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Miniaturized lasers with multicolor output and high spectral purity are indispensable for various ultracompact photonic devices. Here, we propose an optically reconfigurable Forster resonance energ...

We demonstrate a controllable photoluminescence anisotropy amplification in organic luminescent radical-doped microcrystals via exciton funneling. The widely tunable doping ratio resulting from very similar molecular structures between hosts and guests leads to a freely tailorable exciton funneling process, which paves an avenue for the construction of high-performance polarizing optical elements.

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.

Flexible laser display is a critical component for an information output port in next-generation wearable devices. So far, the lack of appropriate display panels capable of providing sustained operation under rigorous mechanical conditions impedes the development of flexible laser displays with high reliability. Owing to the multiple scattering feedback mechanism, random lasers render high mechanical flexibility to withstand deformation, thus making them promising candidates for flexible display planes. However, the inability to obtain pixelated random laser arrays with highly ordered emissive geometries hinders the application of flexible laser displays in the wearable device. Here, for the first time, we demonstrate a mass fabrication strategy of full-color random laser arrays for flexible display panels. The feedback closed loops can be easily fulfilled in the pixels by multiple scatterings to generate durative random lasing. Due to the sustained operation of random laser, the display performance was well-maintained under mechanical deformations, and as a result, a flexible laser display panel was achieved. Our finding will provide a guidance for the development of flexible laser displays and laser illumination devices.

ConspectusIn the past decade, micro/nanoscale lasers have captured broad research interest for their feasibility in advancing the fields of photonics and optoelectronics. Owing to ease of spectral ...

Detecting conformational changes in protein is imperative due to its major role in neurodegenerative disorders. Here, we propose an alternative strategy for monitoring the structural change of proteins based on biological microlasers. Smart responsive protein-based microscale biolasers were constructed by incorporating organic gain medium into the microspheres of silk fibroin via emulsion-solvent evaporation. The lasing characteristic of the biolasers exhibited a sensitive response to the structural transformation of the silk fibroin. With narrowed linewidth, the as-prepared biolasers as sensing signals enable highly sensitive protein conformation detection. These results offer an effective approach to monitoring the protein conformational changes and provide valuable guidance for a better understanding of the relationship between bio-microstructures and their photonic properties.

Metal-organic frameworks (MOFs) have recently emerged as appealing platforms to construct microlasers owing to their compelling characters combining the excellent stability of inorganic materials and processable characters of organic materials. However, MOF microstructures developed thus far are generally composed of multiple edge boundaries due to their crystalline nature, which consequently raises significant scattering losses that are detrimental to lasing performance. In this work, we propose a strategy to overcome the above drawback by designing spherically shaped MOFs microcavities. Such spherical MOF microstructures are constructed by amorphizing MOFs with a topological distortion network through introducing flexible building blocks into the growth environment. With an ultra-smooth surface and excellent circular boundaries, the acquired spherical microcavities possess a Q factor as high as ≈104 and can provide sufficient feedback for high-quality single-mode lasing oscillations. We hope that these results will pave an avenue for the construction of new types of flexible MOF-based photonic components.

Switchable multimode microlasers are of great significance to the development of photonic devices with high integration levels. Herein, we demonstrate an acid/alkaline gas-responsive multimode AIEgen@starch microsphere-based microlaser. The aggregation-induced emission (AIE) active fluorescent dye ASCPI was used as the gain medium in this study. ASCPI was weakly emissive in water but became highly emissive when introduced to a starch microsphere as a guest molecule. The resultant ASCPI@starch microsphere worked well as a typical whispering-gallery-mode microlaser. The laser mode wavelengths were size-dependent. Due to the sensitivity of ASCPI to pH, the output of the microlaser could be switched to a shorter wavelength by acetic acid vapor treatment or a longer wavelength by NH3 vapor treatment. This work will provide useful enlightenment for the rational design of effective switchable lasers using AIE materials with simple preparation procedures.

Lenticular printing technique provides a promising way to realize stereoscopic displays, especially, when microscopic optical structures are integrated into light-emitting materials/devices. Here, we fabricated large-area periodic structures with a spatial resolution at a wavelength scale from hybrid perovskite materials via a space-confined solution growth method. It takes advantages of both high refractive index contrast and high luminescence brightness, which allows the optical modulation on not only the reflection of illumination, but also the light emission from hybrid perovskites. The distributed feedback within these periodic structures significantly improves the degree of polarization and directionality of laser actions while their threshold is also reduced. These findings enable us to present a prototype of lenticular printing laser displays that vary emission colors at different view angles, which may find applications in creating high-resolution and high-contrast holographical images.

Thermally activated delayed-fluorescent (TADF) materials are anticipated to overcome triplet-related losses towards electrically driven organic lasers. Thus far, contributions from triplets to lasing have not yet been experimentally demonstrated owing to the limited knowledge about the excited-state processes. Herein, we experimentally achieve reverse intersystem crossing (RISC)-boosted lasing in organic microspheres with uniformly dispersed TADF emitters. In these materials, triplets are continuously converted to radiative singlets through RISC, giving rise to reduced losses in stimulated emission. The involvement of regenerated singlets in population inversion results in a thermally activated lasing; that is, the lasing intensity increases with increasing temperature, accompanied by accelerated depletion of the excited-state population. Benefiting from the suppression of triplet accumulations by RISC processes, a high-repetition-rate microlaser was achieved.

