Controllable Chiral Light Generation and Vortex Field Investigation Using Plasmonic Holes Revealed by Cathodoluminescence.

Control of the angular momentum of light is a key technology for next-generation nano-optical devices and optical communications, including quantum communication and encoding. We propose an approach to controllably generate circularly polarized light from a circular hole in a metal film using an electron beam by coherently exciting transition radiation and light scattering from the hole through surface plasmon polaritons. The circularly polarized light generation is confirmed by fully polarimetric four-dimensional cathodoluminescence mapping, where angle-resolved spectra are simultaneously obtained. The obtained intensity and Stokes maps show clear interference fringes as well as almost fully circularly polarized light generation with controllable parities by the electron beam position. By applying this approach to a three-hole system, a vortex field with a phase singularity is visualized in the middle of three holes.

Strong Linearly Polarized Light Emission by Coupling Out-of-Plane Exciton to Anisotropic Gap Plasmon Nanocavity.

With exceptional quantum confinement, 2D monolayer semiconductors support a strong excitonic effect, making them an ideal platform for exploring light-matter interactions and as building blocks for novel optoelectronic devices. Different from the well-known in-plane excitons in transition metal dichalcogenides (TMD), the out-of-plane excitons in indium selenide (InSe) usually show weak emission, which limits their applications as light sources. Here, by embedding InSe in an anisotropic gap plasmon nanocavity, we have realized plasmon-enhanced linearly polarized photoluminescence with an anisotropic ratio up to ∼140, corresponding to degree of polarization (DoP) of ∼98.6%. Such polarization selectivity, originating from the polarization-dependent plasmonic enhancement supported by the "nanowire-on-mirror" nanocavity, can be well tuned by the InSe thickness. Moreover, we have also realized an InSe-based light-emitting diode with polarized electroluminescence. Our research highlights the role of excitonic dipole orientation in designing nanophotonic devices and paves the way for developing InSe-based optoelectronic devices with polarization control.

Tuning the Chiral Growth of Plasmonic Bipyramids via the Wavelength and Polarization of Light.

Circularly polarized light (CPL) is a versatile tool to prepare chiral nanostructures, but the mechanism for inducing enantioselectivity is not well understood. This work shows that the energy and polarization of visible photons can initiate photodeposition at different sites on plasmonic nanocrystals. Here, CPL on achiral gold bipyramids (AuBPs) creates hot holes that oxidatively deposit PbO2 asymmetrically. We show for the first time that the location of PbO2 photodeposition and hence optical dissymmetry depends on the CPL wavelength. Specifically, 488 and 532 nm CPL induce PbO2 growth in the middle of AuBPs, whereas 660 nm CPL induces PbO2 growth at the tips. Our observations show that wavelength-dependent plasmonic field distributions are more important than surface lightning rod effects in localizing plasmon-mediated photochemistry. The largest optical dissymmetry occurs at excitation wavelengths between the transverse and longitudinal resonances of the AuBPs because higher-order modes are required to induce chiral electric fields.

Lead-Free Chiral Perovskite for High Degree of Circularly Polarized Light Emission and Spin Injection.

We report a zero-dimensional (0D) lead-free chiral perovskite (S-/R-MBA)4Bi2I10 with a high degree of circularly polarized light (CPL) emission. Our 0D lead-free chiral perovskite exhibits an average degree of circular polarization (DOCP) of 19.8% at 78 K under linearly polarized laser excitation, and the maximum DOCP can reach 25.8%, which is 40 times higher than the highest DOCP of 0.5% in all reported lead-free chiral perovskites to the best of our knowledge. The high DOCP of (S-/R-MBA)4Bi2I10 is attributed to the free exciton emission with a Huang-Rhys factor of 2.8. In contrast, all the lead-free chiral perovskites in prior reports are dominant by self-trapped exciton in which the spin relaxation reduces DOCP dramatically. Moreover, we realize the manipulation of the valley degree of freedom of monolayer WSe2 by using the spin injection of the 0D chiral lead-free perovskites. Our results provide a new perspective to develop lead-free chiral perovskite devices for CPL light source, spintronics, and valleytronics.

Manipulation of Chiral Nonlinear Optical Effect by Light-Matter Strong Coupling.

