Spatially Correlated Chirality in Chiral Two-Dimensional Perovskites Revealed by Second-Harmonic-Generation Circular Dichroism Microscopy.

Understanding the chiral mechanism of chiral hybrid perovskites is a prerequisite for developing relevant chiroptoelectronic applications. Although conventional circular dichroism (CD) spectroscopy can be used to characterize chirality in chiral perovskites, it has a low signal-to-noise ratio and can provide only information about macroscopic chirality. Herein, with the aim of revealing the microscopic chiral mechanism in chiral perovskites, we utilize a spacer cation alloying strategy to construct chiral two-dimensional perovskites. For the first time, we demonstrate second-harmonic-generation CD microarea imaging in chiral perovskite thin films to unveil their spatially correlated chirality. In combination with theoretical calculations, it is revealed that the spatially correlated chirality is caused by localized out-of-plane supramolecular orientations. This work will not only advance the understanding of the mechanism of chiroptical activity in chiral perovskites but also provide inspiration for the rational design and synthesis of perovskites for chirality-related nonlinear optoelectronic devices.

Spin-orbit optical Hall effect in π-vector fields.

Given the tremendous increase of data in digital era, vector vortex light with strongly coupled spin and orbital angular momenta of photons have attracted great attention for high-capacity optical applications. To fully utilize such rich degrees of freedom of light, it is highly anticipated to separate the coupled angular momentum with a simple but powerful method, and the optical Hall effect becomes a promising scheme. Recently, the spin-orbit optical Hall effect has been proposed in terms of general vector vortex light using two anisotropic crystals. However, angular momentum separation for π-vector vortex modes, another important part in vector optical fields, have not been explored and it remains challenging to realize broadband response. Here, the wavelength-independent spin-orbit optical Hall effect in π-vector fields has been analyzed based on Jones matrices and verified experimentally using a single-layer liquid-crystalline film with designed holographic structures. Every π-vector vortex mode can be decoupled into spin and orbital components with equal magnitude but opposite signs. Our work could enrich the fields of high-dimensional optics.

Classification of quantum correlation using deep learning.

Quantum correlation, as an intrinsic property of quantum mechanics, has been widely employed to test the fundamental physical principles and explore the quantum-enhanced technologies. However, such correlation would be drowned and even destroyed in the conditions of high levels of loss and noise, which drops into the classical realm and renders quantum advantage ineffective. Especially in low light conditions, conventional linear classifiers are unable to extract and distinguish quantum and classical correlations with high accuracy. Here we experimentally demonstrate the classification of quantum correlation using deep learning to meet the challenge in the quantum imaging scheme. We design the convolutional neural network to learn and classify the correlated photons efficiently with only 0.1 signal photons per pixel. We show that decreasing signal intensity further weakens the correlation and makes an accurate linear classification impossible, while the deep learning method has a strong robustness of such task with the accuracy of 99.99%. These results open up a new perspective to optimize the quantum correlation in low light conditions, representing a step towards diverse applications in quantum-enhanced measurement scenarios, such as super-resolution microscope, quantum illumination, etc.

Regulating Optical Activity and Anisotropic Second-Harmonic Generation in Zero-Dimensional Hybrid Copper Halides.

Structural engineering permits the introduction of chirality into organic-inorganic hybrid metal halides (HMHs), which creates a promising and exclusive material for applications in various optoelectronics. However, the optical activity regulation of chiral HMHs remains largely unexplored. In this work, we have synthesized two pairs of lead-free chiral HMHs with a zero-dimensional tetrahedral arrangement, i.e., (R- and S-1-(1-naphthyl)ethylammonium)2CuCl4 and (R- and S-1-(2-naphthyl)ethylammonium)2CuCl4. The magnitude of optical activity in these HMHs can be efficiently modulated as a result of the different magnetic transition dipole moments. Furthermore, these HMHs exhibited effective second-harmonic generation (SHG) and distinct SHG-circular dichroism (CD), with (R-1-(1-naphthyl)ethylammonium)2CuCl4 having an anisotropy factor (gSHG-CD) of up to 0.41. This work not only provides insights into regulating the optical activity and anisotropic SHG effect of lead-free chiral HMHs but also confirms the feasibility of SHG-CD spectroscopy as a promising tool for characterizing the intrinsic optical activity of chiral materials.

The salt secretion of leaves promotes the competitiveness of Reaumuria soongarica in a desert grassland.

