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A diarylethene-based zwitterionic molecule (DZM) is newly synthesized for the development of smart films exhibiting reversible color change and switchable ionic conductivity in response to external light stimuli. This dual molecular building block is constructed through zwitterionic interlocking and strong phase separation between the dendron-shaped aliphatic tails and the diarylethene head. Uniaxial shear coating and molecular self-assembly result in anisotropically oriented nanostructures, which are further solidified through photopolymerization. In the absence of zwitterionic interlocking, DZM fails to form ordered structures and remains disordered. The anisotropically oriented nanostructures of DZM exhibit polarization-dependent photochromic properties despite the inherent low anisotropy of a single diarylethene chromophore. Structural analysis reveals that the zwitterion-interlocked molecular building block self-assemble into nanocolumns that align uniaxially during the shear coating process. Alternating ultraviolet and visible light reversibly switches the ionic conductivity of the DZM thin film and a change in color is observed due to the photoisomerization of the diarylethene chromophore. Utilizing the polarization-dependent photochromic properties, light-sensitive smart thin films are demonstrated with potential applications in anti-counterfeiting labels and sensors., (© 2024 Wiley‐VCH GmbH.)

Terahertz polarimetric imaging, capable of capturing not only intensity profiles but also the polarization states of the incident pattern, is an essential technique with promising applications such as security scans and medical diagnoses. Recently, a novel approach for terahertz imaging has been proposed using a metasurface absorber that converts terahertz light into a temperature profile. However, polarization remains indistinguishable in the imaging process due to the isotropic geometry of the metasurface. To address this issue, this study introduces an all-dielectric, polarization-sensitive metasurface absorber and showcases its suitability for terahertz polarimetric imaging. Optical and thermal simulations confirm that the polarization dependence of our metasurface is translated into the thermal domain, allowing us to distinguish both intensity and polarization states in the incoming image. Additionally, we demonstrate that polarimetric imaging under general, elliptical polarization is attainable. This metasurface facilitates terahertz polarimetric imaging, eliminating the need for complex setups or bulky components, thereby reducing the form factor and enabling widespread use., (© 2024. The Author(s).)

The light-matter interactions at nanoscale can be enhanced by Bloch-surface plasmon polariton (Bloch-SPP) on the plasmonic lattice. An Ag nanohole array in hexagonal arrangement served as an optical cavity to realize the directional and polarized amplified spontaneous emission (ASE) of R6G. A 100-fold enhanced ASE was observed at 15° emission angle under TM polarization when the pump power density exceeded the threshold of 198 W/cm 2 based on the degenerated high state density modes. Moreover, a specific polarization dependence of ASE was modulated by the Bloch-SPP modes, and the degree of polarization was enhanced from 1.3 to 2.1 when the pump power density exceeded the threshold of ASE. This work clarifies the interaction between the gain media and plasmonic systems, which lays a foundation for the plasmonic device designing.

Nanoparticle clusters provide new degrees of freedom for light control due to their mutual interaction compared with an individual one. Here, the authors demonstrate theoretically and experimentally a type of optical anapole (a nonradiating state) termed as extrinsic anapole, with mode field spreading across Si nanodisk dimers unlike the intrinsic one that is confined within individual nanodisks. The extrinsic anapole is sensitive to the polarized excitation. When the electric vector E of excitation is perpendicular to the dimer axis, the coupled toroidal dipole (TD) mode is largely enhanced and broadened to be spectrally overlapped with the electric dipole (ED) mode. The destructive interference of these two modes results in the generation of the extrinsic anapole. However, it vanishes when E is parallel to the dimer axis. Such polarization dependence can be relieved with the participation of the third nanodisk. Scattering spectra of Si nanodisk trimers stay almost unchanged under different polarized excitations, although the near-field distributions are quite different. Finally, enhanced white-light emission is observed in Si nanodisk clusters, which can be attributed to the near-infrared absorption enhancement induced by extrinsic anapole states. The findings manifest that high-index all-dielectric nanodisk clusters are promising for light manipulation based on mode interference., (© 2022 Wiley-VCH GmbH.)

Micro-photoluminescence was observed while increasing the excitation power in a single GaAs quantum ring (QR) at 4 K. Fine structures at the energy levels of the ground ( N = 1) and excited ( N = 2) state excitons exhibited a blue shift when excitation power increased. The excited state exciton had a strong polarization dependence that stemmed from the asymmetric localized state. According to temperature-dependence measurements, strong exciton-phonon interaction (48 meV) was observed from an excited exciton state in comparison with the weak exciton-phonon interaction (27 meV) from the ground exciton state, resulting from enhanced confinement in the excited exciton state. In addition, higher activation energy (by 20 meV) was observed for the confined electrons in a single GaAs QR, where the confinement effect was enhanced by the asymmetric ring structure.