Micro/nanoscale photonic barcodes based on multicolor luminescent segmented heterojunctions hold potential for applications in information security. However, such multicolor heterojunctions reported thus far are exclusively based on static luminescent signals, thus restricting their application in advanced confidential information protection. Reported here is a strategy to design responsive photonic barcodes with heterobimetallic (Tb3+ /Eu3+ ) metal-organic framework multicolor heterostructures. The spatial colors could be precisely controlled by thermally manipulating the energy-transfer process between the two lanthanides, thus achieving responsive covert photonic barcodes. Also demonstrated is that spatially resolved responsive barcodes with multi-responsive features could be created in a single heterostructure. These findings offer unique opportunities to purposely design highly integrated responsive microstructures and smart devices toward advanced anti-counterfeiting applications.

Tuneable microlasers that span the full visible spectrum, particularly red, green, and blue (RGB) colors, are of crucial importance for various optical devices. However, RGB microlasers usually operate in multimode because the mode selection strategy cannot be applied to the entire visible spectrum simultaneously, which has severely restricted their applications in on-chip optical processing and communication. Here, an approach for the generation of tuneable multicolor single-mode lasers in heterogeneously coupled microresonators composed of distinct spherical microcavities is proposed. With each microcavity serving as both a whispering-gallery-mode (WGM) resonator and a modulator for the other microcavities, a single-mode laser has been achieved. The colors of the single-mode lasers can be freely designed by changing the optical gain in coupled cavities owing to the flexibility of the organic materials. Benefiting from the excellent compatibility, distinct color-emissive microspheres can be integrated to form a heterogeneously coupled system, where tuneable RGB single-mode lasing is realized owing to the capability for optical coupling between multiple resonators. Our findings provide a comprehensive understanding of the lasing modulation that might lead to innovation in structure designs for photonic integration., Lasers: Generating all colors in a better mode A system for improved control over laser light emission generates any frequency in the visible spectrum, creating what is termed a red, green and blue (RGB) laser, in the advantageous form known as ‘single-mode’ lasing. Most RGB lasers deliver ‘multimode’ signals, in which the light is distributed among several wavelengths around the central most intense and desired wavelength. The preferable single-mode RGB lasing has been developed by researchers in China, led by Yong Sheng Zhao at the Institute of Chemistry of the Chinese Academy of Sciences in Beijing. It uses closely coupled organic (carbon compound-based) microcavities as the regions in which the light is generated and amplified, delivering single frequencies of tunable laser light. This innovation will open new possibilities for using RGB lasing in optical processing and communications systems.

Miniaturized lasers with high spectral purity and wide wavelength tunability are crucial for various photonic applications. Here we propose a strategy to realize broadband-tunable single-mode lasing based on a photoisomerization-activated intramolecular charge-transfer (ICT) process in coupled polymer microdisk cavities. The photoisomerizable molecules doped in the polymer microdisks can be quantitatively transformed into a kind of laser dye with strong ICT character by photoexcitation. The gain region was tailored over a wide range through the self-modulation of the optically activated ICT isomers. Meanwhile, the resonant modes shifted with the photoisomerization because of a change in the effective refractive index of the polymer microdisk cavity. Based on the synergetic modulation of the optical gain and microcavity, we realized the broadband tuning of the single-mode laser. These results offer a promising route to fabricate broadband-tunable microlasers towards practical photonic integrations.

A universal approach is demonstrated for realizing dual-wavelength lasing in organic core-shell structured microlaser arrays, which show great promise in serving as all-color laser display panels. By alternately printing hydrophilic and hydrophobic laser dye solutions on preprocessed substrates, precisely patterned core-shell heterostructure arrays were obtained. The spatially separated core and shell independently function as optical resonators to support dual-wavelength tunable lasing in each heterostructure. Such a general method enables to flexibly control the lasing wavelength of the core-shell microlasers across a wide spectral range by systematically designing the gain media. Using as-prepared microlaser arrays as display panels, full-color laser displays were achieved with a color gamut much larger than that of standard RGB space. These results provide insights for design concepts and device construction for novel optoelectronic applications.

Metal-organic frameworks (MOFs) are an emerging kind of laser material, yet they remain a challenge in the controlled fabrication of crystal nanostructures with desired morphology for tuning their optical microcavities. Herein, the shape-engineering of pure MOF microlasers was demonstrated based on the coordination-mode-tailored method. The one-dimensional (1D) microwires and 2D microplates were selectively fabricated through changing the HCl concentration to tailor the coordination modes. Both the single-crystalline microwires and microplates with strong optical confinement functioned as low-threshold MOF microlasers. Moreover, distinct lasing behaviors of 1D and 2D MOF microcrystals confirm a typical shape-dependent microcavity effect: 1D microwires serve as Fabry-Pérot (FP) resonators, and 2D microplates lead to the whispering-gallery-mode (WGM) microcavities. These results provide a special pathway for the exploitation of MOF-based micro/nanolasers with on-demand functions.

