The research in circularly polarized luminescence has attracted wide interest in recent years. Efforts on one side are directed toward the development of chiral materials with both high luminescence efficiency and dissymmetry factors, and on the other side, are focused on the exploitations of these materials in optoelectronic applications. This review summarizes the recent frontiers (mostly within five years) in the research in circularly polarized luminescence, including the development of chiral emissive materials based on organic small molecules, compounds with aggregation-induced emissions, supramolecular assemblies, liquid crystals and liquids, polymers, metal-ligand coordination complexes and assemblies, metal clusters, inorganic nanomaterials, and photon upconversion systems. In addition, recent applications of related materials in organic light-emitting devices, circularly polarized light detectors, and organic lasers and displays are also discussed.

Frontiers in circularly polarized luminescence: molecular design, self-assembly, nanomaterials, and applications

A series of asymmetric dimers with an odd number of atoms in the spacer were found to form different types of twisted structures despite being achiral. The formation of a variety of helical structures is accompanied by a gradual freezing of molecular rotation. The tight pitch heliconical nematic (NTB) phase and heliconical tilted smectic C (SmCTB) phase are formed. In the lowest temperature smectic phase, HexI, the twist is expressed through the formation of hierarchical structure: nano-scale helices and mesoscopic helical filaments. The short pitch helical structure in smectic phases is confirmed by resonant x-ray measurements.

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Heliconical smectic phases formed by achiral molecules

Infrared (IR) adaptation phenomena are ubiquitous in nature and biological systems. Taking inspiration from natural creatures, researchers have devoted extensive efforts for developing advanced IR adaptive materials and exploring their applications in areas of smart camouflage, thermal energy management, biomedical science, and many other IR-related technological fields. Herein, an up-to-date review is provided on the recent advancements of bioinspired IR adaptive materials and their promising applications. First an overview of IR adaptation in nature and advanced artificial IR technologies is presented. Recent endeavors are then introduced toward developing bioinspired adaptive materials for IR camouflage and IR radiative cooling. According to the Stefan-Boltzmann law, IR camouflage can be realized by either emissivity engineering or thermal cloaks. IR radiative cooling can maximize the thermal radiation of an object through an IR atmospheric transparency window, and thus holds great potential for use in energy-efficient green buildings and smart personal thermal management systems. Recent advances in bioinspired adaptive materials for emerging near-IR (NIR) applications are also discussed, including NIR-triggered biological technologies, NIR light-fueled soft robotics, and NIR light-driven supramolecular nanosystems. This review concludes with a perspective on the challenges and opportunities for the future development of bioinspired IR adaptive materials.

Beyond the Visible: Bioinspired Infrared Adaptive Materials.

Fluorescent Photochromic α‐Cyanodiarylethene Molecular Switches: An Emerging and Promising Class of Functional Diarylethene

Mesogenic soft materials, having single or multiple mesogen moieties per molecule, commonly exhibit typical self-organization characteristics, which promotes the formation of elegant helical superstructures or supramolecular assemblies in chiral environments. Such helical superstructures play key roles in the propagation of circularly polarized light and display optical properties with prominent handedness, that is, chiro-optical properties. The leveraging of light to program the chiro-optical properties of such mesogenic helical soft materials by homogeneously dispersing photosensitive chiral material into an achiral soft system or covalently connecting photochromic moieties to the molecules has attracted considerable attention in terms of materials, properties, and potential applications and has been a thriving topic in both fundamental science and application engineering. State-of-the-art technologies are described in terms of the material design, synthesis, properties, and modulation of photoprogrammable chiro-optical mesogenic soft helical architectures. Additionally, the scientific issues and technical problems that hinder further development of these materials for use in various fields are outlined and discussed. Such photoprogrammable mesogenic soft helical materials are competitive candidates for use in stimulus-controllable chiro-optical devices with high optical efficiency, stable optical properties, and easy miniaturization, facilitating the future integration and systemization of chiro-optical chips in photonics, photochemistry, biomedical engineering, chemical engineering, and beyond.

Photoprogrammable Mesogenic Soft Helical Architectures: A Promising Avenue toward Future Chiro-Optics.

Dynamic patterning of soft materials in a fully reversible and programmable manner with light enables applications in anti-counterfeiting, displays and labelling technology. However, this is a formidable challenge due to the lack of suitable chiral molecular photoswitches. Here, we report the development of a unique intrinsic chiral photoswitch with broad chirality modulation to achieve digitally controllable, selectable and extractable multiple stable reflection states. An anti-counterfeiting technique, embedded with diverse microstructures, featuring colour-tunability, erasability, reversibility, multi-stability and viewing-angle dependency of pre-recorded patterns, is established with these photoresponsive superstructures. This strategy allows dynamic helical transformation from the molecular and supramolecular to the macroscopic level using light-activated intrinsic chirality, demonstrating the practicality of photoprogramming photonics. Chiral liquid-crystal materials with optical properties that can be tuned, erased and reversed offer new opportunities in labelling, displays and anti-counterfeiting. 

