Chiral Plasmonic Research Articles

Rotation-Induced Plasmonic Chiral Quasi-Bound States in the Continuum

Rotation-Induced Plasmonic Chiral Quasi-Bound States in the Continuum

Phonon-Induced Geometric Chirality.

Chiral properties have seen increasing use in recent years, leading to the emerging fields of chiral quantum optics, plasmonics, and phononics. While these fields have achieved manipulation of the chirality of light and lattice vibrations, controlling the chirality of materials on demand has yet remained elusive. Here, we demonstrate that linearly polarized phonons can be used to induce geometric chirality in achiral crystals when excited with an ultrashort laser pulse. We show that nonlinear phonon coupling quasistatically displaces the crystal structure along phonon modes that reduce the symmetry of the lattice to that of a chiral point group corresponding to a chiral crystal. By reorienting the polarization of the laser pulse, the two enantiomers can be induced selectively. Therefore, geometric chiral phonons enable the light-induced creation of chiral crystal structures and therefore the engineering of chiral electronic states and optical properties.

Selective and Tunable Absorption of Twisted Light in Achiral and Chiral Plasmonic Metasurfaces.

The symmetry of achiral metasurfaces suggests selective absorption is nonexistent when irradiated either by circularly polarized Gaussian or twisted light beams carrying orbital angular momentum (OAM). In chiral metasurfaces, the lack of symmetry leads to differential absorption when probed with chiral light either in the form of circular polarization (circular dichroism) or helical phase fronts (helical dichroism). Here, we demonstrate differential absorption of asymmetric twisted light beams, known as helical dichroism, which exist in an array and a single achiral structure and can be controlled. When extended to chiral structures, these asymmetrical chiral light modes enable to enhance and tune chiroptical sensitivity. Our technique offers more control parameters than just changing the OAM value, as presented in previous studies. Selective response to asymmetric helical light beams is qualitatively explained in terms of induced multipole moments. The presence of dichroism in achiral nanostructures offers a significant fabrication advantage over complex chiral structures and enables the development of next-generation plasmonic-based chiroptical spectroscopy and molecular sensing.

Spatiotemporally modulated full-polarized light emission for multiplexed optical encryption

Spatiotemporal control of full freedoms of polarized light emission is crucial in multiplexed optical computing, encryption and communication. Although recent advancements have been made in active emission or passive conversion of polarized light through solution-processed nanomaterials or metasurfaces, these design paths usually encounter limitations, such as small polarization degrees, low light utilization efficiency, limited polarization states, and lack of spatiotemporal control. Here, we addressed these challenges by integrating the spatiotemporal modulation of the LED device, the precise control and efficient polarization emission through nanomaterial assembly, and the programmable patterning/positioning using 3D printing. We achieved an extremely high degree of polarization for both linearly and circularly polarized emission from ultrathin inorganic nanowires and quantum nanorods thanks to the shear-force-induced alignment effect during the protruding of printing filaments. Real-time polarization modulation covering the entire Poincaré sphere can be conveniently obtained through the programming of the on-off state of each LED pixel. Further, the output polarization states can be encoded by an ordered chiral plasmonic film. Our device provides an excellent platform for multiplexing spatiotemporal polarization information, enabling visible light communication with an exceptionally elevated level of physical layer security and multifunctional encrypted displays that can encode both 2D and 3D information.

Unveiling the Loss Mode Enabled Tunable Plasmonic Chirality at Flat Metal Surface.

Plasmonic chirality has garnered significant interest in the past decade due to its enhanced chiral light-matter interactions. Current methods for achieving plasmonic chirality often rely on complex nanostructures or metamaterials, which are hampered by intricate fabrication processes. In this work, we present an approach to generate plasmonic chiral structured surface plasmon polariton (s-SPP) fields on a single, flat metal surface, bypassing elaborate fabrication techniques. The plasmonic chiral s-SPP fields are excited by the superposition of multiple differently oriented transverse magnetic polarized plane waves. We demonstrate, both theoretically and experimentally, the flexible tuning of chiral plasmonic patterns by adjusting the symmetry and phase differences of the incident waves. This method provides a facile mean to optically tailor plasmonic chiral properties on a subwavelength scale, offering potential applications in sensing, enantioselective reactions, imaging, and reconfigurable chiral switches.

Dispersion Properties in Uniaxial Chiral–Graphene–Uniaxial Chiral Plasmonic Waveguides

Dispersion Properties in Uniaxial Chiral–Graphene–Uniaxial Chiral Plasmonic Waveguides

Position-dependent plasmonic chirality of particles in tightly focused light field

Position-dependent plasmonic chirality of particles in tightly focused light field

Precise Construction of Chiral Plasmonic Nanoparticles for Enantioselective Discrimination.