Light-matter strong coupling (LMSC) is an intriguing state in which light and matter are hybridized inside a cavity. It is increasingly recognized as an excellent way to control material properties without any chemical modification. Here, we show that the LMSC is a powerful state for manipulating chiral nonlinear optical (NLO) effects through the investigation of second harmonic generation (SHG) circular dichroism. At the upper polariton band in LMSC, in addition to the enhancement of SHG by more than 1 order of magnitude, the responsivity to the handedness of circularly polarized light was largely modified, where sign inversion and increase of the dissymmetry factor were achieved. Quarter waveplate rotation analysis revealed that the LMSC clearly influenced the coefficients associated with chirality in the NLO process and also contributed to the enhancement of nonlinear magnetic dipole interactions. This study demonstrated that LMSC serves as a great platform for controlling chiral and magneto-optics.

Ex ovo omnia-why don't we know more about egg quality via imaging?

Determining egg quality is the foremost challenge in assisted reproductive technology (ART). Although extensive advances have been made in multiple areas of ART over the last 40 years, oocyte quality assessment tools have not much evolved beyond standard morphological observation. The oocyte not only delivers half of the nuclear genetic material and all of the mitochondrial DNA to an embryo but also provides complete developmental support during embryonic growth. Oocyte mitochondrial numbers far exceed those of any somatic cell, yet little work has been done to evaluate the mitochondrial bioenergetics of an oocyte. Current standard oocyte assessment in in vitro fertilization (IVF) centers include the observation of oocytes and their surrounding cell complex (cumulus cells) via stereomicroscope or inverted microscope, which is largely primitive. Additional oocyte assessments include polar body grading and polarized light meiotic spindle imaging. However, the evidence regarding the aforementioned methods of oocyte quality assessment and IVF outcomes is contradictory and non-reproducible. High-resolution microscopy techniques have also been implemented in animal and human models with promising outcomes. The current era of oocyte imaging continues to evolve with discoveries in artificial intelligence models of oocyte morphology selection albeit at a slow rate. In this review, the past, current, and future oocyte imaging techniques will be examined with the goal of drawing attention to the gap which limits our ability to assess oocytes in real time. The implications of improved oocyte imaging techniques on patients undergoing IVF will be discussed as well as the need to develop point of care oocyte assessment testing in IVF labs.

Distinctive Chiral Conformations Induced to Poly (naphthalene-1,4-diyl) by Helix-sense-selective Polymerization and Circularly Polarized Light Irradiation.

Optically active poly(naphthalene-1,4-diyl) was prepared through helix-sense-selective polymerization of the corresponding monomers and also through circularly polarized light (CPL) irradiation, resulting in distinctive circular dichroism (CD) spectral patterns. Chirality of the helix-sense-selective polymerization -based polymer is ascribed to preferred-handed helicity while that of the CPL-based polymer to a non-helical, chiral conformation ('biased-dihedral conformation') with preferred-handedness which was stable only in the solid state. The helix of the helix-sense-selective polymerization-based polymer gradually racemized in tetrahydrofuran while it was stabilized by aggregate formation in a hexane-dichloromethane solution. Both helix-sense-selective polymerization- and CPL-based polymers exhibited efficient circularly polarized luminescence.

Independent and combined effects of obesity and traumatic joint injury to the structure and composition of rat knee cartilage.

Osteoarthritis (OA) is a multifactorial joint disease characterized by articular cartilage degradation. Risk factors for OA include joint trauma, obesity, and inflammation, each of which can affect joint health independently, but their interaction and the associated consequences of such interaction were largely unexplored. Here, we studied compositional and structural alterations in knee joint cartilages of Sprague-Dawley rats exposed to two OA risk factors: joint injury and diet-induced obesity. Joint injury was imposed by surgical transection of anterior cruciate ligaments (ACLx), and obesity was induced by a high fat/high sucrose diet. Depth-dependent proteoglycan (PG) content and collagen structural network of cartilage were measured from histological sections collected previously in Collins et al.. (2015). We found that ACLx primarily affected the superficial cartilages. Compositionally, ACLx led to reduced PG content in lean animals, but increased PG content in obese rats. Structurally, ACLx caused disorganization of collagenous network in both lean and obese animals through increased collagen orientation in the superficial tissues and a change in the degree of fibrous alignment. However, the cartilage degradation attributed to joint injury and obesity was not necessarily additive when the two risk factors were present simultaneously, particularly for PG content and collagen orientation in the superficial tissues. Interestingly, sham surgeries caused a through-thickness disorganization of collagen network in lean and obese animals. We conclude that the interactions of multiple OA risk factors are complex and their combined effects cannot be understood by superposition principle. Further research is required to elucidate the interactive mechanism between OA subtypes.

