Manipulation Of Chirality Research Articles

Dual-band spin-dependent perfect absorber with anisotropic thin films in mid-infrared range

Abstract Motivated by the imperative demand for chirality manipulation within mid-infrared (mid-IR) range, this study presents an innovative solution to obtain selective perfect absorption and chiroptical responses with conventional Otto configuration. Optical responses of the structure have been calculated numerically by the 4×4 anisotropic transfer matrix method (ATMM). The results show that the proposal supports the chiral response with dual-band resonance in absorption spectra by displaying different properties for left-hand circular polarization (LCP) and right-hand circular polarization (RCP) light, its circular dichroism (CD) and working wavelength could be tuned by adjusting the layer thickness and incidence angle. It is demonstrated that the proposed device exhibits an extraordinary absorption efficiency of unity for RCP light and zero for LCP light at a wavelength of 9.32 μm, accompanied by a maximum CD in absorption of -1. The strategy in manipulating dual-band selective chiroptical (CO) responses holds great potential in realizing mid-IR devices capable of chirality manipulation.

Controllable optical chirality of vortex beams via photonic jets

Recent years have witnessed great interest in the optical chirality of vortex beams carrying orbital angular momentum (OAM). An interesting area of research is the control of such an optical chirality. In this work, we report a study of the controllable optical chirality of vortex beams via photonic jets. Within the framework of the generalized Lorenz–Mie theory (GLMT), we present the analytical expressions for describing the electromagnetic fields of the photonic jets formed on the shadow side of the micro-sized dielectric spheres illuminated by Laguerre–Gaussian (LG) vortex beams. The optical chirality of the vortex beams focused in the near-field area of the photonic jets is numerically simulated. It is revealed that the optical chirality of the vortex beams is drastically enhanced via photonic jets. Moreover, the optical chirality of the vortex beams focused in the near-field area of the photonic jets can be controlled by choosing the radius and refractive index of the dielectric sphere. Such controllable optical chirality is expected to be applicable in chiral manipulation, detection, and recognition.

Chiral Stacking Identification of Two-Dimensional Triclinic Crystals Enabled by Machine Learning.

Chiral materials possess broken inversion and mirror symmetry and show great potential in the application of next-generation optic, electronic, and spintronic devices. Two-dimensional (2D) chiral crystals have planar chirality, which is nonsuperimposable on their 2D enantiomers by any rotation about the axis perpendicular to the substrate. The degree of freedom to construct vertical stacking of 2D monolayer enantiomers offers the possibility of chiral manipulation for designed properties by creating multilayers with either a racemic or enantiomerically pure stacking order. However, the rapid recognition of the relative proportion of two enantiomers becomes demanding due to the complexity of stacking orders of 2D chiral crystals. Here, we report the unambiguous identification of racemic and enantiomerically pure stackings for layered ReSe2 and ReS2 using circular polarized Raman spectroscopy. The chiral Raman response is successfully manipulated by the enantiomer proportion, and the stacking orders of multilayer ReSe2 and ReS2 can be completely clarified with the help of second harmonic generation and scanning transmission electron microscopy measurements. Finally, we trained an artificial intelligent Spectra Classification Assistant to predict the chirality and the complete crystallographic structures of multilayer ReSe2 from a single circular polarized Raman spectrum with the accuracy reaching 0.9417 ± 0.0059.

Terahertz Magnetic Moiré Grating for Enhanced Chirality Manipulation and Nonreciprocal Spin Isolation

AbstractMagneto‐optical activity is a significant way to achieve asymmetric transmission for spin photons. However, it is severely limited by the weak light‐matter interaction in the terahertz (THz) region. In this work, a magnetic Moiré grating (MMG) is constructed by sandwiching an Yttrium iron garnet (YIG) single crystal in a pair of twisted 2D subwavelength gratings. The twisted angle between two gratings introduces a strong geometric Moiré chirality related to the Moiré pattern. When an external magnetic field is applied to the YIG layer, three different symmetries of spacial mirror image, time reversal, and spin conjugation are broken simultaneously under the chiral coupling between magneto‐optical activity and Moiré chirality, leading to both the enhanced magneto‐optical chiral transmission and the nonreciprocal spin isolation. Under the magnetic field varying from −0.26 to +0.26 T in the experiment, the MMG achieves an active modulation of circular dichroism from 39 to −37.5 dB and optical activity from −35° to 30°. Moreover, the maximum spin isolation over 32.6 dB is also obtained near 0.5 THz. This mechanism provide a new way to realize independent manipulation and active modulation of THz spin photons more flexibly.

