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1.
J Am Chem Soc ; 146(12): 7885-7904, 2024 Mar 27.
Artigo em Inglês | MEDLINE | ID: mdl-38483827

RESUMO

Integrated electronics and optoelectronics based on organic semiconductors have attracted considerable interest in displays, photovoltaics, and biosensing owing to their designable electronic properties, solution processability, and flexibility. Miniaturization and integration of devices are growing trends in molecular electronics and optoelectronics for practical applications, which requires large-scale and versatile assembly strategies for patterning organic micro/nano-structures with simultaneously long-range order, pure orientation, and high resolution. Although various integration methods have been developed in past decades, molecular electronics still needs a versatile platform to avoid defects and disorders due to weak intermolecular interactions in organic materials. In this perspective, a roadmap of organic integration technologies in recent three decades is provided to review the history of molecular electronics. First, we highlight the importance of long-range-ordered molecular packing for achieving exotic electronic and photophysical properties. Second, we classify the strategies for large-scale integration of molecular electronics through the control of nucleation and crystallographic orientation, and evaluate them based on factors of resolution, crystallinity, orientation, scalability, and versatility. Third, we discuss the multifunctional devices and integrated circuits based on organic field-effect transistors (OFETs) and photodetectors. Finally, we explore future research directions and outlines the need for further development of molecular electronics, including assembly of doped organic semiconductors and heterostructures, biological interfaces in molecular electronics and integrated organic logics based on complementary FETs.

2.
Adv Mater ; 36(23): e2314061, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38350441

RESUMO

Colloidal quantum dots (CQDs) are considered a promising material for the next generation of integrated display devices due to their designable optical bandgap and low energy consumption. Owing to their dispersibility in solvents, CQD micro/nanostructures are generally fabricated by solution-processing methods. However, the random mass transfer in liquid restricts the programmable construction in macroscopy and ordered assembly in microscopy for the integration of CQD optical structures. Herein, a multi-interfacial confined assembly strategy is developed to fabricate CQDs programmable microstructure arrays with a quasisuperlattice configuration through controlling the dynamics of three-phase contact lines (TPCLs). The motion of TPCLs dominates the division of liquid film for precise positioning of CQD microstructures, while pinned TPCLs control the solvent evaporation and concentration gradient to directionally drive the mass transfer and packing of CQDs. Owing to their long-range order and adjustable structural dimensions, CQD microring arrays function as high-quality-factor (high-Q) lasing resonant cavities with low thresholds and tunable lasing emission modes. Through the further surface treatment and liquid dynamics control, the on-chip integration of red (R), green (G), and blue (B) multicomponent CQD microlaser arrays are demonstrated. The technique establishes a new route to fabricate large-area, ultrahigh-definition, and full-color CQD laser displays.

3.
Adv Mater ; 36(16): e2312396, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38198647

RESUMO

Conventional circularly polarized light (CPL) detectors necessitate several optical elements, posing difficulties in achieving miniature and integrated devices. Recently developed organic CPL detectors require no additional optical elements but usually suffer from low detectivity or low asymmetry factor (g-factor). Here, an organic CPL detector with excellent detectivity and a high g-factor is fabricated. By employing an inverted quasi-planar heterojunction (IPHJ) structure and incorporating an additional liquid crystal film, a CPL detector with an outstanding g-factor of 1.62 is developed. Unfavorable charge injection is effectively suppressed by the IPHJ structure, which reduces the dark current of the organic photodetector. Consequently, a left CPL detectivity of 6.16 × 1014 Jones at 640 nm is realized, surpassing all of the latest photodiode-type CPL detectors. Adopting a liquid crystal film with adjustable wavelengths of selectively reflected light, the hybrid device achieves narrow dual-band CPL detection, varying from 530 to 640 nm, with a half-maximum full width below 90 nm. Notably, the device achieves excellent stability of 260 000 on/off cycles without attenuation. To the best of the authors' knowledge, all these features have rarely been reported in previous work. The CPL detector arrays are also demonstrated for encrypted communications and color imaging.

