Plasmon-Mediated Chiroptical Second Harmonic Generation from Seemingly Achiral Gold Nanorods

Zehua Li; Lei Kang; Robert W. Lord; Kyoungweon Park; Andrew Gillman; Richard A. Vaia; Raymond E. Schaak; Douglas H. Werner; Kenneth L. Knappenberger

doi:10.1021/acsnanoscienceau.1c00014

Plasmon-Mediated Chiroptical Second Harmonic Generation from Seemingly Achiral Gold Nanorods

Zehua Li, Lei Kang, Robert W. Lord, Kyoungweon Park, Andrew Gillman, Richard A. Vaia, Raymond E. Schaak, Douglas H. Werner, Kenneth L. Knappenberger

Research output: Contribution to journal › Article › peer-review

3 Scopus citations

Abstract

Throughout nature, simple rules explain complex phenomena, such as the selective interaction of chiral objects with circularly polarized light. Here, we demonstrate chiroptical signals from gold nanorods, which are seemingly achiral structures. Shape anisotropy due to atomic-level faceting and rounding at the tips of nanorods, which are free of chiral surface ligands, induces linear-to-circular polarization modulation during second harmonic generation. The intrinsic nanorod chiroptical response is increased by plasmon-resonant excitation, which preferentially amplifies circularly polarized harmonic signals. This structure-plasmon interplay is uniquely resolved by polarization-resolved second harmonic generation measurements. The material's second-order polarizability is the product of the structure-dependent lattice-normal susceptibility and local surface plasmon field vectors. Synthetically scalable plasmon-supporting nanorods that amplify small circular dichroism signals provide a simple, assembly-free platform for chiroptical transduction.

Original language	English (US)
Pages (from-to)	32-39
Number of pages	8
Journal	ACS Nanoscience Au
Volume	2
Issue number	1
DOIs	https://doi.org/10.1021/acsnanoscienceau.1c00014
State	Published - Feb 16 2022

All Science Journal Classification (ASJC) codes

Chemistry (miscellaneous)
Materials Science (miscellaneous)

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10.1021/acsnanoscienceau.1c00014

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title = "Plasmon-Mediated Chiroptical Second Harmonic Generation from Seemingly Achiral Gold Nanorods",

abstract = "Throughout nature, simple rules explain complex phenomena, such as the selective interaction of chiral objects with circularly polarized light. Here, we demonstrate chiroptical signals from gold nanorods, which are seemingly achiral structures. Shape anisotropy due to atomic-level faceting and rounding at the tips of nanorods, which are free of chiral surface ligands, induces linear-to-circular polarization modulation during second harmonic generation. The intrinsic nanorod chiroptical response is increased by plasmon-resonant excitation, which preferentially amplifies circularly polarized harmonic signals. This structure-plasmon interplay is uniquely resolved by polarization-resolved second harmonic generation measurements. The material's second-order polarizability is the product of the structure-dependent lattice-normal susceptibility and local surface plasmon field vectors. Synthetically scalable plasmon-supporting nanorods that amplify small circular dichroism signals provide a simple, assembly-free platform for chiroptical transduction.",

author = "Zehua Li and Lei Kang and Lord, {Robert W.} and Kyoungweon Park and Andrew Gillman and Vaia, {Richard A.} and Schaak, {Raymond E.} and Werner, {Douglas H.} and Knappenberger, {Kenneth L.}",

note = "Funding Information: This research was supported by the Air Force Office of Scientific Research, Grant No. FA-9550-18-1-0347. This work was also supported by National Science Foundation, Award Nos. CHE-1807999 and CHE-1707830. Partial support for this work was also provided by the John L. and Genevieve H. McCain endowed chair professorship at the Pennsylvania State University. Publisher Copyright: {\textcopyright} 2022 by the Author(s).",

year = "2022",

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doi = "10.1021/acsnanoscienceau.1c00014",

language = "English (US)",

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T1 - Plasmon-Mediated Chiroptical Second Harmonic Generation from Seemingly Achiral Gold Nanorods

AU - Li, Zehua

AU - Kang, Lei

AU - Lord, Robert W.

AU - Park, Kyoungweon

AU - Gillman, Andrew

AU - Vaia, Richard A.

AU - Schaak, Raymond E.

AU - Werner, Douglas H.

AU - Knappenberger, Kenneth L.

N1 - Funding Information: This research was supported by the Air Force Office of Scientific Research, Grant No. FA-9550-18-1-0347. This work was also supported by National Science Foundation, Award Nos. CHE-1807999 and CHE-1707830. Partial support for this work was also provided by the John L. and Genevieve H. McCain endowed chair professorship at the Pennsylvania State University. Publisher Copyright: © 2022 by the Author(s).

PY - 2022/2/16

Y1 - 2022/2/16

N2 - Throughout nature, simple rules explain complex phenomena, such as the selective interaction of chiral objects with circularly polarized light. Here, we demonstrate chiroptical signals from gold nanorods, which are seemingly achiral structures. Shape anisotropy due to atomic-level faceting and rounding at the tips of nanorods, which are free of chiral surface ligands, induces linear-to-circular polarization modulation during second harmonic generation. The intrinsic nanorod chiroptical response is increased by plasmon-resonant excitation, which preferentially amplifies circularly polarized harmonic signals. This structure-plasmon interplay is uniquely resolved by polarization-resolved second harmonic generation measurements. The material's second-order polarizability is the product of the structure-dependent lattice-normal susceptibility and local surface plasmon field vectors. Synthetically scalable plasmon-supporting nanorods that amplify small circular dichroism signals provide a simple, assembly-free platform for chiroptical transduction.

AB - Throughout nature, simple rules explain complex phenomena, such as the selective interaction of chiral objects with circularly polarized light. Here, we demonstrate chiroptical signals from gold nanorods, which are seemingly achiral structures. Shape anisotropy due to atomic-level faceting and rounding at the tips of nanorods, which are free of chiral surface ligands, induces linear-to-circular polarization modulation during second harmonic generation. The intrinsic nanorod chiroptical response is increased by plasmon-resonant excitation, which preferentially amplifies circularly polarized harmonic signals. This structure-plasmon interplay is uniquely resolved by polarization-resolved second harmonic generation measurements. The material's second-order polarizability is the product of the structure-dependent lattice-normal susceptibility and local surface plasmon field vectors. Synthetically scalable plasmon-supporting nanorods that amplify small circular dichroism signals provide a simple, assembly-free platform for chiroptical transduction.

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Plasmon-Mediated Chiroptical Second Harmonic Generation from Seemingly Achiral Gold Nanorods

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