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The large library of organic dye molecules offers almost infinite possibilities for laser design, but still faces a great challenge in achieving pure dye aggregate lasers due to intermolecular quenching. Here, we report a kinetically controlled molecular self-assembly strategy to synthesize unconventional dye microcrystals for lasing. By increasing temperature, the dye self-assembly is transformed from thermodynamic to kinetic control. Unlike the thermodynamic microcrystal products incapable of lasing due to intermolecular charge-transfer-mediated excimer formation, the kinetic dye microcrystals have large intermolecular distances and weak intermolecular interactions, supporting highly efficient intramolecular charge-transfer monomer emission and low-threshold lasing. This work demonstrates single-crystal dye lasers, promising to unleash the full potential of laser dyes in solid-state lasers.

Owing to outstanding optoelectronic properties, halide perovskites are great candidates for novel laser display applications. However, the realization of their practical flat-panel display applications is challenging because of the incapacity to controllably assemble different halide perovskite microlaser arrays onto an identical substrate as pixelated full-color panels due to intrinsic fragile crystal lattices. Here, perovskite red-green-blue (RGB) microdisk arrays are reported, acting as flat-panels for full-color laser displays. A universal screen-overprinting technology is developed to integrate full-color perovskite microdisk arrays on a prepatterned template, which is on the basis of wet-solute-chemical dynamics involving a combination of surface tailoring and solvent selection. Via such an overprinting method, perovskite RGB microlaser matrices with precise localizations and well-defined dimensions were fabricated on an identical substrate, and each set of RGB microlaser served as a pixel for full-color display panels. On this basis, static and dynamic laser displays have been demonstrated with as-prepared full-color panels. These results will provide novel design concepts and device structures for future full-color laser display applications.

Porous organic materials (POMs) have shown great potential for fabricating tunable miniaturized lasers. However, most pure-POM micro/nanolasers are achieved via coordination interactions, during which strong charge exchanges inevitably destroy the intrinsic gain property and even lead to optical quenching, hindering their practical applications. Herein, we reported on an approach to realize hydrogen-bonded organic framework (HOF)-based

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) 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.

Herein, we demonstrated a steric-hindrance-controlled laser switch in pure metal-organic framework (MOF) microcrystals. The well-faceted MOF microwires with aggregation-induced emission (AIE) lumnogens as linkers function as typical Fabry-Pérot microlasers. The steric hindrance around the AIE linkers can be reduced by the loss of guest molecules, which lead to the enhanced rotation of linkers with red-shifted gain behavior. On this basis, the gain region was readily switched through changing the steric hindrance via the desorption/adsorption of guests. As a result, the reversible switching of the dual-wavelength lasing from MOF microwires was achieved. The results provide a promising route to the development of versatile micro-/nanolasers with desired applications.

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

[K(dibenzo-18-crown-6)]+ (KC) cations are used for cocrystallization with manganese halides, producing isostructural single crystals of organic–inorganic hybrid complexes, [K(dibenzo-18-crown-6)]2M...

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.

In this work, we demonstrate a stimulated emission-controlled photonic transistor on a single organic triblock nanowire composed of alternate energy donor and acceptor. The population of acceptor excitons was engineered by energy transfer to achieve enhanced fluorescence, which was further amplified by the stimulated emission of the donor and the optical feedback in the nanowire microcavities, yielding a remarkable nonlinear amplification of the acceptor emission. On this basis, a prototype of photonic transistor with high nonlinear gain at very low pump energy was achieved. The results will provide a useful enlightenment for the rational design of novel all-optical switches with desired performances.

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.

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...

The excitation of surface plasmons by optical emitters based on exciton-plasmon coupling is important for plasmonic devices with active optical properties. It has been theoretically demonstrated that the orientation of exciton dipole can significantly influence the coupling strength, yet systematic study of the coupling process in nanostructures is still hindered by the lack of proper material systems. In this work, we have experimentally investigated the orientation-dependent exciton-plasmon coupling in a rationally designed organic/metal nanowire heterostructure system. The heterostructures were prepared by inserting silver nanowires into crystalline organic waveguides during the self-assembly of dye molecules. Structures with different exciton orientations exhibited varying coupling efficiencies. The near-field exciton-plasmon coupling facilitates the design of nanophotonic devices based on the directional surface plasmon polariton propagations.