4.
Acc Chem Res ; 57(2): 222-233, 2024 Jan 16.
Artigo em Inglês | MEDLINE | ID: mdl-38170611

RESUMO

ConspectusSelf-assembly, a spontaneous process that organizes disordered constituents into ordered structures, has revolutionized our fundamental understanding of living matter, nanotechnology, and molecular science. From the perspective of nanomaterials, self-assembly serves as a bottom-up method for creating long-range-ordered materials. This is accomplished by tailoring the geometry, chemistry, and interactions of the components, thereby facilitating the efficient fabrication of high-quality materials and high-performance functional devices. Over the past few decades, we have seen controllable organization and diverse phases in self-assembled materials, such as organic crystals, biomolecular structures, and colloidal nanoparticle supercrystals. However, most self-assembled ordered materials and their assembly mechanisms are derived from constituents in a liquid bulk medium, where the effects of boundaries and interfaces are negligible. In the context of nanostructure patterning, self-assembly occurs in confined spaces, with feature sizes ranging from a few to hundreds of nanometers. In such settings, ubiquitous boundaries and interfaces can trap the system in a kinetically favored but metastable state, devoid of long-range order. This makes it extremely difficult to achieve ordered structures in micro/nano-patterning techniques that rely on sessile microdroplets, such as inkjet printing, dip-pen lithography, and contact printing.In stark contrast to sessile droplets, capillary bridges─formed by liquids confined between two solid surfaces─provide unique opportunities for understanding the long-range-ordered self-assembly of crystalline materials under spatial confinement. Because capillary bridges are stabilized by Laplace pressure, which is inversely proportional to the feature size, the confinement and manipulation of solutions or suspensions of functional materials at the nanoscale become accessible through the rational design of surface chemistry and geometry. Although global thermodynamic equilibrium is unattainable in evaporative systems, ordered nucleation and packing of constituent components can be locally realized at the contact line of capillary bridges. This enables the unprecedented fabrication of long-range-ordered micro/nanostructures with deterministic patterns.In this Account, we review the advancements in long-range-ordered self-assembly of crystalline micro/nanostructures under confinement. First, we briefly introduce crystalline materials characterized by strong intramolecular interactions and relatively weak intermolecular forces, analyzing both the opportunities and challenges inherent to self-assembled nanomaterials. Next, we delve into the construction and manipulation of confined liquids, focusing especially on capillary bridges controlled by engineered chemistry and geometry to regulate Laplace pressure. Through this approach, we have achieved capillary bridges with thicknesses on the order of a few nanometers and wafer-scale homogeneity, facilitating the self-assembly of ordered structures. Supported by factors such as local free-volume entropy, electrostatic interactions, curvilinear geometry, directional microfluidics, and nanoconfinement, we have achieved long-range-ordered, deterministic patterning of organic semiconductors, metal-halide perovskites, and colloidal nanocrystal superlattices using this capillary-bridge platform. These long-range microstructures serve as a bridge between nanomaterials and integrated devices, enabling emergent functionalities like intrinsic stretchability, giant photoconductivity, propagating and interacting exciton polaritons, and spin-valley-locked lasing, which are otherwise unattainable in disordered materials. Finally, we discuss potential directions for both the fundamental understanding and practical applications of confined self-assembly.