2D anisotropic transport of photons/electrons is crucial for constructing ultracompact on-chip circuits. To date, the photons in organic 2D crystals usually exhibit the isotropic propagation, and the anisotropic behaviors have not yet been fully demonstrated. Now, an orientation-controlled photon-dipole interaction strategy was proposed to rationally realize the anisotropic and isotropic 2D photon transport in two co-crystal polymorph microplates. The monoclinic microplate adopts a nearly horizontal transition dipole moment (TDM) orientation in 2D plane, exhibiting anisotropic photon-dipole interactions and thus distinct re-absorption waveguide losses for different 2D directions. By contrast, the triclinic plate with a vertical TDM orientation, shows 2D isotropic photon-dipole interactions and thus the same re-absorption losses along different directions. Based on this anisotropy, a directional signal outcoupler was designed for the directional transmission of the real signals.

The invention and development of the laser have revolutionized science, technology, and industry. Metal halide perovskites are an emerging class of semiconductors holding promising potential in further advancing the laser technology. In this Review, we provide a comprehensive overview of metal halide perovskite lasers from the viewpoint of materials chemistry and engineering. After an introduction to the materials chemistry and physics of metal halide perovskites, we present diverse optical cavities for perovskite lasers. We then comprehensively discuss various perovskite lasers with particular functionalities, including tunable lasers, multicolor lasers, continuous-wave lasers, single-mode lasers, subwavelength lasers, random lasers, polariton lasers, and laser arrays. Following this a description of the strategies for improving the stability and reducing the toxicity of metal halide perovskite lasers is provided. Finally, future research directions and challenges toward practical technology applications of perovskite lasers are provided to give an outlook on this emerging field.

Surface plasmon polaritons (SPPs) are crucial for the development of next generation information and communication technologies. However, the ohmic losses inherent to all plasmonic devices seriously limit their practical application in on-chip photonic communications. Here, loss compensation of SPPs and their application in photonic logic processing was demonstrated in rationally designed organic/silver nanowire heterostructures. The heterostructures were synthesized by inserting silver nanowires (AgNWs) into crystalline organic microwires, which served as a microscale optical gain medium. These heterostructures with large organic/metal interfacial areas ensured the efficient energy transfer from excitons to SPPs. Gain for subwavelength SPPs in the heterostructure was achieved through stimulated emission of strongly confined SPPs. Furthermore, cascade gain was performed to realize basic nanoscale photonic devices, such as Boolean logic units. The results would pave an alternative avenue to incorporating SPP-enhanced devices into hybrid photonic circuitry.

In recent years, metal-organic frameworks (MOFs) have been attracting ever more interest owing to their fascinating structures and widespread applications. Among the optoelectronic materials, luminescent MOFs (LMOFs) have become one of the most attractive candidates in the fields of optics and photonics thanks to the unique characteristics of their frameworks. Luminescence from MOFs can originate from either the frameworks, mainly including organic linkers and metal ions, or the encapsulated guests, such as dyes, perovskites, and carbon dots. Here, we systematically review the recent progress in LMOFs, with an emphasis on the relationships between their structures and emission behaviour. On this basis, we comprehensively discuss the research progress and applications of multicolour emission from homogeneous and heterogeneous structures, host-guest hybrid lasers, and pure MOF lasers based on optically excited LMOFs in the field of micro/nanophotonics. We also highlight recent developments in other types of luminescence, such as electroluminescence and chemiluminescence, from LMOFs. Future perspectives and challenges for LMOFs are provided to give an outlook of this emerging field. We anticipate that this article will promote the development of MOF-based functional materials with desired performance towards robust optoelectronic applications.

Circularly polarized light (CPL) detection has emerged as a key technology for various optoelectronics. Chiral hybrid perovskites (CHPs) that combine CPL‐sensitive absorption induced by chiral organic ligands and superior photoelectric properties of perovskites are promising candidates for direct CPL detection. To date, most of the CHP detectors are made up of polycrystalline thin‐film, which results in a rather limited discrimination of CPL due to the existence of redundant impurities and intrinsic defect states originating from rapid crystallization process. Here, it is developed a direct CPL detector with high photocurrent and polarization selectivity based on low‐defect CHP single‐crystal nanowire arrays. Large‐scale CHP nanowires are obtained through a micropillar template‐assisted capillary‐bridge rise approach. Thanks to the high crystallinity and ordered crystallographic alignment of these arrays, a CPL photodetector with high light on/off ratio of 1.8 × 104, excellent responsivity of 1.4 A W−1, and an outstanding anisotropy factor of 0.24 for photocurrent has been achieved. These results would provide useful enlightenment for direct CPL detection in high‐performance chiral optoelectronics., An efficient circularly polarized light (CPL) detector is demonstrated with large‐scale chiral hybrid perovskite (CHP) nanowire arrays. Based on the high photocurrent and polarization selectivity of CHP single‐crystals, high‐performance CPL detectors with high light on/off ratio and excellent polarization distinguishability through arranging such single‐crystalline CHP nanowires into low‐defect arrays are achieved.

