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The hybridization of plasmonic energy and charge donors with polymeric acceptors is a possible means to overcome fast internal relaxation that limits potential photocatalytic applications for plasmonic nanomaterials. Polyaniline (PANI) readily hybridizes onto gold nanorods (AuNRs) and has been used for the sensitive monitoring of local refractive index changes. Here, we use single-particle spectroscopy to quantify a previously unreported plasmon damping mechanism in AuNR–PANI hybrids while actively tuning the PANI chemical structure. By eliminating contributions from heterogeneous line width broadening and refractive index changes, we identify efficient resonance energy transfer (RET) between AuNRs and PANI. We find that RET dominates the optical response in our AuNR–PANI hybrids during the dynamic tuning of the spectral overlap of the AuNR donor and PANI acceptor. Harnessing RET between plasmonic nanomaterials and an affordable and processable polymer such as PANI offers an alternate mechanism toward efficient photocatalysis with plasmonic nanoparticle antennas. This document is the Accepted Manuscript version of a Published Work that appeared in final form in The Journal of Physical Chemistry Letters, copyright © The American Chemical Society 2023 after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acs.jpclett.3c01990 

Abstract Plasmonic nanoparticles that can be manipulated with magnetic fields are of interest for advanced optical applications, diagnostics, imaging, and therapy. Alignment of gold nanorods yields strong polarization‐dependent extinction, and use of magnetic fields is appealing because they act through space and can be quickly switched. In this work, cationic polyethyleneimine‐functionalized superparamagnetic Fe₃O₄nanoparticles (NPs) are deposited on the surface of anionic gold nanorods coated with bovine serum albumin. The magnetic gold nanorods (MagGNRs) obtained through mixing maintain the distinct optical properties of plasmonic gold nanorods that are minimally perturbed by the magnetic overcoating. Magnetic alignment of the MagGNRs arising from magnetic dipolar interactions on the anisotropic gold nanorod core is comprehensively characterized, including structural characterization and enhancement (suppression) of the longitudinal surface plasmon resonance and suppression (enhancement) of the transverse surface plasmon resonance for light polarized parallel (orthogonal) to the magnetic field. The MagGNRs can also be driven in rotating magnetic fields to rotate at frequencies of at least 17 Hz. For suitably large gold nanorods (148 nm long) and Fe₃O₄NPs (13.4 nm diameter), significant alignment is possible even in modest (<500 Oe) magnetic fields. An analytical model provides a unified understanding of the magnetic alignment of MagGNRs.