5.
J Am Chem Soc ; 145(16): 8908-8916, 2023 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-37057869

RESUMO

Chiral perovskites have attracted considerable attention owing to their potential applications in spintronic- and polarization-based optoelectronic devices. However, the structural chirality/asymmetry transfer mechanism between chiral organic ammoniums and achiral inorganic frameworks is still equivocal, especially under extreme conditions, as the systematic structural differences between chiral and achiral perovskites have been rarely explored. Herein, we successfully synthesized a pair of new enantiomeric chiral perovskite (S/R-3PYEA)PbI4 (3PYEA2+ = C5NH5C2H4NH32+) and an achiral perovskite (rac-3PYEA)PbI4. Hydrostatic pressure was used, for the first time, to systematically investigate the differences in the structural evolution and optical behavior between (S/R-3PYEA)PbI4 and (rac-3PYEA)PbI4. At approximately 7.0 GPa, (S/R-3PYEA)PbI4 exhibits a chirality-dependent structural transformation with a bandgap "red jump" and dramatic piezochromism from translucent red to opaque black. Upon further compression, a previously unreported chirality-induced negative linear compressibility (NLC) is achieved in (S/R-3PYEA)PbI4. High-pressure structural characterizations and first-principles calculations demonstrate that pressure-driven homodirectional tilting of homochiral ammonium cations strengthens the interactions between S/R-3PYEA2+ and Pb-I frameworks, inducing the formation of new asymmetric hydrogen bonds N-H···I-Pb in (S/R-3PYEA)PbI4. The enhanced asymmetric H-bonding interactions further break the symmetry of (S/R-3PYEA)PbI4 and trigger a greater degree of in-plane and out-of-plane distortion of [PbI6]4- octahedra, which are responsible for chirality-dependent structural phase transition and NLC, respectively. Nevertheless, the balanced H-bonds incurred by equal proportions of S-3PYEA2+ and R-3PYEA2+ counteract the tilting force, leading to the absence of chirality-dependent structural transition, spectral "red jump", and NLC in (rac-3PYEA)PbI4.

6.
Adv Mater ; 35(19): e2210594, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36859570

RESUMO

Orientational growth of single-crystalline structures is pivotal in the semiconductor industry, which is achievable by epitaxy for producing thin films, heterostructures, quantum wells, and superlattices. Beyond silicon and III-V semiconductors, solution-processible semiconductors, such as metal-halide perovskites, are emerging for scalable and cost-effective manufacture of optoelectronic devices, whereas the polycrystalline nature of fabricated structures restricts their application toward integrated devices. Here, electrostatic epitaxy, a process sustained by strong electrostatic interactions between self-assembled surfactants (octanoate anions) and Pb2+ , is developed to realize orientational growth of single-crystalline CsPbBr3 microwires. Strong electrostatic interactions localized at the air-liquid interface not only support preferential nucleation for single crystallinity, but also select the crystal facet with the highest Pb2+ areal density for pure crystallographic orientation. Due to the epitaxy at the air-liquid interface, direct growth of oriented single-crystalline microwires onto different substrates without the processes of lift-off and transfer is realized. Photonic lasing emission, waveguide coupling, and on-chip propagation of coherent light are demonstrated based on these single-crystalline microwires. These findings open an avenue for on-chip integration of single-crystalline materials.

7.
Small ; 19(11): e2206938, 2023 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-36642796

RESUMO

Organic flexible electronic devices are at the forefront of the electronics as they possess the potential to bring about a major lifestyle revolution owing to outstanding properties of organic semiconductors, including solution processability, lightweight and flexibility. For the integration of organic flexible electronics, the precise patterning and ordered assembly of organic semiconductors have attracted wide attention and gained rapid developments, which not only reduces the charge crosstalk between adjacent devices, but also enhances device uniformity and reproducibility. This review focuses on recent advances in the design, patterned assembly of organic semiconductors, and flexible electronic devices, especially for flexible organic field-effect transistors (FOFETs) and their multifunctional applications. First, typical organic semiconductor materials and material design methods are introduced. Based on these organic materials with not only superior mechanical properties but also high carrier mobility, patterned assembly strategies on flexible substrates, including one-step and two-step approaches are discussed. Advanced applications of flexible electronic devices based on organic semiconductor patterns are then highlighted. Finally, future challenges and possible directions in the field to motivate the development of the next generation of flexible electronics are proposed.