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Digital photoprogramming of liquid-crystal superstructures featuring intrinsic chiral photoswitches

Dynamic modulation of soft helix in terms of the molecular organization, handedness, and pitch length could result in a sophisticated control over its functions, opening numerous possibilities toward the exploration of previously unidentified applications. Here, we report a dynamic and reversible transformation of a soft helical superstructure among the helicoidal (molecules orthogonal to helical axis), heliconical (molecules oblique to the helical axis, i.e., oblique helicoidal), and their inverse helices, together with a tunability on the helical pitch, by combining electrical and optical manipulations. This multistate transformation depends on a matching of the temperature, the strength of external stimuli, and the bend and twist elastic effects of the system. A laser emission with tunable wavelength and polarization, and prescribed micropatterns formed by any aforementioned architectures were achieved.

https://advances.sciencemag.org/content/advances/5/10/eaax9501.full.pdf

Stimulated transformation of soft helix among helicoidal, heliconical, and their inverse helices

Dynamic electric field frequency actuated helical and spiral structures enable a plethora of attributes for advanced photonics and engineering in the contemporary era. Nevertheless, leveraging the frequency responsiveness of adaptive devices and systems within a broad dynamic range and maintaining restrained high-frequency induced heating remain challenging. Herein, we establish a frequency-actuated heliconical soft architecture that is quite distinct from that of common frequency-responsive soft materials. We achieve reversible modulation of the photonic bandgap in a wide spectral range by delicately coupling the frequency-dependent thermal effect, field-induced dielectric torque and elastic equilibrium. Furthermore, an information encoder prototype without the aid of complicated algorithm design is established to analogize an information encoding and decoding process with a more convenient and less costly way. A technique for taming and tailoring the distribution of the pitch length is exploited and embodied in a prototype of a spatially controlled soft photonic cavity and laser emission. This work demonstrates a distinct frequency responsiveness in a heliconical soft system, which may not merely inspire the interest in field-assisted bottom-up molecular engineering of soft matter but also facilitate the practicality of adaptive photonics. 

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Dynamically actuated soft heliconical architecture via frequency of electric fields

Dynamic and multi‐dimensional manipulation of laser emission with light allows for optical coding, computing, and imaging photonic chips. However, the coupling balance between photonic resonance and transmission is a formidable challenge due to the uncontrollable chiral microcavity with photo‐reversibility, which is limited to the multi‐freedom of the laser with sustainable and repeatable output beams. Herein, a helical superstructure system with a unique intrinsic chiral photoswitch is developed for resolving the always pendent problems on organized defects in the microcavity. The unique intrinsic chirality based on the photoswitchable system allows laser emission with a sharp and narrow band‐width, with both remarkable thermodynamic stability and robust fatigue‐resistance. A quadri‐dimensional manipulable laser, featuring wavelength‐tunability, wavefront‐shaping, spin angular momentum (SAM), and orbital angular momentum (OAM), is successfully established with the assistance of the photoresponsive intrinsic chiral superstructure with photoreversibility. This technology marks an important milestone, and sketches a future framework for the realms of nanophotonic information encoding, security imprinting, and integrated photonics.

A Quadri‐Dimensional Manipulable Laser with an Intrinsic Chiral Photoswitch

Multidimensional and large‐scale parallel manipulation of light, especially on‐demand tailoring of the working frequency and spatial phase front, is highly pursued in modern optics. Here, broadband tunable planar optics is demonstrated by electrically driving the nanohelix of photopatterned heliconical cholesterics. By preprogramming the initial orientation of the helixes using a dynamic‐mask photoalignment technique, spatial geometric phases can be arbitrarily encoded to the reflected light in a reconfigurable way. Due to the reversible electrically variant pitch of the heliconical superstructures, the reflective Bragg band can be precisely selected in the range from 380 to 1550 nm. In addition to wavelength selection and geometric phase modulation, spatial amplitude modulation and spin reversion can be further expected. This may offer a platform for full‐dimensional manipulation of light, including wavelength/frequency, phase, amplitude, time, and spin, thus upgrading optical information processing techniques.

Binghui Liu

Papers

Digital photoprogramming of liquid-crystal superstructures featuring intrinsic chiral photoswitches

Stimulated transformation of soft helix among helicoidal, heliconical, and their inverse helices

Dynamically actuated soft heliconical architecture via frequency of electric fields

A Quadri‐Dimensional Manipulable Laser with an Intrinsic Chiral Photoswitch

Heliconical Cholesterics Endows Spatial Phase Modulator with an Electrically Customizable Working Band