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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.
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.

3.
J Phys Chem Lett ; 12(51): 12276-12282, 2021 Dec 30.
Artigo em Inglês | MEDLINE | ID: mdl-34931841

RESUMO

Through the combination of transient spectroscopy and theoretical simulations, an accelerated singlet fission (SF) process was evidently observed in the strongly coupled H-type-like aggregation thin films of a dipyrrolonaphthyridinedione skeleton. Results elucidate that in this H-type-like aggregation, the substantially stabilized charge transfer (CT) state is close in energy with singlet and excimer states, resulting in a CT/excimer mixed state, which could drive excited-state population escaping from excimer trap and promote an ultrafast and highly efficient SF process. Our results not only enrich the limited capacity of SF materials but also contribute to an in-depth understanding of SF dynamics in H-type aggregation, which is of fundamental importance for designing new SF sensitizers and implementing practical SF applications.

4.
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 a differential polymer chain scission strategy is proposed 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, the results provide a promising platform for innovative applications of optical microstructures.

5.
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.

6.
Natl Sci Rev ; 8(1): nwaa201, 2021 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-34691557

RESUMO

Exploring stable clusters to understand structural evolution from atoms to macroscopic matter and to construct new materials is interesting yet challenging in chemistry. Utilizing our newly developed deep-ultraviolet laser ionization mass spectrometry technique, here we observe the reactions of neutral cobalt clusters with oxygen and find a very stable cluster species of Co13O8 that dominates the mass distribution in the presence of a large flow rate of oxygen gas. The results of global-minimum structural search reveal a unique cubic structure and distinctive stability of the neutral Co13O8 cluster that forms a new class of metal oxides that we named as 'metalloxocubes'. Thermodynamics and kinetics calculations illustrate the structural evolution from icosahedral Co13 to the metalloxocube Co13O8 with decreased energy, enhanced stability and aromaticity. This class of neutral oxygen-passivated metal clusters may be an ideal candidate for genetic materials because of the cubic nature of the building blocks and the stability due to cubic aromaticity.

7.
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.

8.
Phys Rev Lett ; 127(10): 107402, 2021 Sep 03.
Artigo em Inglês | MEDLINE | ID: mdl-34533335

RESUMO

The geometry of Hamiltonian's eigenstates is encoded in the quantum geometric tensor (QGT), containing both the Berry curvature, central to the description of topological matter, and the quantum metric. So far, the full QGT has been measured only in Hermitian systems, where the role of the quantum metric is mostly limited to corrections. On the contrary, in non-Hermitian systems, and, in particular, near exceptional points, the quantum metric is expected to diverge and to often play a dominant role, for example, in the enhanced sensing and in wave packet dynamics. In this Letter, we report the first experimental measurement of the quantum metric in a non-Hermitian system. The specific platform under study is an organic microcavity with exciton-polariton eigenstates, which demonstrate exceptional points. We measure the quantum metric's divergence, and we determine the scaling exponent n=-1.01±0.08, which is in agreement with the theoretical description of second-order exceptional points.

9.
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.

10.
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.

11.
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.

12.
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.

13.
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.

14.
J Am Chem Soc ; 143(15): 5691-5697, 2021 04 21.
Artigo em Inglês | MEDLINE | ID: mdl-33843229

RESUMO

Singlet fission (SF), the conversion of one high-energy singlet to two low-energy triplets, provides the potential to increase the efficiency of photovoltaic devices. In the SF chromophores with C2h symmetry, exemplified by polyenes, singlet-to-triplet conversion generally involves a low-lying 21Ag dark state, which serves as either a multiexciton (ME) intermediate to promote the SF process or a parasitic trap state to shunt excited-state populations via internal conversion. This controversial behavior calls for a deep understanding of dark-state-related photophysics involving the higher-lying singlet state. However, the optical "dark" and "transient" nature of these dark states and strong correlation feature of double exciton species make their characterization and interpretation challenging from both experimental and computational perspectives. In the present work combining transient spectroscopy and multireference electronic structure calculations (XDW-CASPT2), we addressed a new photophysical model, i.e., a high-lying 31Ag dark-state-mediated ultrafast SF process in the benzodipyrrolidone (BDPP) skeleton. Such a 31Ag dark state with distinctive double excitation character, described as the ME state, could be populated from the initial 11Bu bright state on an ultrafast time scale given the quasi-degeneracy and intersection of the two electronic states. Furthermore, the suitable optical band gap and triplet energy, high triplet yield, and excellent photostability render BDPP a promising SF candidate for photovoltaic devices. These results not only enrich the arsenal of SF materials but also shed new insights into the understanding of dark-state-related photophysics, which could promote the development of new SF-active materials.