The development of smart inks that change color and transparency in response to external stimuli is very important for various fields, from modern art to safety and anticounterfeiting technology. A uniaxially oriented diacetylene thin film on a macroscopic area is obtained by coating, self-assembling and topochemical photopolymerizing of imidazolium-functionalized diacetylenes (M-DA and T-DA) and 4,6-decadiyne ink (70 wt%:20 wt%:10 wt%) exhibiting a lyotropic smectic A liquid-crystalline phase at room temperature. The color and transparency of letters and symbols written with the DA-based secret inks change reversibly from blue to red as well as from colorless transparent to black opaque depending on the temperature and polarization axis. A secret code written with thermoresponsive and polarization-dependent secret inks consisting of imidazolium-functionalized diacetylenes is successfully deciphered by wearing polaroid glasses and holding a burning torch., (© 2020 Wiley-VCH GmbH.)

Photocurrent production in quasi-one-dimensional (1D) transition-metal trichalcogenides, TiS 3 (001) and ZrS 3 (001), was examined using polarization-dependent scanning photocurrent microscopy. The photocurrent intensity was the strongest when the excitation source was polarized along the 1D chains with dichroic ratios of 4:1 and 1.2:1 for ZrS 3 and TiS 3 , respectively. This behavior is explained by symmetry selection rules applicable to both valence and conduction band states. Symmetry selection rules are seen to be applicable to the experimental band structure, as is observed in polarization-dependent nanospot angle-resolved photoemission spectroscopy. Based on these band symmetry assignments, it is expected that the dichroic ratios for both materials will be maximized using excitation energies within 1 eV of their band gaps, providing versatile polarization sensitive photodetection across the visible spectrum and into the near-infrared.

An evaluation of several experimental aspects that can optimize electrochemical attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) performance using a commercially available, specular reflection accessory is provided. A comparison of different silicon single-bounce internal reflection elements (IREs) is made with emphasis on different face-angled crystal (FAC) options. Selection of optimal angle of incidence for maximizing signal and minimizing noise is shown to require consideration of the optical throughput of the accessory, reflection losses at the crystal surfaces, and polarization effects. The benefits of wire-grid polarizers and antireflective (AR) coatings on the IREs is discussed. High signal-to-noise ratios can be achieved by omitting polarizers, using an AR-coated FAC with a larger face angle, and working at angles of incidence close to the maximum throughput angle of the accessory.

Questions surrounding the optical properties of two-dimensional (2D) triangular single gold nanoplates (AuNPs) remain largely unanswered. Herein, a scanning-electron microscopy-correlated single-particle study was conducted to identify polarization-dependent optical properties of AuNPs under dark-field (DF) and differential interference contrast (DIC) microscopy. AuNPs with an aspect ratio of ∼3 showed a single broad DF scattering spectrum without separation of the two dipole and quadrupole resonance modes present in 2D AuNPs. Polarization-sensitive interference properties of the individual AuNPs were revealed through periodic changes in the intensities and types of DIC images obtained. A dipole resonance mode was found to mainly contribute to the polarization-sensitive interference properties of AuNPs. Furthermore, DIC polarization anisotropy allowed us to track the real-time orientation of a dipole resonance mode of a AuNP rotating on a live cell membrane.

Current polarized Raman-based techniques for identifying the crystalline orientation of black phosphorus suffer significant uncertainty and unreliability because of the complex interference involving excitation laser wavelength, scattering light wavelength, and sample thickness. Herein, for the first time, we present a new method, optothermal Raman spectroscopy (OT-Raman), for identifying crystalline orientation. With a physical mechanism based on the anisotropic optical absorption of the polarized laser and the resulting heating, the OT-Raman can identify the crystalline orientation explicitly, regardless of excitation wavelength and sample thickness, by Raman frequency-power differential Φ (=∂ω/∂P). The parameter Φ has the largest (smallest) value when the laser polarization is along the armchair (zigzag) direction. The OT-Raman technique is robust and is able to identify the crystalline orientation of BP samples with thicknesses up to 300 nm at a minimum and potentially as high as 1200 nm., (© 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A new optical method is proposed to investigate the reflectance of structurally coloured objects, such as Morpho butterfly wing scales and cholesteric liquid crystals. Using a reflected-light microscope and a digital single-lens reflex (DSLR) camera, we have successfully measured the two-dimensional reflection pattern of individual wing scales of Morpho butterflies. We demonstrate that this method enables us to measure the bidirectional reflectance distribution function (BRDF). The scattering image observed in the back focal plane of the objective is projected onto the camera sensor by inserting a Bertrand lens in the optical path of the microscope. With monochromatic light illumination, we quantify the angle-dependent reflectance spectra from the wing scales of Morpho rhetenor by retrieving the raw signal from the digital camera sensor. We also demonstrate that the polarization-dependent reflection of individual wing scales is readily observed using this method, using the individual wing scales of Morpho cypris . In an effort to show the generality of the method, we used a chiral nematic fluid to illustrate the angle-dependent reflectance as seen by this method., Competing Interests: We declare we have no competing interests.