8.
Small ; 18(41): e2203429, 2022 10.
Artigo em Inglês | MEDLINE | ID: mdl-36084233

RESUMO

Flexible organic near-infrared (NIR) phototransistors hold promising prospects for potential applications such as noninvasive bioimaging, health monitoring, and biometric authentication. For integrated circuits of high-performance devices, organic single-crystalline micro-/nanostructures with precise positioning are prominently anticipated. However, the manufacturing of organic single-crystalline arrays remains a conundrum due to difficulties encountered in patterning arrays of dewetting processes at micron-scale confined space and modulating the dewetting dynamics. Herein, we utilize a capillary-bridge lithography strategy to fabricate organic 1D arrays with high quality, homogeneous size, and deterministic location toward high-performance flexible organic NIR phototransistors. Regular micro-liquid stripes and unidirectional dewetting are synchronously achieved by adapting micropillar templates with asymmetric wettability. As a result, high-throughput 1D arrays based organic field-effect transistors exhibit high electron mobility up to 9.82 cm2  V-1  s-1 . Impressively, flexible NIR phototransistors also show outstanding photoelectronic performances with a photosensitivity of 9.87 × 105 , a responsivity of 1.79 × 104  A W-1 , and a specific detectivity of 3.92 × 1014 Jones. This work paves a novel way to pattern high-throughput organic single-crystalline microarrays toward flexible NIR organic optoelectronics.


Assuntos
Molhabilidade
9.
Nanoscale Adv ; 4(11): 2399-2411, 2022 May 31.
Artigo em Inglês | MEDLINE | ID: mdl-36134127

RESUMO

Organic ultrathin semiconductor nanostructures have attracted continuous attention in recent years owing to their excellent charge transport capability, favorable flexibility, solution-processability and adjustable photoelectric properties, providing opportunities for next-generation optoelectronic applications. For integrated electronics, organic ultrathin nanostructures need to be prepared as large-area patterns with precise alignment and high crystallinity to achieve organic electronic devices with high performance and high throughput. However, the fabrication of organic ultrathin nanostructure arrays still remains challenging due to uncontrollable growth along the height direction in solution processes. In this review, we first introduce the properties, assembly methods and applications of four typical organic ultrathin nanostructures, including small molecules, polymers, and other organic-inorganic hybrid materials. Five categories of representative solution-processing techniques for patterning organic micro- and nanostructures are summarized and discussed. Finally, challenges and perspectives in the controllable preparation of organic ultrathin arrays and potential applications are featured on the basis of their current development.

10.
ACS Appl Mater Interfaces ; 14(36): 41257-41263, 2022 Sep 14.
Artigo em Inglês | MEDLINE | ID: mdl-36044649

RESUMO

Polymer micro/nanoarchitectures have attracted intense interest for wearable medical applications due to their excellent mechanical flexibility, solution processability, and tunable optoelectronic properties. Based on polymer micro/nanostructures, high-performance ultraviolet (UV) photodetectors can not only functionalize the accurate image sensing but also sustain the biocomfortable flexible devices for real-time health monitoring. The main challenges are focused on the integration of medical wearable devices, which requires large-scale assembly of polymer micro/nanostructures with controlled morphology and strict alignment. Herein, we utilized a confined assembly system through the cautious regulation for the growth of high-quality polymer 1D arrays. UV photodetectors based on these polymer microwire arrays perform a high on/off ratio of 137 and responsivity of 19.1 mA W-1. Polymer microarray photodetectors facilitate the scale-up fabrication of 14 × 18 multiplexed image sensors for highly accurate capturing the signals of Arabic numerals "1," "2," and "3." Flexible UV photodetectors based on these arrays present excellent flexibility and bending durability, maintaining 97% of their original on/off ratio after 4000 cycles with a 10 mm bending radius. UV photodetection signals were also collected from the attached flexible devices on the back skin of the mouse, demonstrating the great potential in wearable medical photodetection.


Assuntos
Nanoestruturas , Dispositivos Eletrônicos Vestíveis , Animais , Camundongos , Nanoestruturas/química , Polímeros/química
11.
ACS Appl Mater Interfaces ; 14(28): 32761-32770, 2022 Jul 20.
Artigo em Inglês | MEDLINE | ID: mdl-35816371

