- Award ID(s):
- 1953045
- NSF-PAR ID:
- 10340545
- Date Published:
- Journal Name:
- Chemical Science
- Volume:
- 13
- Issue:
- 4
- ISSN:
- 2041-6520
- Page Range / eLocation ID:
- 1037 to 1048
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
Circular dichroism (CD) spectroscopy, which measures the differential absorption of circularly polarized light with opposite handedness, is an important technique to detect and identify chiral molecules in chemistry, biology and life sciences. However, CD signals are normally very small due to the intrinsically weak chirality of molecules. Here we theoretically investigate the generation of chiral hotspots in silicon nanocube dimers for CD enhancement. Up to 15-fold enhancement of the global optical chirality is obtained in the dimer gap, which boosts the CD signal by one order of magnitude without reducing the dissymmetry factor. This chiral hotspot originates from the simultaneous enhancement of magnetic and electric fields and their proper spatial overlap. Our findings could lead to integrated devices for CD spectroscopy, enantioselective sensing, sorting and synthesis.more » « less
-
: Chiral inorganic nanostructures strongly interact with photons changing their polarization state. The resulting circularly polarized light emission (CPLE) has cross-disciplinary importance for a variety of chemical/biological processes and is essential for development of chiral photonics. However, the polarization effects are often complex and could be misinterpreted. CPLE in nanostructured media has multiple origins and several optical effects are typically convoluted into a single output. Analysing CPLE data obtained for nanoclusters, NPs, nanoassemblies, and nanocomposites from metals, chalcogenides, perovskite, and other nanostructures, we show that there are several distinct groups of nanomaterials for which CPLE is dominated either by circularly polarized luminescence (CPL) or circularly polarized scattering (CPS); there are also many nanomaterials for which they are comparable. We also show that (1) CPL and CPS contributions involve light-matter interactions at different structural levels; (2) contribution from CPS is especially strong for nanostructured microparticles, nanoassemblies and composites; and (3) engineering of materials with strongly polarized light emission requires synergistic implementation of CPL and CPS effects. These findings are expected to guide development of CPLE materials in a variety of technological fields, including 3D displays, information storage, biosensors, optical spintronics, and biological probes.more » « less
-
Abstract Circularly polarized light interacts preferentially with the biomolecules to generate spectral fingerprints reflecting their primary and secondary structure in the ultraviolet region of the electromagnetic spectrum. The spectral features can be transferred to the visible and near‐infrared regions by coupling the biomolecules with plasmonic assemblies made of noble metals. Nanoscale gold tetrahelices were used to detect the presence of chiral objects that are 40 times smaller in size by using plane‐polarized light of 550 nm wavelength. The emergence of chiral hotspots in the gaps between 80 nm long tetrahelices differentiate between weakly scattering S‐ vs R‐molecules with optical constants similar to that of organic solvents. Simulations map the spatial distribution of the scattered field to reveal enantiomeric discrimination with selectivity up to 0.54.
-
Abstract The giant circular photo‐galvanic effect is realized in chiral metals when illuminated by circularly polarized light. However, the structure itself is not switchable nor is the crystal chirality in the adjacent chiral domains. Here spindle‐shaped liquid crystalline elastomer microparticles that can switch from prolate to spherical to oblate reversibly upon heating above the nematic to isotropic transition temperature are synthesized. When arranged in a honeycomb lattice, the continuous shape change of the microparticles leads to lattice reconfiguration, from a right‐handed chiral state to an achiral one, then to a left‐handed chiral state, without breaking the translational symmetry. Accordingly, the sign of rotation of the polarized light passing through the lattices changes as measured by time‐domain terahertz spectroscopy. Further, it can locally alter the chirality in the adjacent domains using near‐infrared light illumination. The reconfigurable chiral microarrays will allow us to explore non‐trivial symmetry‐protected transport modes of topological lattices at the light–matter interface. Specifically, the ability to controllably create chiral states at the boundary of the achiral/chiral domains will lead to rich structures emerging from the interplay of symmetry and topology.
-
Abstract Optical activity is the ability of chiral materials to rotate linearly polarized electromagnetic waves. A knotted chiral metamolecule is introduced here that exhibits strong optical activity corresponding to a 90° polarization rotation of the incident waves. More importantly, the torus knot structure is intrinsically chiral and multifold axisymmetric. Consequently, the observed polarization rotation behavior is found to be independent of how the incident wave is polarized. The metamolecule is fabricated through selective laser melting and experimentally validated in the microwave spectrum. This work represents the first ever metamolecule to be reported that is intrinsically axisymmetric and capable of simultaneously exhibiting strong optical activity.