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1.
J Am Chem Soc ; 145(3): 1557-1563, 2023 Jan 25.
Article in English | MEDLINE | ID: mdl-36630440

ABSTRACT

Integrated electro-optical switches are essential as one of the fundamental elements in the development of modern optoelectronics. As an architecture for photonic systems exciton polaritons, hybrid bosonic quasiparticles that possess unique properties derived from both excitons and photons, have shown much promise. For this system, we demonstrate a significant improvement of emitted intensity and condensation threshold by applying an electric field to a microcavity filled with an organic microbelt. Our theoretical investigations indicate that the electric field makes the excitons dipolar and induces an enhancement of the exciton-polariton interaction and of the polariton lifetime. Based on these electric field-induced changes, a sub-nanosecond electrical field-enhanced polariton condensate switch is realized at room temperature, providing the basis for developing an on-chip integrated photonic device in the strong light-matter coupling regime.

2.
Nat Commun ; 14(1): 31, 2023 Jan 03.
Article in English | MEDLINE | ID: mdl-36596798

ABSTRACT

Circularly polarized (CP) electroluminescence from organic light-emitting diodes (OLEDs) has aroused considerable attention for their potential in future display and photonic technologies. The development of CP-OLEDs relies largely on chiral-emitters, which not only remain rare owing to difficulties in design and synthesis but also limit the performance of electroluminescence. When the polarization (pseudospin) degrees of freedom of a photon interact with its orbital angular momentum, photonic spin-orbit interaction (SOI) emerges such as Rashba-Dresselhaus (RD) effect. Here, we demonstrate a chiral-emitter-free microcavity CP-OLED with a high dissymmetry factor (gEL) and high luminance by embedding a thin two-dimensional organic single crystal (2D-OSC) between two silver layers which serve as two metallic mirrors forming a microcavity and meanwhile also as two electrodes in an OLED architecture. In the presence of the RD effect, the SOIs in the birefringent 2D-OSC microcavity result in a controllable spin-splitting with CP dispersions. Thanks to the high emission efficiency and high carrier mobility of the OSC, chiral-emitter-free CP-OLEDs have been demonstrated exhibiting a high gEL of 1.1 and a maximum luminance of about 60000 cd/m2, which places our device among the best performing CP-OLEDs. This strategy opens an avenue for practical applications towards on-chip microcavity CP-OLEDs.

3.
Angew Chem Int Ed Engl ; 61(39): e202209211, 2022 Sep 26.
Article in English | MEDLINE | ID: mdl-35923091

ABSTRACT

The spatial separation between the highest occupied and the lowest unoccupied molecular orbitals (HOMO and LUMO) in thermally activated delayed fluorescent (TADF) molecules leads to charge transfer (CT) states, which degrade the oscillator strength of emission transition and sacrifices high solid-state photoluminescence quantum yield (PLQY), together limiting its application in organic solid-state lasers (OSSLs). Here, we demonstrated organic microwire lasers from TADF emitters that combine aggregation induced emission (AIE) and local excited (LE) state characteristics. The unique AIE and LE feature lead to a PLQY approaching 50 % and a high optical gain of 870 cm-1 for TADF microwires. The regenerated singlet excitons by reverse intersystem crossing (RISC) process are conducive to population inversion. As a result, we demonstrated microwire lasers around 465 nm with a low threshold of 3.74 µJ cm-2 . Therefore, our work provides insight to design TADF materials for OSSLs.

4.
Nano Lett ; 22(14): 5803-5809, 2022 Jul 27.
Article in English | MEDLINE | ID: mdl-35848711

ABSTRACT

An organic light-emitting transistor (OLET) is a candidate device architecture for developing electrically pumped organic solid-state lasers, but it remains a critical challenge because of the lack of organic semiconductors that simultaneously possess a high solid-state emission efficiency (Φs), a high and balanced ambipolar mobility (µh,e), and a large stimulated emission cross-section. Here, we designed a molecule of 4,4'-bis(2-dibenzothiophenyl-vinyl)-biphenyl (DBTVB) and prepared its ultrathin single-crystal microplates with herringbone packing arrangements, which achieve balanced mobilities of µh = 3.55 ± 0.5 and µe = 2.37 ± 0.5 cm2 V-1 s-1, a high Φs of 85 ± 3%, and striking low-threshold laser characteristics. Theoretical and experimental investigations reveal that a strong electronic coupling and a small reorganization energy ensure efficient charge transport; meanwhile, the exciton-vibration effect and negligible π-π orbital overlap give rise to highly emissive H-aggregates and facilitate laser emission. Furthermore, OLET-based DBTVB crystals offer an internal quantum efficiency approaching 100% and a record-high electroluminescence external quantum efficiency of 4.03%.

5.
Angew Chem Int Ed Engl ; 61(34): e202205636, 2022 Aug 22.
Article in English | MEDLINE | ID: mdl-35698256

ABSTRACT

Solution-processed, high-gain, and wavelength-tunable perovskite single-crystal microdisk (PVKsc-MD) lasers have emerged as prospective coherent light sources in advanced nanophotonic designs. However, the inevitable multi-directional emission from a highly symmetrical cavity leads to low light collection efficiency which greatly hinders its application in integrated optical circuits. Here, we report on surface-patterned MAPbBr3 PVKsc-MDs synthesized by a cost-efficient bottom-up solution process employing spin-coating and confined-growth nanoimprinting. The patterned microdisks have high crystal quality with regular shape and sharp edges and nano-grating structure on the upper surface. This straightforward process yields surface-patterned PVKsc-MD lasers with a low lasing threshold and high quality (Q) factor. In addition, the grating structure patterned on the PVKsc-MDs reduces the original symmetry of the laser cavity, which improves the emission directionality four times.

