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1.
Nanotechnology ; 31(33): 335602, 2020 May 05.
Artigo em Inglês | MEDLINE | ID: mdl-32369779

RESUMO

Deposition of layers of graphene on silicon has the potential for a wide range of optoelectronic and mechanical applications. However, direct growth of graphene on silicon has been difficult due to the inert, oxidized silicon surfaces. Transferring graphene from metallic growth substrates to silicon is not a good solution either, because most transfer methods involve multiple steps that often lead to polymer residues or degradation of sample quality. Here we report a single-step method for large-area direct growth of continuous horizontal graphene sheets and vertical graphene nano-walls on silicon substrates by plasma-enhanced chemical vapor deposition (PECVD) without active heating. Comprehensive studies utilizing Raman spectroscopy, x-ray/ultraviolet photoelectron spectroscopy (XPS/UPS), atomic force microscopy (AFM), scanning electron microscopy (SEM) and optical transmission are carried out to characterize the quality and properties of these samples. Data gathered by the residual gas analyzer (RGA) during the growth process further provide information about the synthesis mechanism. Additionally, ultra-low friction (with a frictional coefficient ∼0.015) on multilayer graphene-covered silicon surface is achieved, which is approaching the superlubricity limit (for frictional coefficients <0.01). Our growth method therefore opens up a new pathway towards scalable and direct integration of graphene into silicon technology for potential applications ranging from structural superlubricity to nanoelectronics, optoelectronics, and even the next-generation lithium-ion batteries.

2.
J Am Chem Soc ; 2020 Apr 07.
Artigo em Inglês | MEDLINE | ID: mdl-32223139

RESUMO

Dinuclear Pt(III) complexes were commonly reported to have short-lived lowest-lying triplet states, resulting in extremely weak or no photoluminescence. To overcome this obstacle, a new series of dinuclear Pt(III) complexes, named Pt2a-Pt2c, were strategically designed and synthesized using donor (D)-acceptor (A)-type oxadiazole-thiol chelates as bridging ligands. These dinuclear Pt(III) complexes possess a d7-d7 electronic configuration and exhibit intense phosphorescence under ambient conditions. Among them, Pt2a exhibits orange phosphorescence maximized at 618 nm in degassed dichloromethane solution (Φp ≈ 8.2%, τp ≈ 0.10 µs) and near-infrared (NIR) emission at 749 nm (Φp ≈ 10.1% τp ≈ 0.66 µs) in the crystalline powder and at 704 nm (Φp ≈ 33.1%, τp ≈ 0.34 µs) in the spin-coated neat film. An emission blue-shifted by more than 3343 cm-1 is observed under mechanically ground crystalline Pt2a, affirming intermolecular interactions in the solid states. Time-dependent density functional theory (TD-DFT) discloses the lowest-lying electronic transition of Pt2a-Pt2c complexes to be a bridging ligand-metal-metal charge transfer (LMMCT) transition. The long-lived triplet states of these dinuclear platinum(III) complexes may find potential use in lighting. Employing Pt2a as an emitter, high-performance organic light-emitting diodes (OLEDs) were fabricated with NIR emission at 716 nm (η = 5.1%), red emission at 614 nm (η = 8.7%), and white-light emission (η = 11.6%) in nondoped, doped (in mCP), and hybrid (in CzACSF) devices, respectively.

3.
ACS Appl Mater Interfaces ; 11(50): 47054-47062, 2019 Dec 18.
Artigo em Inglês | MEDLINE | ID: mdl-31762264

RESUMO

A sensitive and fast ultraviolet (UV) photodetector is strongly desirable because of its wide range of applications in chemical/biological sensing and imaging. CsPbCl3-based thin film photodetectors have not been constructed previously owing to their extremely poor precursor solubility; however, vapor deposition allows for thin film fabrication without the limitation of solubility. Therefore, this work is the first to demonstrate the optoelectronic properties of inorganic CsPbCl3 perovskite thin films and UV photodiodes using all-vacuum deposition. The perovskites annealed at 120 °C exhibited outstanding performance, including a notable external quantum efficiency value of 797.1% with an applied bias of -2 V, an outstanding detectivity of 1.4 × 1013 Jones, a short response time as low as ∼ 50 µs, and a large linear dynamic range of up to 136 dB. CsPbCl3 thin films manufactured by this vacuum-deposited approach were also found to be moisture-resistant and demonstrated high durability. The devices maintained excellent performance and demonstrated less than 10% degradation after 30 days. Thus, thin film visible-blind UV detectors can potentially be used in transparent smart displays, window-integrated electronic circuits, and sensor applications.

