Electromagnetic coupling between plasmonic resonances in metallic nanoparticles allows for engineering of the optical response and generation of strong localized near-fields. Classical electrodynamics fails to describe this coupling across sub-nanometer gaps, where quantum effects become important owing to non-local screening and the spill-out of electrons. However, full quantum simulations are not presently feasible for realistically sized systems. Here we present a novel approach, the quantum-corrected model (QCM), that incorporates quantum-mechanical effects within a classical electrodynamic framework. The QCM approach models the junction between adjacent nanoparticles by means of a local dielectric response that includes electron tunnelling and tunnelling resistivity at the gap and can be integrated within a classical electrodynamical description of large and complex structures. The QCM predicts optical properties in excellent agreement with fully quantum mechanical calculations for small interacting systems, opening a new venue for addressing quantum effects in realistic plasmonic systems.
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http://dx.doi.org/10.1038/ncomms1806 | DOI Listing |
Enhancing local field intensity through light field compression is one of the core issues in surface plasmon-enhanced spectroscopy. The theoretical framework for the nanostructure composed of a tip and a substrate has predominantly relied on classical electromagnetic models, ignoring the electron tunneling effect. In this paper, we investigate the plasmonic near-field characteristics in the sub-nanometer cavity formed by the tip and the substrate using a quantum-corrected model.
View Article and Find Full Text PDFPhys Rev Lett
July 2024
Center for the Fundamental Laws of Nature, Harvard University, Cambridge, Massachusetts 02138, USA.
Recent work has shown that loop corrections from massless particles generate 3/2logT_{Hawking} corrections to black hole entropy which dominate the thermodynamics of cold near-extreme charged black holes. Here we adapt this analysis to near-extreme Kerr black holes. Like AdS_{2}×S^{2}, the near-horizon extreme Kerr (NHEK) metric has a family of normalizable zero modes corresponding to reparametrizations of boundary time.
View Article and Find Full Text PDFNano Lett
June 2023
Institute of Health and Medical Technology, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei 230031, China.
Fabricating ultrasmall nanogaps for significant electromagnetic enhancement is a long-standing goal of surface-enhanced Raman scattering (SERS) research. However, such electromagnetic enhancement is limited by quantum plasmonics as the gap size decreases below the quantum tunneling regime. Here, hexagonal boron nitride (h-BN) is sandwiched as a gap spacer in a nanoparticle-on-mirror (NPoM) structure, effectively blocking electron tunneling.
View Article and Find Full Text PDFACS Nano
December 2022
Physical Chemistry I, Department of Chemistry and Center of Nanointegration Duisburg-Essen (CENIDE), University of Duisburg-Essen, 45141Essen, Germany.
We report on the nanoparticle-size-dependent onset of quantum tunneling of electrons across the subnanometer gaps in three different sizes (30, 50, and 80 nm) of highly uniform gold nanosphere (AuNS) dimers. For precision plasmonics, the gap distance is systematically controlled at the level of single C-C bonds via a series of alkanedithiol linkers (C-C). Parallax-corrected high-resolution transmission electron microscope (HRTEM) imaging and subsequent tomographic reconstruction are employed to resolve the nm to subnm interparticle gap distances in AuNS dimers.
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