BACKGROUND: For better understanding the mechanism of Reaumuria soongarica community formation in a salt stressed grassland ecosystem, we designed a field experiment to test how leaves salt secretion changes the competitive relationship between species in this plant communities. RESULTS: Among the three species (R. soongarica, Stipa glareosa and Allium polyrhizum) of the salt stressed grassland ecosystem, the conductivity of R. soongarica rhizosphere soil was the highest in five soil layers (0-55 cm depth). The high soil conductivity can increase the daily salt secretion rate of plant leaves of R. soongarica. In addition, we found the canopy size of R. soongarica was positively related to the distance from S. glareosa or A. polyrhizum. The salt-tolerance of R. soongarica was significantly higher than the other two herbs (S. glareosa and A. polyrhizum). Moreover, there was a threshold (600 µS/cm) for interspecific competition of plants mediated by soil conductivity. When the soil conductivity was lower than 600 µS/cm, the relative biomass of R. soongarica increased with the soil conductivity increase. CONCLUSIONS: The efficient salt secretion ability of leaves increases soil conductivity under the canopy. This leads the formation of a "saline island" of R. soongarica. Meanwhile R. soongarica have stronger salt tolerance than S. glareosa and A. polyrhizum. These promote the competitiveness of R. soongarica and inhibit interspecies competition advantage of the other two herbs (S. glareosa and A. polyrhizum) in the plant community. It is beneficial for R. soongarica to establish dominant communities in saline regions of desert grassland.

Strong two-photon absorption induced by energy funneling in chiral quasi-2D perovskites.

Quasi-2D Ruddlesden-Popper-type perovskites (RPPs) exhibit excellent nonlinear optical properties due to their multiple quantum well structures with large exciton binding energy. Herein, we introduce chiral organic molecules into RPPs and investigate their optical properties. It is found that the chiral RPPs possess effective circular dichroism in the ultraviolet to visible wavelengths. Two-photon absorption (TPA)-induced efficient energy funneling from small- to large-n domains is observed in the chiral RPP films, which induces strong TPA with a coefficient up to 4.98 cm MW-1. This work will broaden the application of quasi-2D RPPs in chirality-related nonlinear photonic devices.

Direct Observation of Dynamically Localized Quantum Optical States.

Quantum-correlated biphoton states play an important role in quantum communication and processing, especially considering the recent advances in integrated photonics. However, it remains a challenge to flexibly transport quantum states on a chip, when dealing with large-scale sophisticated photonic designs. The equivalence between certain aspects of quantum optics and solid-state physics makes it possible to utilize a range of powerful approaches in photonics, including topologically protected boundary states, graphene edge states, and dynamic localization. Optical dynamic localization allows efficient protection of classical signals in photonic systems by implementing an analogue of an external alternating electric field. Here, we report on the observation of dynamic localization for quantum-correlated biphotons, including both the generation and the propagation aspects. As a platform, we use sinusoidal waveguide arrays with cubic nonlinearity. We record biphoton coincidence count rates as evidence of robust generation of biphotons and demonstrate the dynamic localization features in both spatial and temporal space by analyzing the quantum correlation of biphotons at the output of the waveguide array. Experimental results demonstrate that various dynamic modulation parameters are effective in protecting quantum states without introducing complex topologies. Our Letter opens new avenues for studying complex physical processes using photonic chips and provides an alternative mechanism of protecting communication channels and nonclassical quantum sources in large-scale integrated quantum optics.

Giant Optical Activity and Second Harmonic Generation in 2D Hybrid Copper Halides.

Hybrid organic-inorganic metal halides have emerged as highly promising materials for a wide range of applications in optoelectronics. Incorporating chiral organic molecules into metal halides enables the extension of their unique optical and electronic properties to chiral optics. By using chiral (R)- or (S)-methylbenzylamine (R-/S-MBA) as the organic component, we synthesized chiral hybrid copper halides, (R-/S-MBA)2 CuCl4 , and investigated their optical activity. Thin films of this material showed a record anisotropic g-factor as high as approximately 0.06. We discuss the origin of the giant optical activity observed in (R-/S-MBA)2 CuCl4 by theoretical modeling based on density functional theory (DFT) and demonstrate highly efficient second harmonic generation (SHG) in these samples. Our study provides insight into the design of chiral materials by structural engineering, creating a new platform for chiral and nonlinear photonic device applications of the chiral hybrid copper halides.

All-optically controlled beam splitting through asymmetric polarization-based holography.

All-optically controlled beam splitting is demonstrated by a tunable split ratio through polarization modulation. The beam splitters are essentially holographic gratings recorded by means of the interference of two 532 nm beams with asymmetric polarization states in an azobenzene liquid crystal film. It is found that the intensity ratio between zero and the first diffraction order is adjustable through the polarization manipulation of the recording light. An arbitrary split ratio from 0 to 1 is obtained with the photoinduced birefringence of the film being set to an appropriate value, which is independent on the polarization state of the probe light. Furthermore, the formation processes of the recorded beam splitters are contributed to the dual-grating coupling, and the tunable split ratio under various polarization conditions is discussed in terms of the Fresnel theory and Jones matrices.

