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1.
Artigo em Inglês | MEDLINE | ID: mdl-35020259

RESUMO

Conventional square planar platinum complexes typically form one-dimensional assemblies as a result of unidirectional metallophilic and/or π···π intermolecular interactions. Organoplatinum(II) complexes with a cruciform shape are presented herein to construct two-dimensional (2D) microcrystals with full-color and white phosphorescence. These 2D crystals show unique monocomponent π···π stacking from either the cyclometalating or noncyclometalating ligand and the bicomponent alternate π···π stacking from both ligands along different facet directions. Anisotropic tri-directional waveguiding is further implemented on a single hexagonal microcrystal. These results demonstrate the great capability of organoplatinum(II) cruciform as a general platform to fabricate 2D phosphorescent micro-/nanocrystals for advanced photonic applications.

2.
J Phys Chem Lett ; 13(1): 130-135, 2022 Jan 13.
Artigo em Inglês | MEDLINE | ID: mdl-34962396

RESUMO

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 in situ wavelength-switchable lasing based on the framework-shrinkage effect. A flexible HOF with reversible framework shrinkage was constructed from gain blocks with multiple rotors. The framework shrinkage of the HOF induced the in situ regulation on the conformation and conjugation degree of gain blocks, leading to distinct energy-level structures with blue/green-color gain emissions. Inspired by this, the in situ wavelength-switchable lasing from HOF microcrystals was achieved through reversibly controlling the framework shrinkage via the absorption/desorption of guests. The results offer useful insight into the use of flexible HOFs for exploiting miniaturized lasers with on-demand nanophotonics performance.

3.
ACS Appl Mater Interfaces ; 14(1): 1774-1782, 2022 Jan 12.
Artigo em Inglês | MEDLINE | ID: mdl-34968027

RESUMO

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.

4.
Adv Mater ; : e2106095, 2021 Dec 08.
Artigo em Inglês | MEDLINE | ID: mdl-34881466

RESUMO

Exciton-polaritons are half-light, half-matter bosonic quasiparticles formed by strong exciton-photon coupling in semiconductor microcavities. These hybrid particles possess the strong nonlinear interactions of excitons and keep most of the characteristics of the underlying photons. As bosons, above a threshold density they can undergo Bose-Einstein condensation to a polariton condensate phase and exhibit a rich variety of exotic macroscopic quantum phenomena in solids. Recently, organic semiconductors have been considered as a promising material platform for these studies due to their room-temperature stability, good processability, and abundant photophysics and photochemistry. Herein, recent advances of exciton-polaritons and their Bose-Einstein condensates in organic semiconductor microcavities are summarized. First, the basic physics is introduced, and then their emerging applications are highlighted. The remaining questions are also discussed and a personal viewpoint about the potential directions for future research is given.

5.
Chem Commun (Camb) ; 2021 Dec 06.
Artigo em Inglês | MEDLINE | ID: mdl-34870655

RESUMO

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.

6.
Adv Mater ; : e2107611, 2021 Dec 30.
Artigo em Inglês | MEDLINE | ID: mdl-34967981

RESUMO

Control over material architectures is essential to the performance of photonic devices and systems. Optical isolation of the photonic materials from substrates can significantly enhance their performance but suffers from complicated fabrication processes and limited applications. Here we propose a differential polymer chain scission strategy to fabricate free-standing photonic structures based on one-step electron-beam direct writing on polymer bilayers (EOB). The polymer molecular mass-dependent sensitivity to electron beam enables differential patterning of the two layers of polymers, leading to the direct formation of suspended optical microcavities. The EOB technique features high materials compatibility and design flexibility for the optical microcavities, which significantly expands the application scope of the suspended optical microcavities. As well as providing a versatile strategy for building high-performance photonic materials, our results provide a promising platform for innovative applications of optical microstructures. This article is protected by copyright. All rights reserved.

7.
J Am Chem Soc ; 143(48): 20249-20255, 2021 Dec 08.
Artigo em Inglês | MEDLINE | ID: mdl-34797057

RESUMO

Thermally activated delayed fluorescent (TADF) materials are promising to overcome triplet-induced optical loss in the pursuit of electrically pumped organic lasers. However, population inversion is difficult to establish in these materials due to the severe suppression of triplet-to-singlet upconversion in their condensed states. In this work, we report thermally activated lasing in solution-processed coassembled microcrystals, where TADF dyes were uniformly dispersed into crystalline matrices to ensure an efficient reverse intersystem crossing (RISC). The dark-state triplet excitons harvested by the RISC were effectively converted into radiative singlet excitons, which subsequently participated in the population inversion to boost lasing with an unusual temperature dependence. The lasing wavelength was tuned over the full visible spectrum by doping various TADF laser dyes, owing to the excellent compatibility. Trichromatic TADF microlasers were precisely patterned into periodic pixelated arrays by a template-confined solution-growth method. With as-prepared TADF microlaser arrays as display panels, vivid laser displays were achieved under programmable excitation. These results offer valuable enlightenment to minimize triplet state-related energy losses toward high-performance lasers.