Chiroptical properties of membrane glycerophospholipids and their chiral backbones.

Glycerophospholipid membranes are one of the key cellular components. Still, their species-dependent composition and homochirality remain an elusive subject. In the context of the astrophysical circularly polarized light scenario likely involved in the generation of a chiral bias in meteoritic amino and sugar acids in space, and consequently in the origin of life's homochirality on Earth, this study reports the first measurements of circular dichroism and anisotropy spectra of a selection of glycerophospholipids, their chiral backbones and their analogs. The rather low asymmetry in the interaction of UV/VUV circularly polarized light with sn-glycerol-1/3-phosphate indicates that chiral photons would have been unlikely to directly induce symmetry breaking to membrane lipids. In contrast, the anisotropy spectra of d-3-phosphoglyceric acid and d-glyceraldehyde-3-phosphate unveil up to 20 and 100 times higher maximum anisotropy factor values, respectively. This first experimental report, targeted on investigating the origins of phospholipid symmetry breaking, opens up new avenues of research to explore alternative mechanisms leading to membrane lipid homochirality, while providing important clues for the search for chiral biosignatures of extant and/or extinct life in space, in particular for the ExoMars 2028 mission.

Passive Polarized Vision for Autonomous Vehicles: A Review.

This review article aims to address common research questions in passive polarized vision for robotics. What kind of polarization sensing can we embed into robots? Can we find our geolocation and true north heading by detecting light scattering from the sky as animals do? How should polarization images be related to the physical properties of reflecting surfaces in the context of scene understanding? This review article is divided into three main sections to address these questions, as well as to assist roboticists in identifying future directions in passive polarized vision for robotics. After an introduction, three key interconnected areas will be covered in the following sections: embedded polarization imaging; polarized vision for robotics navigation; and polarized vision for scene understanding. We will then discuss how polarized vision, a type of vision commonly used in the animal kingdom, should be implemented in robotics; this type of vision has not yet been exploited in robotics service. Passive polarized vision could be a supplemental perceptive modality of localization techniques to complement and reinforce more conventional ones.

Topological Flat Bands in Strained Graphene: Substrate Engineering and Optical Control.

The discovery of correlated phases in twisted moiré superlattices accelerated the search for low-dimensional materials with exotic properties. A promising approach uses engineered substrates to strain the material. However, designing substrates for tailored properties is hindered by the incomplete understanding of the relationship between the substrate's shapes and the electronic properties of the deposited materials. By analyzing effective models of graphene under periodic deformations with generic crystalline profiles, we identify strong C2z symmetry breaking as the critical substrate geometric feature for emerging energy gaps and quasi-flat bands. We find continuous strain profiles producing connected pseudomagnetic field landscapes are important for band topology. We show that the resultant electronic and topological properties from a substrate can be controlled with circularly polarized light, which also offers unique signatures for identifying the band topology imprinted by strain. Our results can guide experiments on strain engineering for exploring interesting transport and topological phenomena.

High-Speed Modulation of Polarized Thermal Radiation from an On-Chip Aligned Carbon Nanotube Film.

Spectroscopic analysis with polarized light has been widely used to investigate molecular structure and material behavior. A broadband polarized light source that can be switched on and off at a high speed is indispensable for reading faint signals, but such a source has not been developed. Here, using aligned carbon nanotube (CNT) films, we have developed broadband thermal emitters of polarized infrared radiation with switching speeds of ≲20 MHz. We found that the switching speed depends on whether the electrical current is parallel or perpendicular to the CNT alignment direction with a significantly higher speed achieved in the parallel case. Together with detailed theoretical simulations, our experimental results demonstrate that the contact thermal conductance to the substrate and the conductance to the electrodes are important factors that determine the switching speed. These emitters can lead to advanced spectroscopic analysis techniques with polarized radiation.

Atomically Precise Chiral Metal Nanoclusters for Circularly Polarized Light Detection.