Multicomponent crystallization is universally important in various research fields including materials science as well as biology and geology, and presents new opportunities in crystal engineering. This process includes multiple kinetic and thermodynamic events that compete with each other, wherein "external triggers" often help the system select appropriate pathways for constructing desired structures. Here we report an unprecedented finding that a lattice strain accumulated with the growth of a crystal serves as an "internal trigger" for pathway selection in multicomponent crystallization. We discovered a "spontaneous" crystal transition, where the kinetically preferred layered crystal, initially formed by excluding the pillar component, carries a single dislocation at its geometrical center. This crystal "spontaneously" liberates a core region to relieve the accumulated lattice strain around the dislocation. Consequently, the liberated part becomes dynamic and enables the pillar ligand to invade the crystalline lattice, thereby transforming into a thermodynamically preferred pillared-layer crystal.

Organic composite materials have been attracting extensive research interest for light‐emitting applications. A wide variety of luminescent organic composite materials have been synthesized, which are of great significance for both the investigation of basic photophysics and the realization of high‐performance photonic devices. Function‐oriented syntheses of luminescent organic composite materials rely on the understanding and manipulating of molecular excited states. In this review, we focus on the discussion about the structure design and dynamics modulation of the electronic excited states in the organic composite materials. The excited‐state structures and dynamics involve singlet/triplet levels, vibronic transition, charge transfer, and energy transfer, and so on, while the light‐emitting behaviors include fluorescence, phosphorescence, persistent luminescence, electroluminescence, and lasing. We aim to give insight into the relationship between light‐emitting properties and excited states of organic composite materials, which is beneficial for reaching higher tiers of design and applications of luminescent organic composite materials.

Metal-organic frameworks (MOFs) heterostructures with domain-controlled emissive colors have shown great potential for achieving high-throughput sensing, anti-counterfeit and information security. Here, a strategy based on steric-hindrance effect is proposed to construct lateral lanthanide-MOFs (Ln-MOFs) epitaxial heterostructures, where the channel-directed guest molecules are introduced to rebalance in-plane and out-of-plane growth rates of the Ln-MOFs microrods and eventually generate lateral MOF epitaxial heterostructures with controllable aspect ratios. A library of lateral Ln-MOFs heterostructures are acquired through a stepwise epitaxial growth procedure, from which rational modulation of each domain with specific lanthanide doping species allows for definition of photonic barcodes in a two-dimensional (2D) domain with remarkably enlarged encoding capacity. The results provide molecular-level insight into the use of modulators in governing crystallite morphology for spatially assembling multifunctional heterostructures.

3D laser displays play an important role in next-generation display technologies owing to the ultimate visual experience they provide. Circularly polarized (CP) laser emissions, featuring optical rotatory power and invariability under rotations, are attractive for 3D displays due to potential in enhancing contrast ratio and comfortability. However, the lack of pixelated self-emissive CP microlaser arrays as display panels hinders the implementation of 3D laser displays. Here, full-color 3D laser displays are demonstrated based on CP lasing with inkjet-printed cholesteric liquid crystal (CLC) arrays as display panels. Individual CP lasers are realized by embedding fluorescent dyes into CLCs with their left-/right-handed helical superstructures serving as distributed feedback microcavities, bringing in ultrahigh circular polarization degree values (gem = 1.6). These CP microlaser pixels exhibit excellent far-field color-rendering features and a relatively large color gamut for high-fidelity displays. With these printed CLC red-green-blue (RGB) microlaser arrays serving as display panels, proof-of-concept full-color 3D laser displays are demonstrated via delivering images with orthogonal CP laser emissions into one's left and right eyes. These results provide valuable enlightenment for the development of 3D laser displays.

Anticounterfeiting labels based on physical unclonable functions (PUFs) exhibit high security with unreplicable code outputs, making them an ideal platform to realize unbreakable anticounterfeiting. Although various schemes are proposed for PUF labels, the utilization of natural randomness suffers from unpredictable signal extraction sites, which poses a challenge to efficient and convenient authentication for practical anticounterfeiting applications. Here, a covert optical PUF-based cryptographic protocol from silk protein-based microlaser (SML) arrays that possess hidden randomness of lasers for unclonable lasing signals as well as a defined location for efficient identification is proposed. The initial SMLs are patterned by casting laser dye-doped regenerated silk fibroin solution, resulting in a uniform microlaser array with regulated positions. With the SML array as substrate, random methanol microdroplets are stochastically sprayed on the SML array, which eventually induces uneven lasing signal changes of the patterned microlasers. The treated SML array possesses the deterministic readout sites of laser signals and unrepeatable signal distribution characteristics, which can guarantee efficient authentication and high security when serving as an anticounterfeiting label.

We present herein an innovative host–guest method to achieve induced molecular chirality from an achiral stilbazolium dye (DSM). The host–guest system is exquisitely designed by encapsulating the dye molecule in the molecule-sized chiral channel of homochiral lanthanide metal–organic frameworks (P-(+)/M-(−)-TbBTC), in which the P- or M-configuration of the dye is unidirectionally generated via a spatial confinement effect of the MOF and solidified by the dangling water molecules in the channel. Induced chirality of DSM is characterized by solid-state circularly polarized luminescence (CPL) and micro-area polarized emission of DSM@TbTBC, both excited with 514 nm light. A luminescence dissymmetry factor of 10−3 is obtained and the photoluminescence quantum yield (PLQY) of the encapsulated DSM in DSM@TbTBC is ∼10%, which is close to the PLQY value of DSM in dilute dichloromethane. Color-tuning from green to red is achieved, owing to efficient energy transfer (up to 56%) from Ln3+ to the dye. Therefore, this study for the first time exhibits an elegant host–guest system that shows induced strong CPL emission and enables efficient energy transfer from the host chiral Ln-MOF to the achiral guest DSM with the emission color tuned from green to red., Homochiral Ln-MOFs are synthesized to encapsulate achiral dyes to induce strong circularly polarized luminescence with a luminescence dissymmetry factor of 10−3.