Chiral plasmonic nanostructures exhibit potential in the advanced manufacturing industry, due to their fascinating characteristics. However, the limitation of existing fabrication methods as difficulty to precisely manipulate chiral nanostructures at the nanoscale restricts their application and optimization of performance. In this work, we report a simple and robust route for the precise construction of chiral Au nanoparticles (NPs), employing star-like block copolymers with well-defined structures as chiral templates. The globular unimolecular micelles as nanoreactors enabled control over the size, shape, and chirality of in situ grown nanocrystals. Utilizing the chiral anisotropy property of surface-enhanced Raman scattering (SERS), the enantioselective discrimination on various substrates was accomplished with an enhancement factor over 9.3 × 106. NPs with a smaller size exhibited strengthened Raman enhancement and chiral recognition. Furthermore, these chiral unimolecular-micelle-based templates with high efficiency and strong controllability could pave the way for tailor-made chiral nanomaterials.

Strong coupling of an epsilon-near-zero mode to a chiral plasmon.

The reconfigurable chiroptical effect is highly desirable for spin photonics, chiral spectroscopy, and photocatalysis due to its merits for dynamic and broadband applications. The coupling of an epsilon-near-zero (ENZ) mode to a chiral plasmon is expected to enable active and effective manipulation of the chiroptical effect but remains unexplored. Here we, for the first time to our knowledge, propose and demonstrate the strong coupling of an ENZ mode to a chiral plasmon by using a hybrid system composed of two identical vertically placed gold nanorods and an in-between ENZ film. An analytical three-oscillator model combined with numerical simulations is established to study the coupling mechanism, which predicts a Rabi splitting up to 240 meV with an ENZ film thickness of 60 nm in circular dichroism.

Cholesteric Liquid Crystal‐Mediated Chiral Plasmonic Films with Strong Chiroptical Response, Dynamic Tunability, and Reversible Thermal Reconfigurability

AbstractChiral assemblies of plasmonic nanocrystals (NCs) are of immense interest due to their distinctive physicochemical characteristics and promising potential in future optoelectronic applications. Despite recent advances in the construction of chiral NC assemblies, most approaches have led to the formation of static irreversible structures with modest optical responses and limited configurational tunability. Herein, a way to prepare a thermally reconfigurable helical assembly of Au nanorods (AuNRs) with a strong chiroptical response is introduced by employing cholesteric liquid crystals (CLCs) as a chiral template. Circular dichroism (CD) spectroscopy and polarized optical microscopy are used to verify the strong chiroptical activity and dynamic optical tunability of chiral plasmonic film of AuNR–CLC composites and to unveil the interactions between constituents. For the system, chiral dopants are employed to induce strong helical procession along the hierarchical structure of the CLC template, resulting in a strong CD response, which can further be enhanced by increasing the amount of AuNRs. Furthermore, the thermotropic nature of the CLC template leads to the reversible on/off switching of the chiroptical responses of the system at a moderate temperature window with almost complete recovery of the original response, suggesting its feasibility as a promising material for chiral optoelectronic devices.

Breaking the mirror symmetry of photonic spin-orbit interaction using a geometrically symmetric chiral resonator

The symmetries of photonic spin-orbit interaction (PSOI) at waveguide interfaces provide flexible modulation capability but limit their practical implementation due to the stringent requirements of excitation conditions. This limitation can be mitigated by intentionally breaking local symmetries, offering a novel platform for achieving directional coupling and optical isolation with PSOI-based interfaces. For example, breaking the inversion symmetry of a nanofiber PSOI interface using a nanosphere scatterer reduces the required accuracy in the size and position of excitation spots. This study introduces a novel approach to break the mirror symmetry of a PSOI-based nanofiber waveguide by coupling it with a geometrically symmetric chiral gold nanohelicoid (GNH) resonator, which relaxes the original requirement of circularly polarized excitations. Finite-difference time-domain simulations demonstrate unidirectional light coupling and propagation under both circularly and linearly polarized excitations, showcasing the versatility of this hybrid symmetry-broken system. The Fano-like features observed in directionality spectra align with the GNH’s circular dichroism spectrum, emphasizing an intricate correlation between plasmonic near-field chirality and far-field scattering dichroism. This work paves the way for enhancing the functionalities of PSOI-based waveguide interfaces through locally coupling them with nanoscale chiral resonators, thereby expanding their application in quantum photonics, information transport and plasmonic nanophotonics.

Inversing Plasmonic Chirality through Locally Turning Building Blocks in a Trident-Shaped Nanostructure Array

Inversing Plasmonic Chirality through Locally Turning Building Blocks in a Trident-Shaped Nanostructure Array

The Mechanism of Manipulating Chirality and Chiral Sensing Based on Chiral Plexcitons in a Strong-Coupling Regime.