Circularly polarized light (CPL) detection is of great significance in various applications such as drug identification, sensing and imaging. Atomically precise chiral metal nanoclusters with intense circular dichroism (CD) signals are promising candidates for CPL detection, which can further facilitate device miniaturization and integration. Herein, we report the preparation of a pair of optically active chiral silver nanoclusters [Ag7(R/S-DMA)2(dpppy)3] (BF4)3 (R/S-Ag7) for direct CPL detection. The crystal structure and molecular formula of R/S-Ag7 clusters are confirmed by single-crystal X-ray diffraction and high-resolution mass spectrometry. R/S-Ag7 clusters exhibit strong CD spectra and CPL both in solution and solid states. When used as the photoactive materials in photodetectors, R/S-Ag7 enables effective discrimination between left-handed circularly polarized and right-handed circularly polarized light at 520 nm with short response time, high responsivity and considerable discrimination ratio. This study is the first report on using atomically precise chiral metal nanoclusters for CPL detection.

Chiral Au@CeO2 Helical Nanorods with Spatially Separated Structures for Polarization-dependent N2 Photofixation.

Chiral photocatalytic nanomaterials possess numerous unique properties and hold promise for various applications in chemical synthesis, environmental protection, energy conversion, and photoelectric devices. Nevertheless, it is uncommon to develop effective means to enhance the asymmetric catalytic performances of chiral plasmonic nanomaterials. In this study, a type of L/D-Au@CeO2 helical nanorods (HNRs) was fabricated by selectively growing CeO2 on the surface of Au HNRs via a facile wet-chemistry construction method. Chiral Au@CeO2 HNRs, featuring Au and CeO2 with spatially separate structures, exhibited the highest photocatalytic performance for N2 fixation, being 50.80 ± 2.64 times greater than Au HNRs. Furthermore, when L-Au@CeO2 HNRs corresponded left circularly polarized light (CPL) and D-Au@CeO2 HNRs corresponded right CPL, their photocatalytic efficiency was enhanced by 3.06 ± 0.06 times in contrast with the samples illuminated with the opposite CPL, which can be attributed to the asymmetrical generation of hot carriers upon CPL excitation. This study not only offered a simple approach to enhance the photocatalytic performance of chiral plasmonic nanomaterials but also demonstrated the potential of chiral plasmonic materials for application in specific photocatalytic reactions, such as N2 fixation.

Magneto-chiral Nonlinear Optical Effect with Large Anisotropic Response in Two-Dimensional Halide Perovskite.

The chiral organic-inorganic halide perovskites (OIHPs) are vital candidates for superior nonlinear optical (NLO) effects associated with circularly polarized (CP) light. NLO in chiral materials often couples with magnetic dipole (MD) transition, as well as the conventional electric dipole (ED) transition. However, the importance of MD transition in NLO process of chiral OIHPs has not yet been well recognized. Here, the circular polarized probe analysis of second harmonic generation circular dichroism (SHG-CD) provides the direct evidence that the contribution of MD leads to a large anisotropic response to CP lights in chiral OIHPs, (R-/S-MBACl)2PbI4. The thin films exhibit great sensitivity to CP lights over a wide wavelength range, and the g-value reaches up to 1.57 at the wavelength where the contribution of MD is maximized. Furthermore, it is also effective as CP light generator, outputting CP-SHG with maximum g-factor of 1.76 upon the stimulation of linearly polarized light. This study deepens the understanding of relation between chirality and magneto-optical effect, and such an efficient discrimination and generation of CP light signal is highly applicable for chirality-based sensor and optical communication devices.

In situ Light-Writable Orientation Control in Liquid Crystal Elastomer Film Enabled by Chalcones.

Liquid crystal elastomers (LCEs) are stimulus-responsive materials with intrinsic anisotropy. However, it is still challenging to in situ program the mesogen alignment to realize three-dimensional (3D) deformations with high-resolution patterned structures. This work presents a feasible strategy to program the anisotropy of LCEs by using chalcone mesogens that can undergo a photoinduced cycloaddition reaction under linear polarized light. It is shown that by controlling the polarization director and the irradiation region, patterned alignment distribution in a freestanding LCE film can be created, which leads to complex and reversible 3D shape-morphing behaviors. The work demonstrates an in situ light-writing method to achieve sophisticated topography changes in LCEs, which has potential applications in encryption, sensors, and beyond.

