Micro, Nano, and Molecular Systems Article 2019

First Observation of Optical Activity in Hyper-Rayleigh Scattering

Hyperrayleigh

Chiral nano- or metamaterials and surfaces enable striking photonic properties, such as negative refractive index and superchiral light, driving promising applications in novel optical components, nanorobotics, and enhanced chiral molecular interactions with light. In characterizing chirality, although nonlinear chiroptical techniques are typically much more sensitive than their linear optical counterparts, separating true chirality from anisotropy is a major challenge. Here, we report the first observation of optical activity in second-harmonic hyper-Rayleigh scattering (HRS). We demonstrate the effect in a 3D isotropic suspension of Ag nanohelices in water. The effect is 5 orders of magnitude stronger than linear optical activity and is well pronounced above the multiphoton luminescence background. Because of its sensitivity, isotropic environment, and straightforward experimental geometry, HRS optical activity constitutes a fundamental experimental breakthrough in chiral photonics for media including nanomaterials, metamaterials, and chemical molecules.

Author(s): Collins, J. T. and Rusimova, K. R. and Hooper, D. C. and Jeong, H. H. and Ohnoutek, L. and Pradaux-Caggiano, F. and Verbiest, T. and Carbery, D. R. and Fischer, P. and Valev, V. K.
Journal: Phys. Rev. X
Volume: 9
Number (issue): 011024
Year: 2019
Month: January
Day: 6
Bibtex Type: Article (article)
DOI: https://doi.org/10.1103/PhysRevX.9.011024
URL: https://journals.aps.org/prx/abstract/10.1103/PhysRevX.9.011024
Electronic Archiving: grant_archive

BibTex

@article{2019Collins,
  title = {First Observation of Optical Activity in Hyper-Rayleigh Scattering},
  journal = {Phys. Rev. X},
  abstract = {Chiral nano- or metamaterials and surfaces enable striking photonic properties, such as negative refractive index and superchiral light, driving promising applications in novel optical components, nanorobotics, and enhanced chiral molecular interactions with light. In characterizing chirality, although nonlinear chiroptical techniques are typically much more sensitive than their linear optical counterparts, separating true chirality from anisotropy is a major challenge. Here, we report the first observation of optical activity in second-harmonic hyper-Rayleigh scattering (HRS). We demonstrate the effect in a 3D isotropic suspension of Ag nanohelices in water. The effect is 5 orders of magnitude stronger than linear optical activity and is well pronounced above the multiphoton luminescence background. Because of its sensitivity, isotropic environment, and straightforward experimental geometry, HRS optical activity constitutes a fundamental experimental breakthrough in chiral photonics for media including nanomaterials, metamaterials, and chemical molecules.},
  volume = {9},
  number = {011024},
  month = jan,
  year = {2019},
  slug = {2019collins},
  author = {Collins, J. T. and Rusimova, K. R. and Hooper, D. C. and Jeong, H. H. and Ohnoutek, L. and Pradaux-Caggiano, F. and Verbiest, T. and Carbery, D. R. and Fischer, P. and Valev, V. K.},
  url = {https://journals.aps.org/prx/abstract/10.1103/PhysRevX.9.011024},
  month_numeric = {1}
}