Tuning the Chirality Evolution in Achiral Subnanometer Systems by Judicious Control of Molecule Interactions.

Chirality evolution from molecule levels to the nanoscale in an achiral system is a fundamental issue that remains undiscovered. Here, we report the assembly of polyoxometalate (POM) clusters into chiral subnanostructures in achiral systems by programmable single-molecule interactions. Driven by the competing binding of Ca2+ and surface ligands, POM assemblies would twist into helical nanobelts, nanorings, and nanotubes with tunable helicity. Chiral molecules can be used to differentiate the formation energies of chiral isomers and immobilize the homochiral isomer, where strong circular dichroism (CD) signals are obtained in both solutions and films. Chiral helical nanobelts can be used as circularly polarized light (CPL) photodetectors due to their distinct chiroptic responsivity for right and left CPL. By the fine-tuning of interactions at single-molecule levels, the morphology and CD spectra of helical assemblies can be precisely controlled, providing an atomic precision model for investigation of the structure-chirality relationship and chirality manipulation at the nanoscale.

Spontaneous Chirality Flipping in an Orthogonal Spin-Charge Ordered Topological Magnet

The asymmetric distribution of chiral objects with opposite chirality is of great fundamental interest ranging from molecular biology to particle physics. In quantum materials, chiral states can build on inversion-symmetry-breaking lattice structures or emerge from spontaneous magnetic ordering induced by competing interactions. Although the handedness of a chiral state can be changed through external fields, a spontaneous chirality flipping has yet to be discovered. We present experimental evidence of chirality flipping via changing temperature in a topological magnet EuAl4, which features orthogonal spin density waves (SDW) and charge density waves (CDW). Using circular dichroism of Bragg peaks in the resonant magnetic x-ray scattering, we find that the chirality of the helical SDW flips through a first-order phase transition with modified SDW wavelength. Intriguingly, we observe that the CDW couples strongly with the SDW and displays a rare commensurate-to-incommensurate transition at the chirality flipping temperature. Combining with first-principles calculations and angle-resolved photoemission spectroscopy, our results support a Fermi surface origin of the helical SDW with intertwined spin, charge, and lattice degrees of freedom in EuAl4. Our results reveal an unprecedented spontaneous chirality flipping and lay the groundwork for a new functional manipulation of chirality through momentum-dependent spin-charge-lattice interactions. Published by the American Physical Society 2024

Chirality manipulation of ultrafast phase switches in a correlated CDW-Weyl semimetal

Light engineering of correlated states in topological materials provides a new avenue of achieving exotic topological phases inaccessible by conventional tuning methods. Here we demonstrate a light control of correlation gaps in a model charge-density-wave (CDW) and polaron insulator (TaSe4)2I recently predicted to be an axion insulator. Our ultrafast terahertz photocurrent spectroscopy reveals a two-step, non-thermal melting of polarons and electronic CDW gap via the fluence dependence of a longitudinal circular photogalvanic current. This helicity-dependent photocurrent reveals continuous ultrafast phase switches from the polaronic state to the CDW (axion) phase, and finally to a hidden Weyl phase as the pump fluence increases. Additional distinctive attributes aligning with the light-induced switches include: the mode-selective coupling of coherent phonons to the polaron and CDW modulation, and the emergence of a non-thermal chiral photocurrent above the pump threshold of CDW-related phonons. The demonstrated ultrafast chirality control of correlated topological states here holds large potentials for realizing axion electrodynamics and advancing quantum-computing applications.

Strong chirality and asymmetric transmission effect in twisted bilayer α-MoO3 in terahertz band

Chirality and asymmetric transmission have wide-ranging applications in fields such as optics, chemical synthesis, pharmaceutical research, biological analysis, materials science and communication technology. In this work, we have demonstrated a terahertz (THz) device with strong chirality and asymmetric transmission effect based on a twisted bilayer α-MoO3. The unique optical response can be realized by adjusting structural parameters such as the thicknesses of the layers as well as the angle of relative rotation. It is found that the proposed structure achieves a giant circular dichroism (CD) value of 0.81 at 9.8 THz, which originates from the symmetry breaking of the structure. The phenomenon has been approved by the polarization conversion and the distributions of the electric field. In addition, the device exhibits the asymmetric transmission effect for circularly polarized wave incidence. The results show that the forward and backward transmissivity of circularly polarized waves with different handedness exhibit a significant difference of up to 0.55 at 9.2 THz. This work simultaneously achieves chirality and asymmetric transmission effect in the terahertz band, which paves the way for developing terahertz devices capable of chirality manipulation and optical isolation.