All-color subwavelength output of lasers was demonstrated in a rationally designed organic microdisk/silver nanowire heterostructures. The dye-doped flexible microdisks served as the wavelength tunable whispering-gallery-mode lasers with low lasing thresholds, whereas the silver nanowires supported the output of the lasing mode as subwavelength coherent light sources. The wavelength of the outcoupled laser was tuned over the full visible spectrum scope owing to the flexibility of the microdisks and their compatibility with various organic laser dyes. Furthermore, a multicolor subwavelength laser was achieved in a single heterostructure and the laser output was successfully modulated by varying the surface plasmon polariton propagation length.

Wavelength switchable micro/nanoscale laser is essential to construct various ultracompact photonic devices. However, traditional semiconductors as the gain media generally provide only monochromatic laser output due to their continuous energy band structures. For luminescent conjugated molecules, the broad emission band usually contains a series of vibronic peaks, which is very helpful for extending the lasing spectrum to several different wavelengths. Here we propose a novel strategy to realize wavelength switchable lasers based on the controlled competition of dual-wavelength vibronic lasing in single-component organic microcrystals. The vibrationally structured fluorescence property of the single-crystal organic microdisks brings dual-wavelength lasing at different vibronic bands. Their relative optical gain intensity was modulated by controlling the population on the certain vibronic level of the ground state with varied temperature, which consequently enabled the reversible switching of the dual-wav...

Micro/nanoscale lasers that can deliver intense coherent light signals at (sub)wavelength scale have recently captured broad research interest because of their potential applications ranging from on-chip information processing to high-throughput sensing. Organic molecular materials are a promising kind of ideal platform to construct high-performance microlasers, mainly because of their superiority in abundant excited-state processes with large active cross sections for high gain emissions and flexibly assembled structures for high-quality microcavities. In recent years, ever-increasing efforts have been dedicated to developing such organic microlasers toward low threshold, multicolor output, broadband tunability, and easy integration. Therefore, it is increasingly important to summarize this research field and give deep insight into the structure-property relationships of organic microlasers to accelerate the future development. In this Account, we will review the recent advances in organic miniaturized lasers, with an emphasis on tunable laser performances based on the tailorable microcavity structures and controlled excited-state gain processes of organic materials toward integrated photonic applications. Organic π-conjugated molecules with weak intermolecular interactions readily assemble into regular nanostructures that can serve as high-quality optical microcavities for the strong confinement of photons. On the basis of rational material design, a series of optical microcavities with different structures have been controllably synthesized. These microcavity nanostructures can be endowed with effective four-level dynamic gain processes, such as excited-state intramolecular charge transfer, excited-state intramolecular proton transfer, and excimer processes, that exhibit large dipole optical transitions for strongly active gain behaviors. By tailoring these excited-state processes with molecular/crystal engineering and external stimuli, people have effectively modulated the performances of organic micro/nanolasers. Furthermore, by means of controlled assembly and tunable laser performances, efficient outcoupling of microlasers has been successfully achieved in various organic hybrid microstructures, showing considerable potential for the integrated photonic applications. This Account starts by presenting 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 nanomaterials for the modulation of lasing performances are highlighted. In the following part, we introduce the construction and advanced photonic functionalities of organic-microlaser-based hybrid structures and their applications in integrated nanophotonics. Finally, we provide our outlook on the current challenges as well as the future development of organic microlasers. It is anticipated that this Account will provide inspiration for the development of miniaturized lasers with desired performances by tailoring of excited-state processes and microcavity structures toward integrated photonic applications.

Nanoscale lasers are ideal light-signal sources for integrated photonic devices. Most of the present lasers made of dielectric materials are restricted to being larger than half the wavelength of the optical field. Plasmon lasers made from metallic nanostructures can help to break the diffraction limit, yet they suffer from low optical pump efficiencies and low quality factors. Integrating dielectric lasers with plasmonic waveguides to construct hybrid material systems may circumvent these problems and combine the advantages of the two components. Here we demonstrate the nanoscale output of dielectric lasers via photon-plasmon coupling in rationally designed perovskite/silver heterostructures. The perovskite crystals offer the gain and high-Q cavity for low-threshold laser generation, while the embedded silver nanowires (AgNWs) help to output the lasing modes efficiently in the form of surface plasmons. The output coupling can be modulated by controlling the resonant modes of the two-dimensional perovskite microcavities. The results would pave an alternative avenue to ultrasmall light sources as well as fundamental studies of light-matter interactions.