RESUMO

Patterning organic semiconductors directly on Au electrodes possesses the advantages of eliminating metal atomic penetration effect, compatibility with fine lithography processes, and feasibility of work function modification on electrodes, and it is therefore of value in the commercial manufacturability application of optoelectronic devices with low cost, large scale, and high efficiency. Solution processing, is relatively inexpensive and is scalable to large areas. Nonetheless, conventional solution processing approaches have trade-offs among controllable morphology, regular alignment, precise position, and ordered molecular packing arising from the uncontrollable dewetting kinetics. Here, one-step patterning of 1D polymer nanowire arrays directly on Au source-drain electrodes with precise position, controlled orientation, regulated distribution, and tunable width size were realized by employing a capillary-bridge manipulation method to guide the processes of liquid dewetting and nanowire assembly. Organic field-effect transistors (OFETs) with mobility of 10.1 cm2 V-1 s-1 and on/off current ratio of 1.9 × 104 were fabricated. Moreover, we verified generality of our method by patterning different solution-processable optoelectronic materials, including small molecules, quantum dot (QD) nanoparticles, and metal-halide perovskites, into ordered structures directly on the target substrate. The work provides a novel insight into efficient manufacturing the regular aligned and precisely positioned 1D organic semiconductors directly on the channel region of prefabricated Au electrodes in one step and facilitates their applications in high-performance electronic devices.

12.
Adv Mater ; 34(28): e2202119, 2022 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-35522854

RESUMO

Long-range-ordered structures of nanoparticles with controllable orientation have advantages in applications toward sensors, photoelectric conversion, and field-effect transistors. The assembly process of nanorods in colloidal systems undergoes a nonequilibrium process from dispersion to aggregation. A variety of assembly methods such as solvent volatilization, electromagnetic field induction, and photoinduction are restricted to suppress local perturbations during the nonequilibrium concentration of nanoparticles, which are adverse to controlling the orientation and order of assembled structures. Here, a confined assembly method is reported by locally controlling free-volume entropy in nonequilibrium fluids to fabricate microstructure arrays based on colloidal nanorods with controllable orientation and long-range order. The unique fluid dynamics of the liquid bridge is utilized to form a local region, where the free volume entropy reduction triggers assembly near the three-phase contact line (TPCL), allowing nanorods to assemble in 2D closest packing parallel to the TPCL for the maximum Gibbs free energy reduction. By manipulating the orientation of liquid flow, microstructures are assembled with programmable geometry, which sustains polarized photoluminescence and polarization-dependent photodetection. This confined assembly method opens up perspectives on assemblies of nanomaterials with controllable orientation and long-range order as a platform for multifunctional integrated devices.

13.
Adv Mater ; 34(11): e2108279, 2022 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-35023586

RESUMO

Large-scale assembly of organic micro/nanocrystals into well-defined patterns with programmable structures is essential for applications such as information encryption at both high data density and high security level. Here, a magnetic-field-assisted approach that produces programmable assemblies of organic microcrystals with various shapes and orientations, using the magnetic domains of the underlying ferromagnetic metal microarrays as the printing templates, is developed. The diamagnetic microcrystals tend to aggregate in the regions of minimal field strength, and thus their assembly behavior is precisely controlled by the local field distribution on top of magnetic domains on substrate. The dynamic assembly process of microcrystal assemblies can be programmed upon the sequence of applied field, and their shape changes are ≈100% reproducible on a large scale (>20 000 sites over 1 cm2 ). These features of magnetically programmable assemblies are ideally suited for information encryption, for which the encryption-decryption-erasing of multilevel information from a QR-code pattern based on the microcrystal assemblies under magnetic field is demonstrated.

14.
ACS Appl Mater Interfaces ; 14(1): 1601-1608, 2022 Jan 12.
Artigo em Inglês | MEDLINE | ID: mdl-34978173

RESUMO

Metal-halide layered perovskites, self-assembled quantum wells with alternating insulating interlayer organic cations, and conductive perovskite layers boost the incorporation of multiple functionalities into a single-phase material. Optoelectronic performances in layered perovskites are more sensitive to crystallinity than their 3D counterparts due to the traps and insulating barriers introduced by interlayer cations. Here, we combine the capillary-bridge lithography method for the fabrication of single-crystalline nanowire arrays with strongly interacted layered perovskites for the enhancement of crystallinity and crystallographic orientation purity. Due to regulated nucleation and growth of layered perovskites in capillary bridges and the sulfur-sulfur interaction between interlayer cations, nanowires with pure (101) orientation are realized for underpinning insulating crystal interiors and photoconductive layer edges. Based on these nanowires, ultrasensitive photodetectors are reached with an ultralow dark current of below 10-12 A, an average responsivity of 7.3 × 103 A W-1, an average specific detectivity of 3.9 × 1015 Jones, and a 3 dB bandwidth of 10.3 kHz.