Manipulating plasmonic chirality has shown promising applications in nanophotonics, stereochemistry, chirality sensing, and biomedicine. However, to reconfigure plasmonic chirality, the strategy of constructing chiral plasmonic systems with a tunable morphology is cumbersome and complicated to apply for integrated devices. Here, we present a simple and effective method that can also manipulate chirality and control chiral light-matter interactions only via strong coupling between chiral plasmonic nanoparticles and excitons. This paper presents a chiral plexcitonic system consisting of L-shaped nanorod dimers and achiral molecule excitons. The circular dichroism (CD) spectra in our strong-coupling system can be calculated by finite element method simulations. We found that the formation of the chiral plexcitons can significantly modulate the CD spectra, including the appearance of new hybridized peaks, double Rabi splitting, and bisignate anti-crossing behaviors. This phenomenon can be explained by our extended coupled-mode theory. Moreover, we explored the applications of this method in enantiomer ratio sensing by using the properties of the CD spectra. We found a strong linear dependence of the CD spectra on the enantiomer ratio. Our work provides a facile and efficient method to modulate the chirality of nanosystems, deepens our understanding of chiral plexcitons in nanosystems, and facilitates the development of chiral devices and chiral sensing.

Single-Particle Photothermal Circular Dichroism and Photothermal Magnetic Circular Dichroism Microscopy.

Recent advances in single-particle photothermal circular dichroism (PT CD) and photothermal magnetic circular dichroism (PT MCD) microscopy have shown strong promise for diverse applications in chirality and magnetism. Photothermal circular dichroism microscopy measures direct differential absorption of left- and right-circularly polarized light by a chiral nanoobject and thus can measure a pure circular dichroism signal, which is free from the contribution of circular birefringence and linear dichroism. Photothermal magnetic circular dichroism, which is based on the polar magneto-optical Kerr effect, can probe the magnetic properties of a single nanoparticle (of sizes down to 20 nm) optically. Single-particle measurements enable studies of the spatiotemporal heterogeneity of magnetism at the nanoscale. Both PT CD and PT MCD have already found applications in chiral plasmonics and magnetic nanomaterials. Most importantly, the advent of these microscopic techniques opens possibilities for many novel applications in biology and nanomaterial science.

Photosensitization of TiO2 electrodes immobilized with chiral plasmonic Au nanocolloids by circularly polarized light irradiation.

Photosensitization of semiconductors by excitation of chiral plasmonic metallic nanostructures has attracted much attention, not only for the analysis and detection of circularly polarized light but also for its potential applications in chiral photosynthesis. Although there have been reports on the detection of semiconductor-sensitized current in chiral nanostructures precisely fabricated by physical vapor deposition and/or lithography techniques, there have been no studies using plasmonic metal nanocolloids synthesized by chemical processes. In this study, we report the establishment of a fabrication method for large-area chiral photoelectrodes and the semiconductor photosensitization phenomenon realized using chiral plasmonic nanoparticles. Chiral plasmonic Au nanoparticles prepared by previously reported colloidal methods were immobilized onto a TiO2 thin film electrode by electrophoresis. When TiO2 electrodes loaded with chiral Au nanoparticles synthesized using L-cysteine were irradiated with circularly polarized light, left circularly polarized light irradiation at a wavelength of 500-600nm generated a larger anodic photocurrent than right circularly polarized light irradiation at the same wavelength. This trend was reversed for TiO2 electrodes immobilized with colloidal Au nanoparticles synthesized with D-cysteine. From these results, we conclude that the efficiency of photocurrent generation by chiral plasmon excitation can be controlled by the polarization direction of the incident light.

Theoretical Study of Strong Coupling between Molecular Shells and Chiral Plasmons of Gold Nanoparticles Helices.

Chiral plasmonic nanostructures can produce strong chiral optical responses and have potential applications in photonics. Experimentally, metallic nanoparticle helices have been synthesized to achieve strong chiral responses. Strong coupling effects between the quantum emitters and the plasmon have attracted significant attention in the past decade and have been recently extended to the chiral plasmon of nanostructures. However, the strong coupling between molecules and metallic nanosphere helices has not been reported yet. In this article we study theoretically such an effect and examine the modulation of chiral and coupling effects by illumination light and molecular layer thickness. Our study may guide further experimental studies.

Creating chirality in the nearly two dimensions.