Porous organic frameworks have emerged as the promising platforms to construct tunable microlasers. Most of these microlasers are achieved from metal-organic frameworks via meticulously accommodating the laser dyes with the sacrifice of the pore space, yet they often suffer from the obstacles of either relatively limited gain concentration or sophisticated fabrication techniques. Herein, we reported on the first hydrogen-bonded organic framework (HOF) microlasers with color-tunable performance based on conformation-dependent stimulated emissions. Two types of HOF microcrystals with the same gain lumnogen as the building block were synthesized via a temperature-controlled self-assembly method. The distinct frameworks offer different conformations of the gain building block, which lead to great impacts on their conjugation degrees and excited-state processes, resulting in remarkably distinct emission colors (blue and green). Accordingly, blue/green-color lasing actions were achieved in these two types of HOFs based on well-faceted assembled wire-like cavities. These results offer a deep insight on the exploitation of HOF-based miniaturized lasers with desired nanophotonics performances.

Near-infrared (NIR) microlasers play a significant role in telecommunication and biomedical tissue imaging. However, it remains a big challenge to realize NIR microlasers because of the difficulty in preparing highly efficient NIR luminescent materials and perfect optical resonators. Here, we propose a molecular design strategy to creatively realize the first spiropyrane (SP)-based NIR microlasers with low threshold from self-assembled microsphercial caps. The tetraphenylethylene (TPE) moiety with a highly twisted conformation provides a large free volume to facilitate the photoisomerization process of SP and enhance NIR emission of merocyanine in the solid state. Moreover, self-assembled TPE-SP microsphercial caps simultaneously serve as gain media and resonant microcavities, providing optical gain and feedback for NIR laser oscillations with a low threshold (3.68 μJ/cm

Micro/nanoscale multicolor barcodes with unique identifiability and a small footprint play significant roles in applications such as multiplexed labeling and tracking systems. Now, a strategy is reported to design multicolor photonic barcodes based on 1D Ln-MOF multiblock heterostructures, where the domain-controlled emissive colors and different block lengths constitute the fingerprint of a corresponding heterostructure. The excellent heteroepitaxial growth characteristics of MOFs enable the effective modulation of the coding structures, thereby remarkably increasing the encoding capacity. The as-prepared multicolor barcodes enable an efficient authentication and exhibit great potential in fulfilling the functions of anti-counterfeiting, information security, and so on. The results will pave an avenue to novel hybrid MOFs for optical data recording and security labels.

The structural flexibility of hybrid perovskite materials allows for phase transition and consequently thermochromic properties. Here we investigate the thermochromic performance in a series of copper-based layered perovskites with organic cations having different alky chain lengths. Their transition temperature is found to be dependent on the organic cations due to molecular motion and hydrogen bond interaction, providing possibilities to prepare thermochromic semiconductors near room temperature for smart window applications.

The monolithic incorporation of electrical and optical components is critically important for achieving high-speed on-chip signal processing, but yet hard to satisfy the explosive growth in the demands on bandwidth and information density. Three-dimensional (3D) circuits, which are desirable for their improved performance in data handling, are ideal candidates to simultaneously promise high-capacity computing with improved speed and energy efficiency. In such highly integrated circuits, however, the selective electrical modulation of light signals is still difficult to achieve owing to the lack of controllable integration of micro-scale optical functional devices and modulation units. In this work, we demonstrate an electrically modulated microlaser module on a 3D-integrated microsystem composed of a dye-doped polymeric microcavity and an underneath microscale electrical heating circuit. The lasing mode was modulated based on electrical heating-assisted thermo-optic response of the polymeric matrices, which were further fabricated into coupled microdisks, yielding wavelength-tunable single-mode microlasers with selective electrical modulation. On this basis, a prototype of electrically controlled microlaser module with reduced signal cross-talk was achieved. The results will provide a useful enlightenment for the rational design of novel tunable optical devices with more complicated functionalities under far-field regulation, paving the way for the on-chip optoelectronic integration.

Organic polymorphs with tunable luminescence are crucial in developing organic luminescent materials, but the regulation of molecular packing modes and intermolecular interactions in organic crystals remains a challenge. Here, we report three triphenylamine–benzothiazole (TZ) compounds by systematically changing the substituents, resulting in different crystal emission characteristics. The polymorphs of blue emission (TZ-1B) and cyan emission (TZ-1C) crystals are obtained by controlling the crystallization conditions, however, we could not obtain organic polymorphs of TZ-2 or TZ-3 in various solvent systems. By molecular systems and detailed single crystal analysis, it is found that appropriate substituents play a key role in manipulating the intermolecular interactions and the molecular packing modes to affect the optical properties of organic crystals. Moreover, TZ-1C exhibits blue-shifted mechanochromism, while TZ-1B does not. More importantly, TZ-1B exhibits a lasing emission at 454 nm with a low threshold and a high cavity quality factor. TZ-1C exhibits amplified spontaneous emission (ASE) at 462 nm. Thus, the molecular systems provide a reasonably potent molecular strategy to understand the molecular packing structure–fluorescence property relationship.