6.
Angew Chem Int Ed Engl ; 60(37): 20274-20279, 2021 Sep 06.
Article in English | MEDLINE | ID: mdl-34278668

ABSTRACT

The development of high mobility organic laser semiconductors with strong emission is of great scientific and technical importance, but challenging. Herein, we present a high mobility organic laser semiconductor, 2,7-diphenyl-9H-fluorene (LD-1) showing unique crystallization-enhanced emission guided by elaborately modulating its crystal growth process. The obtained one-dimensional nanowires of LD-1 show outstanding integrated properties including: high absolute photoluminescence quantum yield (PLQY) approaching 80 %, high charge carrier mobility of 0.08 cm2 V-1 s-1 , Fabry-Perot lasing characters with a low threshold of 86 µJ cm-2 and a high-quality factor of ≈2400. Furthermore, electrically induced emission was obtained from an individual LD-1 crystal nanowire-based light-emitting transistor due to the recombination of holes and electrons simultaneously injected into the nanowire, which provides a good platform for the study of electrically pumped organic lasers and other related ultrasmall integrated electrical-driven photonic devices.

7.
Nat Commun ; 12(1): 1838, 2021 03 23.
Article in English | MEDLINE | ID: mdl-33758192

ABSTRACT

Multimetallic nanostructures can be synthesized by integrating up to seven or eight metallic elements into a single nanoparticle, which represent a great advance in developing complex multicomponent nanoparticle libraries. Contrary, organic micro- and nanoparticles beyond three π-conjugated components have not been explored because of the diversity and structural complexity of molecular assemblies. Here, we report a library of microparticles composed of an arbitrary combination of four luminescent organic semiconductors. We demonstrate that the composition and emission color of each domain as well as its spatial distribution can be rationally modulated. Unary, binary, ternary, and quaternary microparticles are thus realized in a predictable manner based on the miscibility of the components, resulting in mixed-composition phases or alloyed or phase separated heterostructures. This work reports a simple yet available synthetic methodology for rational modulation of organic multicomponent microparticles with complex architectures, which can be used to direct the design of functional microparticles.

8.
ACS Appl Mater Interfaces ; 12(24): 27493-27498, 2020 Jun 17.
Article in English | MEDLINE | ID: mdl-32431143

ABSTRACT

Creating nano-to-macroscopic-sized artificial actuators in response to light has been a challenging issue. Herein, we describe the design, synthesis, and operation of a photomechanical molecular crystal (PMMC) that exhibits well-controlled multiple photo-driven motions, including translation, rotation, and jumping, by adjusting the irradiation sites. Theoretical calculation discloses that conversion of light energy into macroscopic motion occurs through a molecular conformation change between the excited and ground states mediated by ultrafast conical internal conversion, making the photomechanical/recovery responses a rapid cycle. Therefore, our PMMCs can complete the directional and continuous motions using only one laser beam. We also demonstrated the actuated rotation of a cross-shaped sample by rotating the polarization of the laser beam at a rate of >2 Hz, like a dancer under a spotlight. This finding could lead to remote-controlled micrometer-sized vehicles and valves on solid substrates.

9.
J Am Chem Soc ; 142(13): 6332-6339, 2020 Apr 01.
Article in English | MEDLINE | ID: mdl-32186872

ABSTRACT

Here, we design and synthesize an organic laser molecule, 2,7-diphenyl-9H-fluorene (LD-1), which has state-of-the-art integrated optoelectronic properties with a high mobility of 0.25 cm2 V-1 s-1, a high photoluminescence quantum yield of 60.3%, and superior deep-blue laser characteristics (low threshold of Pth = 71 µJ cm-2 and Pth = 53 µJ cm-2 and high quality factor (Q) of ∼3100 and ∼2700 at emission peaks of 390 and 410 nm, respectively). Organic light-emitting transistors based on LD-1 are for the first time demonstrated with obvious electroluminescent emission and gate tunable features. This work opens the door for a new class of organic semiconductor laser molecules and is critical for deep-blue optical and laser applications.

10.
Angew Chem Int Ed Engl ; 59(27): 11080-11086, 2020 Jun 26.
Article in English | MEDLINE | ID: mdl-32219946

ABSTRACT

Organic solid-state semiconductor lasers are attracting ever-increasing interest for their potential application in future photonic circuits. Despite the great progress made in recent years, an organic laser from 3D chiral structures has not been achieved. Now, the first example of an organic nano-laser from the micro-helix structure of an achiral molecule is presented. Highly regular micro-helixes with left/right-handed helicity from a distyrylbenzene derivative (HM-DSB) were fabricated and characterized under microscope spectrometers. These chiral micro-helixes exhibit unique photonic properties, including helicity-dependent circularly polarized luminescence (CPL), periodic optical waveguiding, and length-dependent amplified spontaneous emission (ASE) behavior. The successful observation of laser behavior from the organic micro-helix extends our understanding to morphology chirality of organic photonic materials and provides a new design strategy towards chiral photonic circuits.

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