15.
Nat Commun ; 12(1): 7038, 2021 Dec 02.
Artigo em Inglês | MEDLINE | ID: mdl-34857751

RESUMO

Organic semiconducting polymers have opened a new paradigm for soft electronics due to their intrinsic flexibility and solution processibility. However, the contradiction between the mechanical stretchability and electronic performances restricts the implementation of high-mobility polymers with rigid molecular backbone in deformable devices. Here, we report the realization of high mobility and stretchability on curvilinear polymer microstructures fabricated by capillary-gradient assembly method. Curvilinear polymer microstructure arrays are fabricated with highly ordered molecular packing, controllable pattern, and wafer-scale homogeneity, leading to hole mobilities of 4.3 and 2.6 cm2 V-1 s-1 under zero and 100% strain, respectively. Fully stretchable field-effect transistors and logic circuits can be integrated in solution process. Long-range homogeneity is demonstrated with the narrow distribution of height, width, mobility, on-off ratio and threshold voltage across a four-inch wafer. This solution-assembly method provides a platform for wafer-scale and reproducible integration of high-performance soft electronic devices and circuits based on organic semiconductors.

16.
ACS Appl Mater Interfaces ; 13(42): 50197-50205, 2021 Oct 27.
Artigo em Inglês | MEDLINE | ID: mdl-34652904

RESUMO

Structural design of organic π-conjugated small molecules allows the energy band structure and electronic properties of the molecules to be tuned as needed, which provides a feasible strategy for enhancing the performance of optoelectronic devices. The introduction of bridging structures is a common structural modification method to adjust the rigidity and coplanarity of the molecular backbone, thus affecting the molecular packing. However, patterning of organic single-crystalline microstructures based on conjugated ladder molecules with different bridging structures still remains challenging for large-area integration of optoelectronic devices. In this paper, a controlled dewetting process is applied to obtain organic single-crystalline arrays with precise positioning and a regular morphology based on two isomers with silicon-oxygen bridging and their two carbon-oxygen-bridged analogues. Molecules with different bridging structures show disparate packing models due to the difference of dihedral angles and ring tensions. A microwire-array ultraviolet photodetector based on the oxygen-silicon-bridging ladder molecule exhibits a high light on/off ratio of 24 and a responsivity of 0.63 mA W-1 owing to the effective π-π stacking governed by the molecular planarity. This work not only provides a universal method for the integration of organic optoelectronic devices but also explains the effect of bridging structure engineering on molecular assembly and optoelectronic performance.

17.
J Am Chem Soc ; 143(22): 8437-8445, 2021 Jun 09.
Artigo em Inglês | MEDLINE | ID: mdl-34000194

RESUMO

Structural engineering in multiple scales permits the integration of exotic properties into a single material, which boosts the development of ultracompact multifunctional devices. Layered perovskites are capable of cross-linking efficient carrier transport originating from few-layer perovskite frameworks with extended functionalities contributed by designable bulky organic cations and nanostructures, thus providing a platform for multiscale material engineering. Herein, high-performance Stokes-parameter photodetectors for arbitrary polarized light detection are realized on the basis of solution-processed chiral-perovskite nanowire arrays. The chiral ammonium cations intercalated between the perovskite layers are responsive to circularly polarized light with a maximum anisotropy factor of 0.15, while the strictly aligned nanowires with the anisotropic dielectric function result in a large polarized ratio of 1.6 to linearly polarized light. Single crystallinity and pure crystallographic orientation permit efficient in-plane carrier transport along the nanowires, yielding a responsivity of 47.1 A W-1 and a detectivity of 1.24 × 1013 Jones. By synergy of linear- and circular-polarization response with high optoelectronic performance for providing sufficient photocurrent contrasts, Stokes-parameter photodetection is demonstrated on these nanowires. Our Stokes-parameter photodetectors with a small footprint and high performances present promising applications toward polarization imaging.