The controlled construction of organic heterostructured architectures derived from molecules with similar nucleation thresholds and concentrations has been rare and remains a great challenge. Herein, we report a sequential epitaxial growth to synthesize dual-color-emitting organic heterostructures with 9,10-bis(phenylethynyl)anthracene (BPEA) microwire trunks and tris-(8-hydroxyquinoline)aluminium (Alq3) microstructure branches by an anti-solvent induced sequential crystallization strategy. During the epitaxial growth process, the hydrogen-bonding interactions of the anti-solvent and solvent cause a large change in the solubility and crystallization rate of BPEA and Alq3 molecules in the mixed system, which facilitates sequential crystallization of organic molecule pairs with similar nucleation thresholds and concentrations into desired heterostructures by manipulating the synergism of anti-solvents and solvents. The Förster resonant energy transfer process in heterostructures could be modulated by varying the structure of heterostructures, such as the shape, amount and angles of the branches. The present synthesis strategy provides a unique insight into the detailed formation mechanism of complex organic heterostructures, further guiding the construction of more functional heterostructure materials.

Summary Electrically pumped organic lasers have been eagerly sought for several decades, although they have not been fully demonstrated yet. Recently, impressive progresses have been made with respect to molecular design, theoretical prediction, and device fabrication for light-emitting organic semiconductors. In this perspective, we outline the key issues of balanced optical gain, carrier mobility, and excitonic losses as well as other challenges associated with electrical pump of organic lasers after examining the breakthroughs made in recent efforts. Then, we provide a concise overview of several potential solutions to the challenges from the viewpoint of lasing principle by exploring the relationship between lasing emissions and molecular structures, device engineering, and exciton dynamics, which might stand out as the most promising way toward the pursuit of electrically driven lasing with organic semiconductors.

Organic cocrystals with unique energy-level structures are potentially a new class of materials for the development of versatile solid-state lasers. However, till now, the stimulated emission in cocrystal materials remains a big challenge possibly because of the nonradiative charge-transfer (CT) transitions. Here, for the first time, we report organic cocrystal microlasers constructed by simultaneously tailoring the energy levels and cavity structures based on the intermolecular halogen-bonding interactions. The intermolecular interactions triggered different self-assembly processes, resulting in distinct types of high-quality resonant microcavities. More importantly, the halogen-bonding interactions alleviated intermolecular CT and thus brought about a favorable four-level energy structure for the population inversion and tunable lasing in the cocrystals.

Organic-inorganic metal-halide materials (OIMMs) with zero-dimensional (0D) structures offer useful optical properties with a wide range of applications. However, successful examples of 0D structural OIMMs with well-defined optical performance at the micro-/nanometer scale are limited. We prepared one-dimensional (1D) (DTA)2 SbCl5 ⋅DTAC (DTAC=dodecyl trimethyl ammonium chloride) single-crystal microrods and 2D microplates with a 0D structure in which individual (SbCl5 )2- quadrangular units are completely isolated and surrounded by the organic cation DTA+ . The organic molecular unit with a long alkyl chain (C12 ) and three methyl groups enables microrod and -plate formation. The single-crystal microrods/-plates exhibit a broadband orange emission peak at 610 nm with a photoluminescence quantum yield (PLQY) of ca. 90 % and a large Stokes shift of 260 nm under photoexcitation. The broad emission originates from self-trapping excitons. Spatially resolved PL spectra confirm that these microrods exhibit an optical waveguide effect with a low loss coefficient (0.0019 dB μm-1 ) during propagation, and linear polarized photoemission with a polarization contrast (0.57).

Synthesis of novel mesoscopic semiconductor architectures continually generates new photonic knowledge and applications. However, it remains a great challenge to synthesize semiconductor microcrystals with smoothly curved surfaces owing to the crystal growth anisotropy. Here, a superkinetic crystal growth method is developed to synthesize 2D oval organic semiconductor microcrystals. The solid source dispersion induces an exceptionally large molecular supersaturation for vapor deposition, which breaks the crystal growth anisotropy. The synthesized stadium-shaped organic semiconductor microcrystals naturally constitute fully chaotic optical microresonators. They support low-threshold lasing on high-quality-factor scar modes localized near the stadium boundary and directional laser emission assisted by the chaotic modes. These results will reshape the understanding of the crystal growth theory and provide valuable guidance for crystalline photonic materials design.

Information encryption and decryption have attracted particular attention; however, the applications are frequently restricted by limited coding capacity due to the indistinguishable broad photoluminescence band of conventional stimuli-responsive fluorescent materials. Here, we present a concept of confidential information encryption with photoresponsive liquid crystal (LC) lasing materials, which were used to fabricate ordered microlaser arrays through a microtemplate-assisted inkjet printing method. LC microlasers exhibit narrow-bandwidth single-mode emissions, and the wavelength of LC microlasers was reversibly modulated based on the optical isomerization of the chiral dopant in LCs. On this basis, we demonstrate phototunable information authentication on LC microlaser arrays using the wavelength of LC microlasers as primary codes. These results provide enlightenment for the implementation of microlaser-based cryptographic primitives for information encryption and anticounterfeiting applications.