Wavelength tunable micro/nanolasers are indispensable components for various photonic devices. Here, we report broadband tunable microlasers built by incorporating a highly polarized organic intramolecular charge-transfer (ICT) compound with a supramolecular host. The spatial confinement of the ICT dye generates an optimized energy level system that favors controlled population distribution between the locally excited (LE) state and the twisted intramolecular charge-transfer (TICT) state, which is beneficial for significantly broadening the tailorable gain region. As a result, we realized a wide tuning of lasing wavelength in the organic supramolecular microcrystals based on temperature-controlled population transfer from the LE to TICT state. The results will provide a useful enlightenment for the rational design of miniaturized lasers with desired performances.

Metal materials, supporting plasmon modes on their surface, can confine the optical field at deep subwavelength scale, which is desired for photonic integration. However, their intrinsic high Ohmic losses make it impossible to construct the whole circuit solely with the metal materials. Integrating the plasmonic components with dielectric materials may offer a solution to this dilemma. With outstanding active optical performance, these dielectric components not only can greatly reduce the optical losses of the entire circuits but also offer an efficient way to launch the surface plasmon polaritons through the evanescent field coupling or the direct exciton-plasmon conversion. Furthermore, the cooperative interaction between metal and dielectric materials would bring vast novel optical phenomena and functional photonic devices. In this review, the synergistic effects among metal and dielectric materials in various heterostructures as well as their related applications are highlighted. Comprehensive understanding on their synergistic interactions would offer useful guidance for the design and fabrication of the ultracompact novel optical devices.

Hybrid fluorescent nanoparticles (NPs) capable of fluorescing near-infrared (NIR) light (centered ∼730 nm) upon excitation of 800 nm laser light were constructed. A new type of conjugated polymer with two-photon excited fluorescence (TPEF) feature, P-F8-DPSB, was used as the NIR-light harvesting component and the energy donor while a NIR fluorescent dye, DPA-PR-PDI, was used as the energy acceptor and the NIR-light emitting component for the construction of the fluorescent NPs. The hybrid NPs possess δ value up to 2.3 × 10(6) GM per particle upon excitation of 800 nm pulse laser. The excellent two-photon absorption (TPA) property of the conjugated polymer component, together with its high fluorescence quantum yield (ϕ) up to 45% and the efficient energy transfer from the conjugated polymer to NIR-emitting fluorophore with efficiency up to 90%, imparted the hybrid NPs with TPEF-based NIR-input-NIR-output fluorescence imaging ability with penetration depth up to 1200 μm. The practicability of the hybrid NPs for fluorescence imaging in Hela cells was validated.

Flexible microdisk whispering-gallery-mode (WGM) resonators with high quality factors were achieved through the controlled assembly of organic materials with an emulsion-solvent-evaporation method. The high material compatibility of the assembled microdisks enabled us to realize low-threshold WGM lasers by doping with organic dyes as gain media. Furthermore, the emulsion-assisted self-assembly provided a strategy for the one-step fabrication of microwire-waveguide-connected microdisk heterostructures, which can be utilized for the efficient output of the isotropic WGM lasers from the coupled waveguides. We hope that these results will pave an avenue for the construction of new types of flexible WGM-based components for photonic integration.

A novel amphiphilic porphyrin derivative DOCP-Zn has been synthesized and utilized to construct tunable nanostructures from 0D to 1D by controlling the axial coordination of zinc porphyrin with 4,4′-bipyridine. SEM images indicated that patterns between 0D nanospheres and 1D nanorods or nanoslices can be reversibly converted by the construction or destroy of the axial coordination interaction. This facile approach provided a new method for controlling the nanostructure morphologies and dimension by patterns conversion. The photoluminescence microscopy images indicated the 1D nanorods material has the potential application as nanoscale photonic elements.