Structural chirality, defined as the lack of mirror symmetry in materials' atomic structure, is only meaningful in three-dimensional space. Yet two-dimensional (2D) materials, despite their small thickness, can show chirality that enables prominent asymmetric optical, electrical and magnetic properties. In this Perspective, we first discuss the possible definition and mathematical description of '2D chiral materials', and the intriguing physics enabled by structural chirality in van der Waals 2D homobilayers and heterostructures, such as circular dichroism, chiral plasmons and the nonlinear Hall effect. We then summarize the recent experimental progress and approaches to induce and control structural chirality in 2D materials from monolayers to superlattices. Finally, we postulate a few unique opportunities offered by 2D chiral materials, the synthesis and new properties of which can potentially lead to chiral optoelectronic devices and possibly materials for enantioselective photochemistry.

On chip all-optical distinguishing of independently placed distinct types of single Rayleigh particle

In order to determine whether a particle is plasmonic, dielectric, or chiral, different complex processes and chemicals are applied in lab setups and pharmaceutical industries. Sorting or categorizing a particle based on distinct optical forces can be a novel technique. When a beam of light interacts with a particle, it usually pushes the particle in the direction of the light's propagation. Counterintuitively, it can also pull the particle toward the light beam or move it toward a lateral direction. As far as we know, to date, no comprehensive report exists regarding a single optical arrangement capable of inducing entirely distinct behaviors of force for three disparate types of independently placed single Rayleigh particle. This study introduces an all-optical technique aimed at effectively sorting nanoscale Rayleigh-sized objects employing a plasmonic substrate, when each distinct type of single particle is placed over the substrate independently. Unfortunately, this proposed technique does not work for the cluster or mixture of distinct particles. In our proposed configuration, a simple linearly polarized plane wave is incident onto the plasmonic substrate, thereby engendering completely different responses from three different types of nanoparticles: Gold (plasmonic), SiO2 (dielectric), and Chiral particles. We conducted individual tests for our setup using linearly polarized plane waves at angles of 30-degree, 45-degree, and 60-degree individually. Consistent results were obtained across all angles. In each of the three distinct setups involving the aforementioned particle, a dielectric Rayleigh particle experiences an optical pulling force, a plasmonic Rayleigh particle experiences an optical pushing force, and a chiral Rayleigh particle encounters an optical lateral force. These distinctive force behaviors manifest as a result of the intricate interplay between the material properties of the nanoparticles and the characteristics of the plane-polarized beam, encompassing aspects such as plasmonic response, chirality, and refractive index. Moreover, this technique presents an environmentally sustainable and economically viable alternative to the utilization of expensive and potentially hazardous chemicals in nanoparticle sorting processes within industrial domains.

Edge magnetoplasmon dispersion and time-resolved plasmon transport in a quantum anomalous Hall insulator

A quantum anomalous Hall (QAH) insulator breaks reciprocity by combining magnetic polarization and spin-orbit coupling to generate a unidirectional transmission of signals in the absence of an external magnetic field. Such behavior makes QAH materials a good platform for the innovation of circulator technologies. However, it remains elusive as to how the wavelength of the chiral edge plasmon relates to its frequency and how the plasmon wave packet is excited in the time domain in a QAH insulator. Here, we investigate the edge magnetoplasmon (EMP) resonances in Cr-(Bi,Sb)2Te3 by frequency and time domain measurements. From disk shaped samples with various dimensions, we obtain the dispersion relation of EMPs and extract the drift velocity of the chiral edge state. From the time-resolved transport measurements, we identify the velocity of the plasmon wave packet and observe a transition from the edge to bulk transport at an elevated temperature. We show that the frequency and time domain measurements are well modeled by loss from the microwave induced dissipative channels in the bulk area. Our results demonstrate that the EMP decay rate can be significantly reduced by applying a low microwave power and fabricating devices of larger diameter ≥100µm. In a R=125µm sample, a nonreciprocity of 20 dB has been realized at 1.3 GHz, shining light on using QAH insulators to develop on-chip nonreciprocal devices. Published by the American Physical Society 2024

Universal Chiral-Plasmon-Induced Upward and Downward Transfer of Circular Dichroism to Achiral Molecules.

Electromagnetic chirality transfer represents an effective means of the nanoscale manipulation of optical chirality. While most of the previous reports have exclusively focused on the circular dichroism (CD) transfer from UV-responsive chiral molecules toward visible-resonant achiral colloidal nanoparticles, here we demonstrate a reverse process in which plasmonic chirality can be transferred to achiral molecules, either upward from visible to UV or downward from visible to near infrared (NIR). By hybridizing achiral UV- or NIR-responsive dye molecules with chiral metal nanoparticles in solution, we observe a chiral-plasmon-induced CD (CPICD) signal at the intrinsically achiral molecular absorption bands. Full-wave electromagnetic modeling reveals that both near-field Coulomb interaction and far-field radiative coupling contribute to the observed CPICD, indicating that the mechanism considered here is universal for different material systems and types of optical resonances. Our study provides a set of design guidelines for broadband nanophotonic chiral sensing from the UV to NIR spectral regime.