Phonon Chirality Manipulation Mechanism in Transition-Metal Dichalcogenide Interlayer-Sliding Ferroelectrics.

As an ideal platform, both the theoretical prediction and first experimental verification of chiral phonons are based on transition-metal dichalcogenide materials. The manipulation of phonon chirality in these materials will have a profound effect on the study of chiral phonons. In this work, we utilize the sliding ferroelectric effect to realize the phonon chirality manipulation mechanism in transition-metal dichalcogenide materials. Based on first-principles calculations, we find the different manipulation effects of interlayer sliding on the phonon chirality and Berry curvature in bilayer and four-layer MoS2 sliding ferroelectrics. These further affect the phonon angular momentum and magnetization under a temperature gradient and the phonon Hall effect under a magnetic field. Our work connects two emerging fields and opens up a new route to manipulating phonon chirality in transition-metal dichalcogenide materials through the sliding ferroelectric mechanism.

Arbitrary terahertz chirality construction and flexible manipulation enabled by anisotropic liquid crystal coupled chiral metasurfaces

Chiral metasurfaces integrated with active materials can dynamically control the chirality of electromagnetic waves, making them highly significant in physics, chemistry, and biology. Herein, we theoretically proposed a general and feasible design scheme to develop a chiral metadevice based on a bilayer anisotropic metasurface and a monolayer liquid crystal (LC), which can construct and flexibly manipulate arbitrary terahertz (THz) chirality. When the twist angle between the anisotropic axes of two metasurfaces θ is not 0°, the spatial mirror symmetry of the chiral metadevice is broken, resulting in a strong THz chiral response. In addition, the introduction of anisotropic LCs not only enhances the chiral response of the metadevice but also induces the flipping modulation and frequency tunability of the chirality. More importantly, by optimizing the θ, we can flexibly design the arbitrary chiral response and the operating frequency of chirality, thereby promoting the emergence of various chiral manipulation devices. The experimental results show that the maximum circular dichroism can reach −33 dB at 0.94 THz and flip to 28 dB at 0.69 THz by rotating the LC optical axis from the x to y axis, with the maximum operating frequency tunable range of ∼120 GHz. We expect this design strategy can create new possibilities for the advancement of active THz chiral devices and their applications, including chiral spectroscopy, molecular recognition, biosensing, and fingerprint detection.

Maximum helical dichroism enabled by an exceptional point in non-Hermitian gradient metasurfaces

Helical dichroism (HD) utilizing unbounded orbital angular momentum degree of freedom, has provided an important means of exploring chiral effects in diverse wave systems, surpassing the two-state constraint in circular dichroism that relies on intrinsic spin. However, the naturally feeble chiral signals that arise during wave-matter interactions pose significant challenges to the effective enlargement of HD. Here, we introduce a new paradigm for realizing maximum HD through non-Hermitian gradient metasurfaces by engineering a chiral exceptional point (EP) in intrinsic topological charge. The non-Hermitian gradient metasurfaces are empowered by the asymmetric coupling feature at the EP, enabling flexible construction to realize versatile chirality control in extreme circumstances where one chiral vortex is totally reflected and the opposite counterpart is completely absorbed or transmitted into the customized vortex modes. As the manifestation of the maximum HD, we present the first experimental demonstration of perfect chirality-selected vortex transmission in acoustics. Our findings open new venues to achieve maximum chirality and explore chiral physics of wave-matter interactions, which can boost many vortical applications in asymmetric chirality manipulation, one-way propagation, and information multiplexing.

Chiral Molecular Cage with Tunable Stereoinversion Barriers.

The manipulation of chirality in molecular entities that rapidly interconvert between enantiomeric forms is challenging, particularly at the supramolecular level. Advances in controlling such dynamic stereochemical systems offer opportunities to understand chiral symmetry breaking and homochirality. Herein, we report the synthesis of a face-rotating tetrahedron (FRT), an organic molecular cage composed of tridurylborane facial units that undergo stereomutations between enantiomeric trefoil propeller-like conformations. After resolution, we show that the racemization barrier of the enantiopure FRT can be regulated in situ through the reversible binding of fluoride anions onto the tridurylborane moieties. Furthermore, the addition of an enantiopure phenylethanol to the FRT can effectively induce chirality of the molecular cage by preferentially binding to one of its enantiomeric conformers. This study presents a new paradigm for controlling dynamic chirality in supramolecular systems, which may have implications for asymmetric synthesis and dynamic stereochemistry.

