticles, individual nanoparticles can be selectively removed, reshaped, or patterned with nanometer-level resolution, effectively modifying the plasmonic response in both space and energy. This process significantly increases the scope for design possibilities and presents opportunities for unique structure development, which are ultimately the key for nanophotonic design.
| Original language | English |
|---|---|
| Article number | 2105099 |
| Journal | Small |
| Volume | 18 |
| Issue number | 1 |
| DOIs | |
| State | Published - Jan 6 2022 |
Funding
This effort was based upon work supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), Materials Sciences and Engineering Division (K.M.R., S.V.K.). Work was conducted using resources supported by Oak Ridge National Laboratory's Center for Nanophase Materials Sciences (CNMS), which is a U.S. DOE Office of Science User Facility. S.‐H.C and D.J.M. acknowledge (NSF CHE‐1905263, and CDCM, an NSF MRSEC DMR‐1720595), the Welch Foundation (F‐1848), and the Fulbright Program (IIE‐15151071). Electron microscopy was performed using instrumentation within ORNL's Materials Characterization Core provided by UT‐Battelle, LLC, under Contract No. DE‐AC05‐ 00OR22725 with the DOE and sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT‐Battelle, LLC, for the U.S. Department of Energy. The authors would like to thank Jordan Hachtel for his insightful discussions and invaluable advice. This effort was based upon work supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), Materials Sciences and Engineering Division (K.M.R., S.V.K.). Work was conducted using resources supported by Oak Ridge National Laboratory's Center for Nanophase Materials Sciences (CNMS), which is a U.S. DOE Office of Science User Facility. S.-H.C and D.J.M. acknowledge (NSF CHE-1905263, and CDCM, an NSF MRSEC DMR-1720595), the Welch Foundation (F-1848), and the Fulbright Program (IIE-15151071). Electron microscopy was performed using instrumentation within ORNL's Materials Characterization Core provided by UT-Battelle, LLC, under Contract No. DE-AC05- 00OR22725 with the DOE and sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy. The authors would like to thank Jordan Hachtel for his insightful discussions and invaluable advice.