Enantioselective sensing by collective circular dichroism

Ryeong Myeong Kim, Ji-Hyeok Huh, SeokJae Yoo, Tae Gyun Kim, Changwon Kim, Hyeohn Kim, Jeong Hyun Han, Nam Heon Cho, Yae-Chan Lim, Sang Won Im, EunJi Im, Jae Ryeol Jeong, Min Hyung Lee, Tae-Young Yoon, Ho-Young Lee, Q-Han Park (), Seungwoo Lee () and Ki Tae Nam ()
Additional contact information
Ryeong Myeong Kim: Seoul National University
Ji-Hyeok Huh: Korea University
SeokJae Yoo: Inha University
Tae Gyun Kim: Seoul National University
Changwon Kim: Seoul National University
Hyeohn Kim: Seoul National University
Jeong Hyun Han: Seoul National University
Nam Heon Cho: Seoul National University
Yae-Chan Lim: Seoul National University
Sang Won Im: Seoul National University
EunJi Im: Korea University
Jae Ryeol Jeong: Kyung Hee University
Min Hyung Lee: Kyung Hee University
Tae-Young Yoon: Seoul National University
Ho-Young Lee: Seoul National University Bundang Hospital
Q-Han Park: Korea University
Seungwoo Lee: Korea University
Ki Tae Nam: Seoul National University

Nature, 2022, vol. 612, issue 7940, 470-476

Abstract: Abstract Quantitative determination and in situ monitoring of molecular chirality at extremely low concentrations is still challenging with simple optics because of the molecular-scale mismatch with the incident light wavelength. Advances in spectroscopy1–4 and nanophotonics have successfully lowered the detection limit in enantioselective sensing, as it can bring the microscopic chiral characteristics of molecules into the macroscopic scale5–7 or squeeze the chiral light into the subwavelength scale8–17. Conventional nanophotonic approaches depend mainly on the optical helicity density8,9 by localized resonances within an individual structure, such as localized surface plasmon resonances (LSPRs)10–16 or dielectric Mie resonances17. These approaches use the local chiral hotspots in the immediate vicinity of the structure, whereas the handedness of these hotspots varies spatially. As such, these localized resonance modes tend to be error-prone to the stochasticity of the target molecular orientations, vibrations and local concentrations18,19. Here we identified enantioselective characteristics of collective resonances (CRs)20 arising from assembled 2D crystals of isotropic, 432-symmetric chiral gold nanoparticles (helicoids)21,22. The CRs exhibit a strong and uniform chiral near field over a large volume above the 2D crystal plane, resulting from the collectively spinning, optically induced dipoles at each helicoid. Thus, energy redistribution by molecular back action on the chiral near field shifts the CRs in opposite directions, depending on the handedness of the analyte, maximizing the modulation of the collective circular dichroism (CD).

Date: 2022
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DOI: 10.1038/s41586-022-05353-1

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