Journal
NANO LETTERS
Volume 20, Issue 8, Pages 5792-5798Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.0c01659
Keywords
chirality; nanophotonics; hyper-Rayleigh scattering; optical activity; spectroscopy; plasmonics
Categories
Funding
- Royal Society [PEF1\170015, RGF\EA\180228]
- STFC [ST/R005842/1]
- EPSRC [EP/L015544/1]
- Creative Materials Discovery Program through the National Research Foundation of Korea (NRF) - Ministry of Science and ICT [NRF-2017M3D1A1039377]
- National Research Foundation of Korea (NRF) - Korea government (MSIT) [NRF-2017R1A2B3012003]
- EPSRC through grant EPSRC DTP [EBBB1250]
- STFC [ST/R005842/1] Funding Source: UKRI
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Linear optical methods of determining the chirality of organic and inorganic materials have relied on weak chiral optical (chiroptical) effects. Nonlinear chiroptical characterization holds the potential of much greater sensitivity and smaller interaction volumes. However, suitable materials on which to perform measurements have been lacking for decades. Here, we present the first nonlinear chiroptical characterization of crystallographic chirality in gold helicoids (approximate to 150 nm size) and core/shell helicoids with the newly discovered hyper-Rayleigh scattering optical activity (HRS OA) technique. The observed chiroptical signal is, on average, originating from between approximate to 0.05 and approximate to 0.13 helicoids, i.e., less than a single nanoparticle. The measured HRS OA ellipticities reach approximate to 3 degrees, for a concentration approximate to 10(9) times smaller than that of chiral molecules with similar nonlinear chiroptical response. These huge values indicate that the helicoids are excellent candidates for future nonlinear chiroptical materials and applications.
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