Second harmonic generation in plasmonic metasurfaces enhanced by symmetry-protected dual bound states in the continuum.

We numerically investigate linear and nonlinear optical responses in metasurfaces consisting of Au double-gap split ring resonators (DSRRs). Symmetry-protected dual bound states in the continuum (BICs) in such plasmonic metasurfaces are observed at the near-infrared optical regime. Efficient second harmonic generation (SHG) is obtained at the quasi-BIC models due to the symmetry broken. The optimized SHG responses are obtained at the critical couplings between radiation and nonradiation processes at the linearly x- and y-polarized light, respectively. High conversion efficiency of SHG of a value 10-6 is arrived at the fundamental intensity of 10 GW/cm2 at the quasi-BIC wavelength under the y-polarized illumination. Large extrinsic and tunable chirality of linear and nonlinear optical responses empowered by quasi-BICs is acquired in asymmetry metasurfaces at oblique circularly polarized incidence. The results indicate that the plasmonic metasurfaces of symmetry-protected BICs at the near-infrared optical regime have great potential applications in the on-chip efficient frequency conversion, and the linear and nonlinear chiral manipulation.

Tuning of the Supramolecular Helicity of Peptide-Based Gel Nanofibers.

Helical supramolecular architectures play important structural and functional roles in biological systems. The helicity of synthetic molecules can be tuned mainly by the chiral manipulation of the system. However, tuning of helicity by the achiral unit of the molecules is less studied. In this work, the helicity of naphthalimide-capped peptide-based gel nanofibers is tuned by the alteration of methylene units present in the achiral amino acid. The inversion of supramolecular helicity has been extensively studied by CD spectroscopy and morphological analysis. The density functional theory (DFT) study indicates that methylene spacers influence the orientation of π-π stacking interactions of naphthalimide units in the self-assembled structure that regulates the helicity. This work illustrates a new approach to tuning the supramolecular chirality of self-assembled biomaterials.

On-Demand Dynamic Chirality Selection in Flower Corolla-like Micropillar Arrays.

Chiral morphology has been intensively studied in various fields including biology, organic chemistry, pharmaceuticals, and optics. On-demand and dynamic chiral inversion not only cannot be realized in most intrinsically chiral materials but also has mostly been limited to chemical or light-induced methods. Herein, we report reversible real-time magneto-mechanical chiral inversion of a three-dimensional (3D) micropillar array between achiral, clockwise, and counterclockwise chiral arrangements. Inspired by the flower corolla, achiral arrays of five and six radially arranged semicylindrical micropillars were employed as model systems to investigate the dynamic symmetry properties of arrays consisting of odd and even numbers of micropillars, respectively. Each micropillar underwent twisting actuation with a different twisting angle depending on the angle with the magnetic field direction and magnetic flux density, thereby collectively changing the chirality from the achiral to chiral state. Importantly, the morphological handedness of the micropillars was inverted within a few seconds by manipulating the direction of the magnetic field. A chiral morphology consisting of magnetically twisted micropillars was shape-fixed by the introduction of a polymeric binder. This binder could be simply washed off to return the shape-fixed twisted micropillars to their initial straight state. Magnetically programmable and reproducible 3D flower corolla-like micropillar arrays are expected to expand the potential of shape-reconfigurable devices that require real-time chiral manipulation in ambient environments.

Spin–Orbit-Engineered Selective Transport of Photons in Plasmonic Nanocircuits with Panda-Patterned Transporters

The spin–orbit coupling of light, which can be utilized to manipulate the polarization and spatial degrees of freedom of photons, has shown unprecedented potential in realizing on-chip integrated nanocircuits and quantum information processing. Particularly, this chiral coupling mechanism can result in unidirectional transport of spin-dependent light at a subwavelength scale by designing specific nanostructures. Here we propose and demonstrate a dielectric-loaded plasmonic nanocircuit with a panda-patterned transporter to directionally couple and guide plasmonic waves through two-branched waveguides. Both simulation and experimental results reveal that the waveguide modes excited by circularly polarized light with different spin states can be selectively coupled to one of two branching waveguides, with a measured unidirectionality efficiency up to 0.95. The proposed configuration may open up more possibilities in developing multifunctional nanocircuits that could be utilized for exploiting chiral manipulation with flexible degrees of freedom.