Polarization modulation by means of tunable polarization gratings in an azobenzene side-chain liquid-crystalline polymer film.

Polarization modulation was achieved by means of a new type of grating recorded with two 532 nm beams at varying polarization angles in an azobenzene side-chain liquid-crystalline polymer film through light regulation instead of voltage control. In contrast to conventional polarization holographic gratings, the polarization state of the ± first-order diffracted beams of the recorded gratings depended strongly on angles between polarization directions of two recording beams, while the polarization state of the second-order diffraction remained unchanged. With the polarization angle changing from 0 to 90 deg, the ± first-order diffraction efficiency increased from 5.15% to 10.53%. Diffraction properties of the recorded gratings were attributed to the combination of polarization holographic gratings and amplitude gratings based on the calculation of Jones matrices and polarization holographic theory.

Dependence of plasmon coupling on curved interfaces.

The optical properties of coupled plasmon systems can be tuned by individual material and geometry, gap distance, and surrounding dielectric. This paper reports a dramatic effect of a curved interface in the nanoparticles dimer on the optical responses. Compared with gold nanorod (AuNR) monomer, AuNR dimers with different assembly types (such as end-to-end and side-by-side) can manipulate the longitudinal surface plasmon resonance (SPRL) to red/blueshift. The electromagnetic field of the dimer is further enhanced in the interactive region. Under the incident polarization along the gap, a new resonance mode will be excited when AuNR dimers touch each other, and the SPR mode turns to blueshift from redshift due to the formation of the conductive coupling. It can be assumed that when one of the interactive surfaces is curved, an additional plasmon resonance can be stimulated under the polarization of incident light along the gap. The particular phenomenon can be explained by the plasmon hybridization theory. Silver nanocubes dimers (with sharp or smooth corners and edges) also possess the same property. Supported by finite-difference time-domain solutions, the coupled plasmon resonance mode represents high sensitivity to structural geometry.

Enhanced diffraction properties of photoinduced gratings in nematic liquid crystals doped with Disperse Red 1.

Diffraction properties of photoinduced gratings recorded by overlapping two coherent beams at 532 nm in nematic liquid crystals doped with Disperse Red 1 were investigated with a probe beam at 632.8 nm. The grating was formed due to the alignment of dye molecules that leaded to the reorientation of the liquid crystal phase. The diffraction efficiency of the photoinduced grating was found to increase rapidly when the sample temperature was close to the clearing point in the nematic phase and a nearly 30-fold enhancement of the first-order diffraction efficiency was obtained. The pretransitional enhancement of the diffraction efficiency was discussed in terms of the reorientation of liquid crystals, optical nonlinearity effects and the onset of critical opalescence near the nematic-isotropic phase transition. Moreover, a peak shift of diffraction efficiency towards the lower temperature was observed with the increase of recording light intensity, which was attributed to laser induced photochemical disordering.

Polarization modulation of two-photon excited fluorescence in a V-shaped dipicolinate-triphenylamine compound.

Polarization modulation of two-photon excited fluorescence in a V-shaped dipicolinate-triphenylamine compound was investigated with 100 fs 800 nm laser pulses. The peak fluorescence intensity versus the input irradiance was measured to meet a square dependence, which offered evidence for two-photon excited fluorescence. The variations of the two-photon excited fluorescence intensity showed strong response to the different polarized incident lights and were tightly dependent on the linearly polarized component of the incident light. Furthermore, the polarization modulation efficiency of the two-photon excited fluorescence had an obvious concentration dependence when the concentration of solution was under 2.5×10(-4) mol/L. The enhancement of modulation efficiency was attributed to the concentration dependence of the two-photon absorption cross section.

Polarization-controlled images based on double-exposure polarization holography in an azobenzene liquid-crystalline polymer.

Polarization-controlled optical image operations were demonstrated based on the double-exposure polarization holographic method. Two images were stored in the same volume of an azobenzene liquid-crystalline polymer by recording superimposed holograms, a pair of polarization gratings with one spatial frequency, using two orthogonal circularly polarized 532 nm beams and were reconstructed with a 650 nm laser. The recorded polarization holographic gratings were investigated to show distinctive polarization selectivity, high diffraction efficiency, and good stability. The brightness and the polarization of the diffracted images were found to be dependent on the polarization of the readout beam, and two images could be reconstructed individually or simultaneously.

Polarization-induced fluorescence modulation in a self-assembled coordination cage-shaped complex.