Laser displays, which offer wide achievable color gamut and excellent color rendering, have emerged as a promising next-generation display technology. Constructing display panels composed of pixelated microlaser arrays is of great significance for the actualization of laser displays in the flat-panel sector. Here, we report microscale light-emitting electrochemical cell (LEC) arrays that operate as both optically pumped lasers and electroluminescence devices, which can be applied as self-emissive panels for high quality displays. Optically pumped red, green, and blue laser emissions were achieved in individual circular microcells consisting of corresponding conjugated polymers and electrolytes, suggesting that the microstructures can act as resonators for coherent outputs. As-prepared microstructures possess a narrowed recombination region, which dramatically increases the current density by 3 orders of magnitude under pulsed operation, compared with the corresponding thin-film devices, representing a promising solution-processed device platform for electrical pumping. Under programmable electrical excitation, both static and dynamic displays were demonstrated with such microscale LEC arrays as display panels. The prominent performance of the demonstrated structures (microlaser arrays embedded in LEC devices) provide us deep insight into the concepts and device constructions of electrically driven laser displays.

Constructing three-dimensional (3D) metamaterials from functional nanoparticles endows them with emerging collective properties tailored by the packing geometries. Herein, we report 3D supercrystals self-assembled from upconversion nanorods (NaYF4:Yb,Er NRs), which exhibit both translational ordering of NRs and orientational ordering between constituent NRs in the superlattice (SL). The construction of 3D reciprocal space mappings (RSMs) based on synchrotron-based X-ray scattering measurements was developed to uncover the complex structure of such an assembly. That is, the two main orthogonal sets of hexagonal close-packing (hcp)-like SLs share the [110]SL axis, and NRs within the SL possess orientational relationships of [120]NR//[100]SL, [210]NR//[010]SL, and [001]NR//[001]SL. Notably, these supercrystals containing well-aligned NRs exhibit collectively anisotropic upconversion fluorescence in two perpendicular directions. This study not only demonstrates novel crystalline superstructures and functionality of NR-based 3D assemblies but also offers a unique tool for deciphering a wide range of complex nanoparticle supercrystals.

Halide perovskites have shown tremendous potential for next-generation flat-panel laser displays due to their remarkable optoelectronic properties and outstanding material processability; however, the lack of a general approach for the fast growth of perovskite laser arrays capable of electrical operations impedes actualization of their display applications. Herein, a universal and robust wettability-guided screen-printing technique is reported for the rapid growth of large-scale multicolor perovskite microdisk laser arrays, which can serve as laser display panels and further be used to realize current-driven displays. The perovskite microlasers are precisely defined with controlled physical dimensions and spatial locations by such a printing strategy, and each perovskite microlaser serves as a pixel of a display panel. Moreover, the screen-printing procedure is highly compatible with light-emitting diode (LED) device architectures, which is favorable for the mass production of micro-LED arrays. On this basis, a prototype of a current-driven display is demonstrated with desired functionalities. The outstanding performance and feasible fabrication of screen-printed perovskite microlaser arrays embedded in LEDs provide deep insights into the concepts and device architectures of electrically driven laser display technology.

Organic materials are an important class of gain media for fabricating miniaturized lasers because they combine fabrication simplicity with wide spectral coverage and tunability. However, progress toward near-infrared (NIR) organic solid-state lasers has been limited because of serious nonradiative processes originating from the severe intermolecular interaction in the condensed state. Here, we develop a strategy to realize room-temperature NIR microscale lasers through encapsulating organic dyes into the cavities of metal-organic frameworks (MOFs). The spatial confinement of the dye molecules within the MOF pores contributes to suppressing the multiple nonradiative processes (i.e., aggregation-caused quenching and exciton-exciton annihilation). This results in a much higher radiative efficiency and thus much easier population inversion and low-threshold NIR lasing. Furthermore, the lasing wavelength can be further expanded based on the tailorable energy levels of the dye molecules. The results will provide useful enlightenment for the development of miniaturized NIR laser sources for new photonic applications.

Microscale laser switches have been playing irreplaceable roles in the development of photonic devices with high integration levels. However, it remains a challenge to switch the lasing wavelengths across a wide range due to relatively fixed energy bands in traditional semiconductors. Here, we report a strategy to switch the lasing wavelengths among multiple states based on a proton-controlled intramolecular charge-transfer (ICT) process in organic dye-doped flexible microsphere resonant cavities. The protonic acids can effectively bind onto the ICT molecules, which thus enhance the ICT strength of the dyes and lead to a red-shifted gain behavior. On this basis, the gain region was effectively modulated by using acids with different proton-donating ability, and as a result, laser switching among multiple wavelengths was achieved. The results will provide guidance for the rational design of miniaturized lasers with performances based on the characteristic of organic optoelectronic materials.