15.
Angew Chem Int Ed Engl ; 60(26): 14595-14600, 2021 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-33822449

RESUMO

A simple and general method is presented herein for the in situ preparations of circularly polarized luminescence (CPL)-active microcrystals with a large luminescence dissymmetry factor glum , high fluorescence quantum efficiency (ΦFL ), wide emission color tenability, and well-ordered morphology. The reactions of pyridine-containing achiral molecules 1-7 with chiral camphor sulfonic acid ((±)-CSA) gave crystalline microplates formed by hydrogen bonding interactions between the protonated pyridinium units and the sulfonic anions. The chiral information of CSA are effectively transferred to the microcrystals by hydrogen bonding to afford full-color CPL from deep-blue to red with glum in the order of 10-2 and ΦFL up to 80 %. Moreover, organic microcrystals with high-performance white CPL (ΦFL =46 %; |glum |=0.025) are achieved via the light-harvesting energy transfer between blue and yellow emitters.

16.
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.

17.
Nanoscale ; 13(10): 5300-5306, 2021 Mar 18.
Artigo em Inglês | MEDLINE | ID: mdl-33660721

RESUMO

We have synthesized single crystals of a highly stable Cu-doped undeca-gold cluster protected by both triphenylphosphine (PPh3) and 2-pyridinethiol (-SPy) ligands, formulated as [Au11Cu1(PPh3)7(SPy)3]+. This cluster (Au11Cu1 NCs for short) has a metallic core of C3v Au@Au10 with the Cu atom capped on one of the nine triangular facets and it is triply-coordinated to three N atoms of the SPy ligands of which the sulfur atom simultaneously binds to three adjacent Au atoms via singly-coordinated S-Au bonds, respectively. The other seven gold atoms form a crown structure by a link of three orthogons with common sides and are protected by seven PPh3 ligands. Besides the well-organized coordination, this Au11Cu1 nanocluster is demonstrated to exhibit superatom stability of the metallic core within 8 valence electrons (assuming that the 3 electrophilic-SPy ligands capture 3 electrons from the metal center). More interestingly, this Au11Cu1 nanocluster shows interesting emissions in both ultraviolet visible (UV-Vis) and near infrared (NIR) regions, and the emissions display novel anti-Stokes up-conversion lasing characteristics. TD-DFT calculated UV-vis and emission spectra well reproduce the experimental results, shedding light on the nature of excitation states and underlying mechanism of electronic transitions between diverse energy levels of such a monolayer-protected bimetallic cluster.

18.
Nat Commun ; 12(1): 689, 2021 Jan 29.
Artigo em Inglês | MEDLINE | ID: mdl-33514702

RESUMO

Optical activity, also called circular birefringence, is known for two hundred years, but its applications for topological photonics remain unexplored. Unlike the Faraday effect, the optical activity provokes rotation of the linear polarization of light without magnetic effects, thus preserving the time-reversal symmetry. In this work, we report a direct measurement of the Berry curvature and quantum metric of the photonic modes of a planar cavity, containing a birefringent organic microcrystal (perylene) and exhibiting emergent optical activity. This experiment, performed at room temperature and at visible wavelength, establishes the potential of organic materials for implementing non-magnetic and low-cost topological photonic devices.

19.
J Am Chem Soc ; 142(42): 17892-17896, 2020 Oct 21.
Artigo em Inglês | MEDLINE | ID: mdl-33044060

RESUMO

The exploitation of singlet fission (SF) in photovoltaic devices is restricted by the limited number of SF materials available and the conflicting requirement of intermolecular interactions to satisfy both efficient SF and subsequent triplet extraction. Intramolecular SF (iSF) represents an emerging alternative and may prove simpler to implement in devices. On account of the excellent chemical structure tunability and solution processability, conjugated polymers have emerged as promising candidates for iSF materials despite being largely underexplored. It remains a significant challenge to develop SF-capable conjugated polymers and achieve efficient dissociation of the formed triplet pairs simultaneously. In this contribution, we present a new iSF material in a para-azaquinodimethane-based quinoidal conjugated polymer. Using transient optical techniques, we show that an ultrafast iSF process dominates the deactivation of the excited state in such polymer, featuring ultrafast population (<1 ps) and stepwise dissociation of triplet pairs. Notably, these multiexciton states could further diffuse apart to produce long-lived free triplets (tens of µs) in strongly coupled aggregates in solid thin film. Such findings not only introduce a new iSF-active conjugated polymer to the rare SF material family but also shed unique insight into interchain interaction-promoted triplet pair dissociation in aggregates of conjugated polymers, thus openning new avenues for developing next-generation SF-based photovoltaic materials.

20.
Light Sci Appl ; 9: 151, 2020.
Artigo em Inglês | MEDLINE | ID: mdl-32904405

RESUMO

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.

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