期刊
ACS NANO
卷 12, 期 6, 页码 5445-5451出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.8b00601
关键词
chirality; second-harmonic generation; optical rotation
类别
资金
- Royal Society [CHG\R1\170067, PEF1\170015, RGF\EA\180228]
- STFC Grant [ST/R005842/1]
- EPSRC Centre for Doctoral Training Grant, EPSRC Centre for Doctoral Training in Condensed Matter Physics (CDT-CMP) [EP/L015544/1]
- STFC [ST/R005842/1] Funding Source: UKRI
Chiral plasmonic nanostructures, those lacking mirror symmetry, can be designed to manipulate the polarization of incident light resulting in chiroptical (chiral optical) effects such as circular dichroism (CD) and optical rotation (OR). Due to high symmetry sensitivity, corresponding effects in second-harmonic generation (SHG-CD and SHG-OR) are typically much stronger in comparison. These nonlinear effects have long been used for chiral molecular analysis and characterization; however both linear and nonlinear optical rotation can occur even in achiral structures, if the structure is birefringent due to anisotropy. Crucially, chiroptical effects resulting from anisotropy typically exhibit a strong dependence on structural orientation. Here we report a large second-harmonic generation optical rotation of +/- 45 degrees, due to intrinsic chirality in a highly anisotropic helical metamaterial. The SHG intensity is found to strongly relate to the structural anisotropy; however, the angle of SHG-OR is invariant under sample rotation. We show that by tuning the geometry of anisotropic nanostructures, the interaction between anisotropy, chirality, and experimental geometry can allow even greater control over the chiroptical properties of plasmonic metamaterials.
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