Micro/nanoscale lasers that can deliver intense coherent light signals at (sub)wavelength scale have attracted great interest because of their promising applications ranging from on-chip information processing to high-throughput sensing. Compared with traditional inorganic materials, organic materials are ideal platforms to construct high performance microlasers, mainly because of their superiority in flexibly assembled structures for high-quality microcavities and abundant excited-state processes with large active cross sections for high gain emissions. This review begins with an overview of the research evolution of organic microlasers in terms of microcavity resonators and energy-level gain. Then a series of strategies to tailor the microcavity structures and excited-state dynamics of organic materials for the modulation of lasing performances are highlighted. Subsequently, we present the design and construction of organic-microlaser-based hybrid structures with advanced photonic functionalities. In the following part, we introduce their applications in chemical sensing, biosensing and integrated nanophotonics. Finally, we provide our outlook on the current challenges as well as the future direction of organic microlasers. It is anticipated that this review will provide inspiration for the development of miniaturized lasers with desired performances by tailoring of excited-state processes and microcavity structures toward practical applications.

Two-dimensional (2D) layered materials, with large second-order nonlinear susceptibility, have received much scientific interest due to their potential applications in nonlinear optical devices. However, the atomic thickness of 2D layered materials leads to poor field confinement and weak light–matter interaction at the nanoscale, resulting in low nonlinear conversion efficiency. Here, 2D pyramid-like multilayer (P-multilayer) layered structures are fabricated for efficient edge second-harmonic generation (SHG) based on the enhanced light–matter interaction in whispering-gallery mode (WGM) cavities. The P-multilayer 2D layered materials, where the basal planes shrink gradually from the bottom to the top layers, exhibit efficient edge SH radiation due to the partial destructive interference of nonlinear polarizations between the neighboring atomic layers. Moreover, the well-defined 2D plate-like triangle morphology of P-multilayer WS2 forms a WGM resonance cavity, which results in enhanced light–matter int...

Low-dimensional organic materials have given rise to tremendous interest in optoelectronic applications, owing to their controllable photonic properties. However, the controlled-synthesis approaches for organic nano-/micro-architectures are very difficult to attain, because the weak interaction (van der Waals force) between the organic molecules cannot dominate the kinetic process of crystal growth. We report a simple method, which involves selective adhesion to the organic crystal plane by hydrogen-bonding interaction for modulating the crystal growth process, which leads either to the self-assembly of one organic molecule into two-dimensional (2D) microsheets with an obvious asymmetric light propagation or one-dimensional (1D) microrods with low propagation loss. The method of tailoring the structures and photonic properties for fabricating different micro-structures would provide enlightenment for the development of tailor-made mini-sized devices for photonic integrated circuits.

Directing the architecture of complex organic nanostructures is desirable and still remains a challenge in areas of materials science due to their structure-dependent collective optoelectronic properties. Herein, we demonstrate a simple and versatile solution strategy that allows surface tension to drive low-dimensional nanostructures to aggregate into complex structures via a lab in a droplet technique. By selecting a suitable combination of a solvent and an anti-solvent with controllable surface tension difference, the droplets can be automatically cracked into micro-droplets, which provides an aggregation force directed toward the centre of the droplet to drive the low-dimensional building blocks to form the special aggregations during the self-assembly process. This synthetic strategy has been shown to be universal for organic materials, which is beneficial for further optimizing the optoelectronic properties. These results contribute to gaining an insightful understanding on the detailed growth mechanism of complex organic nanostructures and greatly promoting the development of organic nanophotonics.

Ultracompact coherent light sources with broadband wavelength tunability and subwavelength optical waveguiding have attracted extensive attention due to their potential applications ranging from multicolor detection to multiband on-chip photonic communication. Metal–dielectric nonlinear structures, which comprise nonlinear dielectric materials and metal films, have been widely used to generate nanoscale broadband tunable coherent light sources through the second-harmonic generation process below the diffraction limit. However, restricted by high ohmic losses at the metal–dielectric surface, subwavelength propagation of SHG signals with low loss remains a big challenge. Here, a novel strategy is utilized to reduce the propagation loss of SHG signals based on the coupling between the waveguide mode and plasmonic mode in a hybrid plasmonic waveguide (HPW). The generated hybrid plasmonic mode in the HPW exhibits strong optical confinement around the nonlinear dielectric and insulating gap, which is beneficial for minimizing the ohmic losses at the metal–dielectric interface and enhancing the light–matter interaction below the diffraction limit. Moreover, under the phase matching condition, the propagation loss of SHG signals is partially compensated for by the frequency conversion of the fundamental wave (FW) through the SHG process. As a result, low propagation loss of enhanced SHG signals at a subwavelength scale is realized in HPWs.

Solid-state fluorescent materials have attracted a surge of interest in recent years due to their wide applications in the fields of photoelectric devices, memory storage and fluorescent probes. Compared to the synthesis of new molecules, exploring new properties in known molecules is a facile approach to obtain functionalized fluorescent materials. In this report, we systematically explored the solid-state photoluminescence properties and applications of 7-(diethylamino)coumarin-3-aldehyde (DCA) and 7-(diethylamino)coumarin-3-carboxylic acid (DCCA). Both fluorophores exhibited a special concentration-dependent emission effect. They displayed polymorphism dependent solid-state emission and single crystal analysis revealed that enhanced overlap between neighbouring molecules resulted in a red-shifted emission. Crystal-to-crystal transformation has also been achieved for both DCA and DCCA by employing an external thermal treatment. In addition, the solid powder of DCA and DCCA displayed fluorescence response to HCl and NH3 gas with high sensitivity. Furthermore, 1D micromaterials were assembled for both fluorophores and DCA exhibited outstanding optical waveguide behavior.