In the last 10 years, nanomaterials based on small organic molecules have attracted increasing attention. Such materials have unique optical and electronic properties, which could lead to new applications in nanoscale devices. Zero-dimensional (0D) organic nanoparticles with amorphous structures have been widely studied; however, the systematic investigation of crystalline one-dimensional (1D) organic nanostructures has only emerged in recent years. Researchers have used inorganic 1D nanomaterials, such as wires, tubes, and belts, as building blocks in optoelectronic nanodevices. We expect that their organic counterparts will also play an important role in this field. Because organic nanomaterials are composed of molecular units with weaker intermolecular interactions, they allow for higher structural tunability, reactivity, and processability. In addition, organic materials usually possess higher luminescence efficiency and can be grown on almost any solid substrate. In this Account, we describe recent progress in our group toward the construction of organic 1D nanomaterials and studies of their unique optical and electronic properties. First, we introduce the techniques for synthesizing 1D organic nanostructures. Because this strategy is both facile and reliable, liquid phase synthesis is most commonly used. More importantly, this method allows researchers to produce composite materials, including core/sheath and uniformly doped structures, which allow to investigate the interactions between different components in the nanomaterials, including fluorescent resonance energy transfer and photoinduced electron transfer. Physical vapor deposition allows for the synthesis of organic 1D nanomaterials with high crystallinity. Nanomaterials produced with this method offer improved charge transport properties and better optoelectronic performance in areas including multicolor emission, tunable emission, optical waveguide, and lasing. Although inorganic nanomaterials have developed rapidly, our findings highlight the importance of organic compounds as components of novel 1D nanomaterials.

During cooling of the ( R)-N-Fmoc-Octylglycine (Fmoc-OG)/cyclohexane solution, gelation is observed exclusively when ultrasound is used as an external stimulus, while deposit is obtained without sonication. The xerogel consists of entangled fibrous network made by interconnected nanofibers, while the deposit comprises large numbers of unbranched nanowires. It is found that the Fmoc-OG molecules form bilayer structures in both the deposit and the gel. However, the ratio ( R) between the Fmoc-OG molecules in a stable intramolecular H-bonding conformation and those in a metastable intermolecular H-bonding conformation can be tuned by the ultrasound, R (deposit)R (gel). The increased population of the intermolecular H-bonding Fmoc-OG molecules induced by the ultrasonication facilitates to the interconnection of nanofibers for the formation of the fibrous network, and therefore gelation. The alteration in the morphologies and properties of the obtained nanomaterials induced by the ultrasound wave demonstrates a potential method for smart controlling of the functions of nanomaterials from the molecular level.

The single crystalline nanowires have been fabricated from a small organic functional molecule, 2,4,5-triphenylimidazole (TPI), through an adsorbent-assisted physical vapor deposition (PVD) method. The introduction of the absorbents can significantly improve the dimensional uniformity of the as-prepared TPI nanowires. The TPI nanowires displayed interesting size-dependent optical properties, that is, the absorption spectra of the wires exhibit an obvious blue shift with the decrease of diameter, and simultaneously, the vibrational fine structures of the emission spectra emerge and become more pronounced with the diameter decreasing from 500 to 40 nm even at room temperature, which are usually observed only under cryogenic conditions. The emergence and enhancement of the vibrational structures are contributed to the increase of the long-range order and the degree of orientation with the decrease of diameter. The strategy described here should give a useful enlightenment for the fabrication of wirelike nano...

The single crystalline submicrotubes of a small organic functional molecule, 2,4,5-triphenylimidazole (TPI), were successfully prepared with a facile method. A series of characterizations indicated that the tubes were obtained from the rolling followed by seaming of a preorganized two-dimensional sheet-like structure, whose formation was due to the efficient cooperation of several molecular recognition elements. The length and diameter of the TPI tubes can be readily controlled by adjusting the experimental conditions. The as-prepared submicrotubes have intensive luminescence and size-dependent optical properties, which allows them to find potential applications in novel optical and optoelectronic devices together with their single crystalline structure and good stability. The strategy described here should give a useful enlightenment for the design and fabrication of tubular structures from small organic molecules.

Vertical organic nanowire arrays of 1,5-diaminoanthraquinone (DAAQ) on solid substrates were prepared by a facile physical vapor transport method. The crystal structure and growth direction of the nanowires were determined with electron diffraction. The color and fluorescence of the DAAQ nanowires can be bleached and quenched by acid vapor and rapidly regenerated by base vapor, making them useful as optical sensor materials. The ease of oriented vertical growth makes them promising nanophotonic elements that may be directly integrated into photonic devices during growth.