An official website of the United States government
Abstract Designing broadband enhanced chirality is of strong interest to the emerging fields of chiral chemistry and sensing, or to control the spin orbital momentum of photons in recently introduced nanophotonic chiral quantum and classical optical applications. However, chiral light‐matter interactions have an extremely weak nature, are difficult to control and enhance, and cannot be made tunable or broadband. In addition, planar ultrathin nanophotonic structures to achieve strong, broadband, and tunable chirality at the technologically important visible to ultraviolet spectrum still remain elusive. Here, these important problems are tackled by experimentally demonstrating and theoretically verifying spectrally tunable, extremely large, and broadband chiroptical response by nanohelical metamaterials. The reported new designs of all‐dielectric and dielectric‐metallic (hybrid) plasmonic metamaterials permit the largest and broadest ever measured chiral Kuhn's dissymmetry factor achieved by a large‐scale nanophotonic structure. In addition, the strong circular dichroism of the presented bottom‐up fabricated optical metamaterials can be tuned by varying their dimensions and proportions between their dielectric and plasmonic helical subsections. The currently demonstrated ultrathin optical metamaterials are expected to provide a substantial boost to the developing field of chiroptics leading to significantly enhanced and broadband chiral light‐matter interactions at the nanoscale.
more »
« less
This content will become publicly available on February 13, 2026
Chiral Gold Nanoprisms by Tuning the Wavelength and Handedness of Light
Plasmonic nanoparticles with chiral resonances in the visible wavelengths complement optical dissymmetry in the ultraviolet and near-infrared wavelengths in natural products and metamaterials respectively. Here, we show that under oxidative conditions, hot holes photogenerated with circularly polarized light in gold nanoprisms can spatially direct the photodeposition of lead oxide (PbO2), resulting in chiral nanostructures tunable with the polarization and wavelength of light. We observe a g-factor of 3.6 × 10–3, which can be attributed to the enhanced optical dissymmetry with PbO2 deposition of the side of nanoprisms upon illumination with green 532 nm light. Our finite-difference time-domain calculations support the site-specific photodeposition of PbO2 onto nanoprisms. This work shows that plasmonic nanoparticles can have tunable chiral properties imbued as a function of the wavelength and polarization of light.
more »
« less
- PAR ID:
- 10628127
- Publisher / Repository:
- American Chemical Society
- Date Published:
- Journal Name:
- The Journal of Physical Chemistry C
- Volume:
- 129
- Issue:
- 6
- ISSN:
- 1932-7447
- Page Range / eLocation ID:
- 3352 to 3358
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
null (Ed.)Plasmonic chiral metamaterials have attracted broad research interest because of their potential applications in optical communication, biomedical diagnosis, polarization imaging, and circular dichroism spectroscopy. However, optical losses in plasmonic structures severely limit practical applications. Here, we present the design concept and experimental demonstration for highly efficient subwavelength-thick plasmonic chiral metamaterials with strong chirality. The proposed designs utilize plasmonic metasurfaces to control the phase and polarization of light and exploit anisotropic thin-film interference effects to enhance optical chirality while minimizing optical loss. Based on such design concepts, we demonstrated experimentally optical devices such as circular polarization filters with transmission efficiency up to 90% and extinction ratio >180, polarization converters with conversion efficiency up to 90%, as well as on-chip integrated microfilter arrays for full Stokes polarization detection with high accuracy over a broad wavelength range (3.5–5 μm). The proposed design concepts are applicable from near-infrared to Terahertz regions via structural engineering.more » « less
-
null (Ed.)Plasmonic chiral metamaterials have attracted broad research interest because of their potential applications in optical communication, biomedical diagnosis, polarization imaging, and circular dichroism spectroscopy. However, optical losses in plasmonic structures severely limit practical applications. Here, we present the design concept and experimental demonstration for highly efficient subwavelength-thick plasmonic chiral metamaterials with strong chirality. The proposed designs utilize plasmonic metasurfaces to control the phase and polarization of light and exploit anisotropic thin-film interference effects to enhance optical chirality while minimizing optical loss. Based on such design concepts, we demonstrated experimentally optical devices such as circular polarization filters with transmission efficiency up to 90% and extinction ratio >180, polarization converters with conversion efficiency up to 90%, as well as on-chip integrated microfilter arrays for full Stokes polarization detection with high accuracy over a broad wavelength range (3.5–5 μm). The proposed design concepts are applicable from near-infrared to Terahertz regions via structural engineering.more » « less
-
Chiral plasmonic surfaces with 3D “forests” from nanohelicoids should provide strong optical rotation due to alignment of helical axis with propagation vector of photons. However, such three-dimensional nanostructures also demand multi-step nanofabrication, which is incompatible with many substrates. Large-scale photonic patterns on polymeric and flexible substrates remain unattainable. Here, we demonstrate the substrate-tolerant direct-write printing and patterning of silver nanohelicoids with out-of-plane 3D orientation using circularly polarized light. Centimeter-scale chiral plasmonic surfaces can be produced within minutes using inexpensive medium-power lasers. The growth of nanohelicoids is driven by the symmetry-broken site-selective deposition and self-assembly of the silver nanoparticles (NPs). The ellipticity and wavelength of the incident photons control the local handedness and size of the printed nanohelicoids, which enables on-the-fly modulation of nanohelicoid chirality during direct writing and simple pathways to complex multifunctional metasurfaces. Processing simplicity, high polarization rotation, and fine spatial resolution of the light-driven printing of stand-up helicoids provide a rapid pathway to chiral plasmonic surfaces, accelerating the development of chiral photonics for health and information technologies.more » « less
-
Modern integrated circuits have active components on the order of nanometers. However, optical devices are often limited by diffraction effects with dimensions measured in wavelengths. Nanoscale photodetectors capable of converting light into electrical signals are necessary for the miniaturization of optoelectronic applications. Strong coupling of light and free electrons in plasmonic nanostructures overcomes these limitations by confining light into sub-wavelength volumes with intense local electric fields. Localized electric fields are intensified at nanorod ends and in nanogap regions between nanostructures. Hot carriers generated within these high-field regions from nonradiative decay of surface plasmons can be injected into the conduction band of adjacent semiconductors, enabling sub-bandgap photodetection. The optical properties of these plasmonic photodetectors can be tuned by modifying antenna materials and geometric parameters like size, thickness, and shape. Electrical interconnects provide connectivity to convert light into electrical signals. In this work, interconnected nanogap antennas fabricated with 35 nm gaps are encapsulated with ALD-deposited [Formula: see text], enabling photodetection via Schottky barrier junctions. Photodetectors with high responsivity (12[Formula: see text][Formula: see text]A/mW) are presented for wavelengths below the bandgap of [Formula: see text] (3.2[Formula: see text]eV). These plasmonic nanogap antennas are sub-wavelength, tunable photodetectors with sub-bandgap responsivity for a broad spectral range.more » « less