Chirality of optical vortex beams reflected from an air-chiral medium interface.

Chirality plays an important role in understanding of the chiral light-matter interaction. In this work, we study theoretically and numerically the chirality of optical vortex beams reflected from an air-chiral medium interface. A theoretical model that takes into full account the vectorial nature of electromagnetic fields is developed to describe the reflection of optical vortex beams at an interface between air and a chiral medium. Some numerical simulations are performed and discussed. The results show that the chirality of the reflected vortex beams can be well controlled by the relative chiral parameter of the medium and is significantly affected by the incidence angle, topological charge, and polarization state of the incident beam. Our results provide new, to the best of our knowledge, insights into the interactions between optical vortex beams with chiral matter, and may have potential application in optical chirality manipulation.

Chiral Asymmetric Polarizations Generated by Bioinspired Helical Carbon Fibers to Induce Broadband Microwave Absorption and Multispectral Photonic Manipulation

AbstractChirality, in which electromagnetic characteristic promotes asymmetric polarization, is expected to realize broadband absorption for microwave absorption materials (MAMs). Herein, inspired by the microstructure of nepenthes, a scalable approach is reported for fabricating hierarchical‐chiral helical carbon fibers with broadband microwave absorption as well as multispectral chiral manipulation. The chiral potential barriers are established by applying helically distributed stress to the fiber, which induce helical electric dipoles via positive and negative charges accumulated at the potential barriers. The states of polarization loss by Debye relaxation are 2, 3, and 4 in the samples with achirality, single‐chirality, and dual‐chirality, respectively; the polar vector of achiral electric dipoles is transformed into pseudovectors through chiral potential barriers to improve the synergistically magnetic loss, and the grade of chirality is quantified based on symmetry breaking theory. The single‐chiral fibers reach strongest absorption peak value of −30.67 dB at 2.96 GHz (carbon content is 50 wt%), and the dual‐chiral fibers achieve effective absorption bandwidth (RL ≤ −10 dB) of 8.8–18 GHz. In addition to microwaves, the chiral photonic manipulation plays a role in near‐ultraviolet and visible spectra. The present discovery points to a pathway for using chiral model to open up new microwave absorption mechanism and integrated application.

Phase-field simulations of vortex chirality manipulation in ferroelectric thin films

The ferroelectric chiral vortex domains are highly desirable for the application of data storage devices with low-energy consumption and high-density integration. However, the controllable switching of vortex chirality remains a challenge in the current ferroelectric community. Utilizing phase-field simulations, we investigate the vortex domain evolution and chirality formation in BiFeO3 thin films. By applying local surface charge or electric field, we demonstrate that the vorticity and the polarity can be manipulated by the initial bi-domain arrangement and the external field with different directions, respectively. By exchanging the domain arrangements, the opposite chirality can be obtained. Importantly, the topological vortex domain is retained after removing the external field. The vortex chirality can be switched reversibly with high reproducibility, which is beneficial to fatigue tolerance of the material in the operation. These results provide theoretical guidance for manipulating the vortex chirality in ferroelectric films.

Chiral Generation of Hot Carriers for Polarization-Sensitive Plasmonic Photocatalysis.

Mastering the manipulation of chirality at the nanoscale has long been a priority for chemists, physicists, and materials scientists, given its importance in the biochemical processes of the natural world and in the development of novel technologies. In this vein, the formation of novel metamaterials and sensing platforms resulting from the synergic combination of chirality and plasmonics has opened new avenues in nano-optics. Recently, the implementation of chiral plasmonic nanostructures in photocatalysis has been proposed theoretically as a means to drive polarization-dependent photochemistry. In the present work, we demonstrate that the use of inorganic nanometric chiral templates for the controlled assembly of Au and TiO2 nanoparticles leads to the formation of plasmon-based photocatalysts with polarization-dependent reactivity. The formation of plasmonic assemblies with chiroptical activities induces the asymmetric formation of hot electrons and holes generated via electromagnetic excitation, opening the door to novel photocatalytic and optoelectronic features. More precisely, we demonstrate that the reaction yield can be improved when the helicity of the circularly polarized light used to activate the plasmonic component matches the handedness of the chiral substrate. Our approach may enable new applications in the fields of chirality and photocatalysis, particularly toward plasmon-induced chiral photochemistry.