Low Detection Limit Circularly Polarized Light Detection Realized by Constructing Chiral Perovskite/Si Heterostructures.

Chiral perovskites have been demonstrated as promising candidates for direct circularly polarized light (CPL) detection due to their intrinsic chirality and excellent charge transport ability. However, chiral perovskite-based CPL detectors with both high distinguishability of left- and right-handed optical signals and low detection limit remain unexplored. Here, a heterostructure, (R-MPA)2 MAPb2 I7 /Si (MPA = methylphenethylamine, MA = methylammonium) is constructed, to achieve high-sensitive and low-limit CPL detection. The heterostructures with high crystalline quality and sharp interface exhibit a strong built-in electric field and a suppressed dark current, not only improving the separation and transport of the photogenerated carriers but also laying a foundation for weak CPL signals detection. Consequently, the heterostructure-based CPL detector obtains a high anisotropy factor up to 0.34 with a remarkably low CPL detection limit of 890 nW cm-2 under the self-driven mode. As a pioneering study, this work paves the way for designing high-sensitive CPL detectors that simultaneously have great distinguishing capability and low detection limit of CPL.

Multispectral and Circular Polarization-Sensitive Carbon Dot-Polydiacetylene Capacitive Photodetector.

Multispectral photodetectors (MSPs) and circularly polarized light (CPL) sensors are important in opto-electronics, photonics, and imaging. A capacitive photodetector consisting of an interdigitated electrode coated with carbon dot/anthraquinone-polydiacetylene is constructed. Photoexcitation of the carbon dots induces transient electron transfer to the anthraquinone moieties, and concomitant change in the film dielectric constant and recorded capacitance. This unique photodetection mechanism furnishes wavelength selectivity that is solely determined by the absorbance of the carbon dots incorporated in the anthraquinone-polydiacetylene matrix. Accordingly, employing an array of polymerized-anthraquinone photodetector films comprising carbon dots (C-dots) exhibiting different excitation wavelengths yielded optical "capacitive fingerprints" in a broad spectral range (350-650 nm). Furthermore, circular light polarization selectivity is achieved through chiral polymerization of the polydiacetylene framework. The carbon dot/anthraquinone-polydiacetylene capacitive photodetector features rapid photo-response, high fidelity, and recyclability as the redox reactions of anthraquinone are fully reversible. The carbon dot/anthraquinone-polydiacetylene platform is inexpensive, easy to fabricate, and consists of environmentally friendly materials.

Room-Temperature Polarized Light-Emitting Diode-Based on a 2D Monolayer Semiconductor.

Transition metal dichalcogenide (TMD)-based 2D monolayer semiconductors, with the direct bandgap and the large exciton binding energy, are widely studied to develop miniaturized optoelectronic devices, e.g., nanoscale light-emitting diodes (LEDs). However, in terms of polarization control, it is still quite challenging to realize polarized electroluminescence (EL) from TMD monolayers, especially at room temperature. Here, by using Ag nanowire top electrode, polarized LEDs are demonstrated based on 2D monolayer semiconductors (WSe2 , MoSe2 , and WS2 ) at room temperature with a degree of polarization (DoP) ranging from 50% to 63%. The highly anisotropic EL emission comes from the 2D/Ag interface via the electron/hole injection and recombination process, where the EL emission is also enhanced by the polarization-dependent plasmonic resonance of the Ag nanowire. These findings introduce new insights into the design of polarized 2D LED devices at room temperature and may promote the development of miniaturized 2D optoelectronic devices.

Self-Assembled Tetratic Crystals by Orthogonal Colloidal Force.

Bonding simple building blocks to create crystalline materials with design has been sophisticated in the molecular world, but this is still very challenging for anisotropic nanoparticles or colloids, because the particle arrangements, including position and orientation, cannot be manipulated as expected. Here biconcave polystyrene (PS) discs to present a shape self-recognition route are used, which can control both the position and orientation of particles during self-assembly by directional colloidal forces. An unusual but very challenging two-dimensional (2D) open superstructure-tetratic crystal (TC)-is achieved. The optical properties of the 2D TCs are studied by the finite difference time domain method, showing that the PS/Ag binary TC can be used to modulate the polarization state of the incident light, for example, converting the linearly polarized light into left-handed or right-handed circularly polarized light. This work paves an important way for self-assembling many unprecedented crystalline materials.