A micro-spectroscopic method has been developed to probe the accessibility of zeolite crystals using a series of fluorescent 4-(4-diethylaminostyryl)-1-methylpyridinium iodide (DAMPI) probes of increasing molecular size. Staining large zeolite crystals with MFI (ZSM-5) topology and subsequent mapping of the resulting fluorescence using confocal fluorescence microscopy reveal differences in structural integrity: the 90° intergrowth sections of MFI crystals are prone to develop structural imperfections, which act as entrance routes for the probes into the zeolite crystal. Polarization-dependent measurements provide evidence for the probe molecule's alignment within the MFI zeolite pore system. The developed method was extended to BEA (Beta) crystals, showing that the previously observed hourglass pattern is a general feature of BEA crystals with this morphology. Furthermore, the probes can accurately identify at which crystal faces of BEA straight or sinusoidal pores open to the surface. The results show this method can spatially resolve the architecture-dependent internal pore structure of microporous materials, which is difficult to assess using other characterization techniques such as X-ray diffraction., (© 2017 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.)

The atomic-scale origin of the unusually high performance and long-term stability of wurtzite p-GaN oriented nanowire arrays is revealed. Nitrogen termination of both the polar (0001¯) top face and the nonpolar (101¯0) side faces of the nanowires is essential for long-term stability and high efficiency. Such a distinct atomic configuration ensures not only stability against (photo) oxidation in air and in water/electrolyte but, as importantly, also provides the necessary overall reverse crystal polarization needed for efficient hole extraction in p-GaN., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

As a new two-dimensional layered material, black phosphorus (BP) is a very promising material for nanoelectronics and optoelectronics. We use Raman spectroscopy and first-principles theory to characterize and understand the low-frequency (LF) interlayer breathing modes (<100 cm(-1)) in few-layer BP for the first time. Using a laser polarization dependence study and group theory analysis, the breathing modes are assigned to Ag symmetry. Compared to the high-frequency (HF) Raman modes, the LF breathing modes are considerably more sensitive to interlayer coupling and, thus, their frequencies show a stronger dependence on the number of layers. Hence, they constitute an effective means to probe both the crystalline orientation and thickness of few-layer BP. Furthermore, the temperature dependence shows that in the temperature range -150 to 30 °C, the breathing modes have a weak anharmonic behavior, in contrast to the HF Raman modes that exhibit strong anharmonicity.

We demonstrate plasmonic enhancement of upconversion luminescence in individual nanocrystal heterodimers formed by template-assisted self-assembly. Lithographically defined, shape-selective templates were used to deterministically coassemble single Au nanorods in proximity to single hexagonal (β-phase) NaYF4:Yb(3+),Er(3+) upconversion nanophosphors. By tailoring the dimensions of the rods to spectrally tune their longitudinal surface plasmon resonance to match the 977 nm excitation wavelength of the phosphors and by spatially localizing the phosphors in the intense near-fields surrounding the rod tips, several-fold luminescence enhancements were achieved. The enhancement effects exhibited a strong dependence on the excitation light's polarization relative to the rod axis. In addition, greater enhancement was observed at lower excitation power densities due to the nonlinear behavior of the upconversion process. The template-based coassembly scheme utilized here for plasmonic coupling offers a versatile platform for improving our understanding of optical interactions among individual chemically prepared nanocrystal components.

Metallic point contacts (MPCs) with dimensions comparable to the Fermi wavelength of conduction electrons act as electronic waveguides and might operate as plasmon transmitters. Here we present a correlated study of optical and conductance response of MPCs under irradiation with laser light. For elucidating the role of surface plasmon polaritons (SPPs), we integrate line gratings into the leads that increase the SPP excitation efficiency. By analyzing spatial, polarization, and time dependence, we identify two SPP contributions that we attribute to transmitted and decaying SPPs, respectively. The results demonstrate the role of SPPs for optically controlling the transport in metallic nanostructures and are important for designing opto-nanoelectronic devices.