8.
Natl Sci Rev ; 8(2): nwaa162, 2021 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-34691572

RESUMO

Modern high-security cryptography and optical communication call for covert bit sequences with high coding capacity and efficient authentication. Stimuli-responsive lasing emissions with easily distinguishable readout are promising in the coding field as a novel cryptographic primitive, while the application is frequently restricted by the limited number of emission states. Here, we report a strategy of achieving multiple competitive lasing signals in responsive organic microspheres where a donor-acceptor pair was introduced. The competitive lasing from the donor and acceptor was reversibly switched by modulating the competition between the radiative rate of the donor and the rate of energy transfer, and the generated multiple lasing signals enabled a quaternary coding for recognizable cryptographic implementation. Data encryption and extraction were demonstrated using a 4 × 4 microlaser array, showing vast prospects in avoiding the disclosure of security information. The results offer a comprehensive understanding of excited-state dynamics in organic composite materials, which may play a major role in high-security optical recording and information encryption.

9.
J Am Chem Soc ; 143(37): 15319-15325, 2021 Sep 22.
Artigo em Inglês | MEDLINE | ID: mdl-34506155

RESUMO

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.

10.
Adv Mater ; 33(42): e2102586, 2021 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-34477249

RESUMO

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.

11.
Adv Sci (Weinh) ; 8(21): e2102065, 2021 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-34561964

RESUMO

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.

12.
Adv Mater ; 33(37): e2104418, 2021 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-34337797

RESUMO

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.

13.
Angew Chem Int Ed Engl ; 60(46): 24519-24525, 2021 Nov 08.
Artigo em Inglês | MEDLINE | ID: mdl-34339093

RESUMO

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.

14.
Nano Lett ; 21(16): 6792-6799, 2021 Aug 25.
Artigo em Inglês | MEDLINE | ID: mdl-34398615

RESUMO

Lasing signals with easily distinguishable readout and cavity-geometry-dependent output are emerging as novel cryptographic primitives for two-dimensional (2D) optical encryption, while their practical application is restricted by the challenge of integrating different lasing elements onto an identical 2D pattern. Herein, a lithographic template-confined crystallization approach was proposed to prepare large-scale perovskite microstructures with any desired geometries and locations, which enabled them to serve as 2D lasing patterns for reliable encryption and authentication. These prepatterned perovskite microstructures realized whispering-gallery-mode lasing and also demonstrated outstanding reproducibility of lasing actions. Benefiting from the feature of their cavity-geometry-dependent lasing thresholds, we achieved controllable laser output from different shaped elements, which was further utilized for the proof-of-concept demonstration of a cryptographic implementation. The remarkable lasing performance and feasible preparation of 2D microlaser patterns with customized geometries and locations provide us deep insights into the concepts and fabrication technologies for 2D optical encryption.

15.
Sci Adv ; 7(31)2021 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-34330710

RESUMO

Flexible photonics is rapidly emerging as a promising platform for artificial smart skins to imitate or extend the capabilities of human skins. Organic material systems provide a promising avenue to directly fabricate large-scale flexible device units; however, the versatile fabrication of all-organic integrated devices with desired photonic functionalities remains a great challenge. Here, we develop an effective technique for the mass processing of organic microlaser arrays, which act as sensing units, on the chip of photonic skins. With a bilayer electron-beam direct writing method, we fabricated flexible mechanical sensor networks composed of coupled-cavity single-mode laser sources on pliable polymer substrates. These microlaser-based mechanical sensor chips were subsequently used to recognize hand gestures, showing great potential for artificial skin applications. This work represents a substantial advance toward scalable construction of high-performance and low-cost flexible photonic chips, thus paving the way for the implementation of smart photonic skins into practical applications.

16.
Nat Commun ; 12(1): 3265, 2021 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-34075038

RESUMO

Exciton-polariton Bose-Einstein condensation (EP BEC) is of crucial importance for the development of coherent light sources and optical logic elements, as it creates a new state of matter with coherent nature and nonlinear behaviors. The demand for room temperature EP BEC has driven the development of organic polaritons because of the large binding energies of Frenkel excitons in organic materials. However, the reliance on external high-finesse microcavities for organic EP BEC results in poor compactness and integrability of devices, which restricts their practical applications in on-chip integration. Here, we demonstrate room temperature EP BEC in organic single-crystal microribbon natural cavities. The regularly shaped microribbons serve as waveguide Fabry-Pérot microcavities, in which efficient strong coupling between Frenkel excitons and photons leads to the generation of EPs at room temperature. The large exciton-photon coupling strength due to high exciton densities facilitates the achievement of EP BEC. Taking advantages of interactions in EP condensates and dimension confinement effects, we demonstrate the realization of controllable output of coherent light from the microribbons. We hope that the results will provide a useful enlightenment for using organic single crystals to construct miniaturized polaritonic devices.

17.
ACS Appl Mater Interfaces ; 13(24): 28662-28667, 2021 Jun 23.
Artigo em Inglês | MEDLINE | ID: mdl-34114811

RESUMO

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.

18.
Angew Chem Int Ed Engl ; 60(24): 13548-13553, 2021 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-33792143

RESUMO

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).

19.
ACS Appl Mater Interfaces ; 13(16): 19187-19192, 2021 Apr 28.
Artigo em Inglês | MEDLINE | ID: mdl-33871261

RESUMO

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.


Assuntos
Fibroínas/química , Lasers , Microesferas , Conformação Proteica
20.
Adv Mater ; 33(18): e2100484, 2021 May.
Artigo em Inglês | MEDLINE | ID: mdl-33783062

RESUMO

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.

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