Polarization-induced fluorescence modulation behavior of a self-assembled coordination cage-shaped complex was investigated using femtosecond laser pulses. The variations of the total two-photon-induced fluorescence (TPF) intensity were found to be strongly modulated by different polarized incident lights and tightly dependent on the linearly polarized component of the excited light. The polarization-induced modulation efficiency of the TPF underwent intensity-dependent decrease, which could be attributed to the two-photon-induced excited-state absorption. The nonlinear absorption behavior of the complex was also studied by performing both femtosecond open aperture Z-scan and nonlinear transmission measurements, which help to better understand the intrinsic optical properties of the molecule and portend its practical applications.

Achieving an Excellent Strength and Ductility Balance in Additive Manufactured Ti-6Al-4V Alloy through Multi-Step High-to-Low-Temperature Heat Treatment.

Selective laser melting (SLM) can effectively replace traditional processing methods to prepare parts with arbitrary complex shapes through layer-by-layer accumulation. However, SLM Ti-6Al-4V alloy typically exhibits low ductility and significant mechanical properties anisotropy due to the presence of acicular α' martensite and columnar prior ß grains. Post-heat treatment is frequently used to obtain superior mechanical properties by decomposing acicular α' martensite into an equilibrium α + ß phase. In this study, the microstructure and tensile properties of SLM Ti-6Al-4V alloy before and after various heat treatments were systematically investigated. The microstructure of the as-fabricated Ti-6Al-4V sample was composed of columnar prior ß grains and acicular α' martensite, which led to high strength (~1400 MPa) but low ductility (~5%) as well as significantly tensile anisotropy. The single heat treatment samples with lamellar α + ß microstructure exhibited improved elongation to 6.8-13.1% with a sacrifice of strength of 100-200 MPa, while the tensile anisotropy was weakened. A trimodal microstructure was achieved through multi-step high-to-low-temperature (HLT) heat treatment, resulting in an excellent combination of strength (~1090 MPa) and ductility (~17%), while the tensile anisotropy was almost eliminated. The comprehensive mechanical properties of the HLT samples were superior to that of the conventional manufactured Ti-6Al-4V alloy.

Large-Scale, Abrasion-Resistant, and Solvent-Free Superhydrophobic Objects Fabricated by a Selective Laser Sintering 3D Printing Strategy.

Manufacturing abrasion-resistant superhydrophobic matters is challenging due to the fragile feature of the introduced micro-/nanoscale surface roughness. Besides the long-term durability, large scale at meter level, and 3D complex structures are of great importance for the superhydrophobic objects used across diverse industries. Here it is shown that abrasion-resistant, half-a-meter scaled superhydrophobic objects can be one-step realized by the selective laser sintering (SLS) 3D printing technology using hydrophobic-fumed-silica (HFS)/polymer composite grains. The HFS grains serve as the hydrophobic guests while the sintered polymeric network provides the mechanical strength, leading to low-adhesion, intrinsic superhydrophobic objects with desired 3D structures. It is found that as-printed structures remained anti-wetting capabilities even after undergoing different abrasion tests, including knife cutting test, rude file grinding test, 1000 cycles of sandpaper friction test, tape test and quicksand impacting test, illustrating their abrasion-resistant superhydrophobic stability. This strategy is applied to manufacture a shell of the unmanned aerial vehicle and an abrasion-resistant superhydrophobic shoe, showing the industrial customization of large-scale superhydrophobic objects. The findings thus provide insight for designing intrinsic superhydrophobic objects via the SLS 3D printing strategy that might find use in drag-reduce, anti-fouling, or other industrial fields in harsh operating environments.

Femtosecond third-order optical nonlinearity of an azobenzene-containing ionic liquid crystalline polymer.

The nonlinear optical properties of an azobenzene-containing ionic liquid crystalline polymer were investigated using single beam Z-scan and optical Kerr effect (OKE) techniques. The nonlinear refractive index of electronic origin (3.1×10(-19) m(2)/W) and the nonlinear absorption coefficient (3.63×10(-13) m/W) were determined with 800 nm femtosecond laser pulses at a repetition rate of 1 KHz. The corresponding one-photon and two-photon figures of merit are determined to be 6.05 and 0.94, respectively, at irradiance of 50 GW/cm(2). The response time of the observed nonlinearities is estimated to be as fast as 300 fs. These experiment results demonstrate that the polymer is a promising candidate for applications in all-optical switching modulators and nonlinear photonic devices.

Geometric-phase-based shearing interferometry for broadband vortex state decoding.

Given that spin and orbital angular momenta of photons have been widely investigated in optical communication and information processing systems, efficient decoding of optical vortex states using a single element is highly anticipated. In this work, a wavelength-independent holographic scheme has been proposed for total angular momentum sorting of both scalar and vector vortex states with a stationary broadband geometric-phase waveplate by means of reference-free shearing interferometry. The entangled spin and orbital angular momentum modes can be distinguished simultaneously based on the spin-orbit optical Hall effect in order to realize single-shot vortex detection. The viability of our scheme has also been demonstrated experimentally.