18.
Small ; 17(21): e2100332, 2021 May.
Artigo em Inglês | MEDLINE | ID: mdl-33864427

RESUMO

Optoelectronic applications of organic semiconductors demand single-crystalline structures with long-range order and suppressed defects for sustaining efficient carrier transport and long photocarrier lifetime, which are pivotal in photodetection, photovoltaic, and light emission. For integrated devices, an additional requirement of precise patterning is imposed, whereas the patterning of single-crystalline organic microstructures is still challenging because the molecular stacking is easily perturbed by disordered fluids in microdroplets. Herein, a capillary-bridge lithography is developed for driving the directional transport of capillary flows to control the confined crystallization of organic 1D single-crystalline arrays with aligned positioning and pure orientation. Through tuning the concentration and pressure, the size of organic 1D arrays in three dimensions can be controlled with 2.9-5.8 µm in width and 1.2 µm to 110 nm in height. Organic 1D array photodetectors exhibit a stable performance with on/off ratio of 180 and responsivity of 4.99 mA W-1 . Based on the scalable fabrication of 1D array photodetectors, 20 × 20 multiplexed image sensors with high accuracy are demonstrated for capturing the light signals of capital letter "A," "B," and "C." This research will open opportunities for the large-scale fabrication of organic single-crystalline semiconductors toward the integrated optoelectronic modules.

19.
Sci Total Environ ; 756: 144063, 2021 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-33288269

RESUMO

Coal-fired power plants are important sources of polycyclic aromatic hydrocarbon (PAH) emissions in the world. The effects of various air pollution control devices (APCDs) on PAH emissions were investigated by analyzing samples from inlets and outlets of APCDs in six coal-fired power plants (A-F) and two coal-fired industrial boilers (G and H). The APCDs were electrostatic precipitators (ESPs), wet flue gas desulfurization systems (WFGDs), and wet ESPs (WESPs). The PAH congener patterns for the coal-fired plants were similar. Gas-phase PAHs were dominant in flue gases, and the most abundant PAH was naphthalene. Three- and four-ring PAHs were dominant in fly ash. Positive correlations were found between the PAH and total organic carbon contents of fly ash (R2 0.87) and slag (R2 0.92). Plants D-F, equipped with low-low-temperature ESPs (LLT-ESPs) and WESPs discharged the lowest PAHs. Circulating water was an important source of PAHs in the desulfurization except in plant A, which used desalinated seawater rather than circulating water in the desulfurization process. WESPs decreased PAH concentrations by an average of 20.67%, which can be spread to other plants to reduce PAHs.

20.
Front Chem ; 8: 632, 2020.
Artigo em Inglês | MEDLINE | ID: mdl-33062630

RESUMO

Single-crystalline lead halide perovskites with remarkable physical properties offer great potential in integrated optoelectronic applications but are restricted by their instability and toxicity. To address these problems, various strategies including lead-free halide double perovskites with high stabilities of heat, light, and moisture have been developed. However, it still requires an efficient method to pattern single-crystalline, double-perovskite micro-/nanostructures with strict alignment and ordered orientation for the integration of optoelectronic devices. Here, our solution-processing approach employs capillary bridges to control the dewetting dynamics and confine the crystallization in the assembly of non-toxic Cs2AgBiBr6 microwire arrays. We demonstrate the strict alignment, high crystallinity, eliminated grain boundary, and ordered orientation of these as-prepared single-crystalline, double-perovskite microwire arrays. Based on these high-quality microwire arrays, we fabricate high-performance photodetectors with a responsivity of 1,625 A W-1, on/off ratio of 104, and fast response speed of τdecay = 0.04 ms and τrise = 0.28 ms. The long-term crystallographic and spectroscopic stability of Cs2AgBiBr6 microwire arrays has also been demonstrated through the 1 month exposure to air conditioning. Our strategy provides a new perception to fabricate stable perovskite microarrays for the integration of non-toxic optoelectronic devices.

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