4.
Inorg Chem ; 58(20): 13892-13901, 2019 Oct 21.
Artigo em Inglês | MEDLINE | ID: mdl-31565936

RESUMO

Four diplatinum(II) complexes with the formula [Pt(pypm)(µ-Fn)]2 (2, 3a-c) bearing both a pyridine-pyrimidinate chelate and formamidinate bridge, where (pypm)H and FnH stand for 5-(pyridin-2-yl)-2-(trifluoromethyl)pyrimidine and functional formamidines with various substituents of iPr (n = 1), Ph (n = 2), C6H4tBu (n = 3), and C6H4CF3 (n = 4), were synthesized en route from a mononuclear intermediate represented by [Pt(pypm)Cl(F1H)] (1). Single-crystal X-ray diffraction studies confirmed the structure of 1 and 3a comprised of an individual "Pt(pypm)" unit and two "Pt(pypm)" units with a Pt···Pt distance of 2.8845(2) Å, respectively. Therefore, in contrast to the structured emission of mononuclear 1 with the first vibronic peak wavelength at 475 nm, all other diplatinum complexes with shortened Pt···Pt separation exhibited greatly red shifted and structureless metal-metal to ligand charge transfer (MMLCT) emission that extended into the near-infrared region in solid states. Their photophysical characteristics were measured under three distinctive morphological states (i.e., crystals, sublimed powders, and vacuum-deposited thin films) by steady-state UV-vis spectroscopy, while retention of Pt···Pt interactions in deposited thin films of 2 and 3a-c was confirmed using Raman spectroscopy, demonstrating lowered Pt···Pt stretching at 80-200 cm-1. Most importantly, complexes 3a-c exhibited a gradual red shift with the trends crystals < sublimed powders < vacuum-deposited thin films, a result of increased intermolecular π-π stacking interactions and Pt···Pt interactions, while crystalline samples exhibited the highest luminescence among all three morphological states due to the fewest defects in comparison to other morphologies. Finally, 3b was selected as a nondoped emitter for the fabrication of NIR-emitting OLEDs, giving an electroluminescence peak at 767 nm and a maximum external quantum efficiency of 0.14% with negligible roll-off.

5.
Opt Express ; 27(16): A1308-A1323, 2019 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-31510595

RESUMO

A simulation scheme was developed to explore the light distribution of full-color micron-scale light-emitting diode (LED) arrays. The influences of substrate thickness, patterning, and cutting angle of the substrate on several important features, such as light field pattern, light extraction efficiency, and color variation, were evaluated numerically. An experiment was conducted; the results were consistent with simulation results for a 225 × 125 µm2 miniLED and those for an 80 × 80 µm2 microLED. Based on the simulation results, the light extraction efficiency of LED devices with a substrate increases by 67.75% over the extraction efficiency of those without a substrate. The light extraction efficiency of LED devices with a substrate increases by 113.55% when an additional patterned design is used on green and blue chips. The calculated large angle Δu'v' can be as low as 0.015 for miniLED devices.

6.
ACS Appl Mater Interfaces ; 11(28): 25186-25194, 2019 Jul 17.
Artigo em Inglês | MEDLINE | ID: mdl-31268648

RESUMO

Tuning the electronic band structure of black titania to improve photocatalytic performance through conventional band engineering methods has been challenging because of the defect-induced charge carrier and trapping sites. In this study, KSCN-modified hydrogenated nickel nanocluster-modified black TiO2 (SCN-H-Ni-TiO2) exhibits enhanced photocatalytic CO2 reduction due to the interfacial dipole effect. Upon combining the experimental and theoretical simulation approach, the presence of an electrostatic interfacial dipole associated with chemisorption of SCN has dramatic effects on the photocatalyst band structure in SCN-H-Ni-TiO2. An interfacial dipole possesses a more negative zeta potential shift of the isoelectric point from 5.20 to 3.20, which will accelerate the charge carrier separation and electron transfer process. Thiocyanate ion passivation on black TiO2 demonstrated an increased work function around 0.60 eV, which was induced by the interracial dipole effect. Overall, the SCN-H-Ni-TiO2 photocatalyst showed an enhanced CO2 reduction to solar fuel yield by 2.80 times higher than H-Ni-TiO2 and retained around 88% product formation yield after 40 h.

7.
Sci Rep ; 8(1): 14859, 2018 Oct 05.
Artigo em Inglês | MEDLINE | ID: mdl-30291267

RESUMO

All-optical logics are realized on nanoscale SiC waveguides with add-drop micro-ring functionality, including the TE/TM polarized data decoding, the dual-port Kerr switching and gating beyond 12 Gbit/s. With employing the C-C bond enriched SiC thin film upon thermal oxide, the nonlinear refractive index of up to 2.44 × 10-12 cm2/W enables the asymmetric waveguide with polarization distinguishable transmission, which provides a polarization-selectivity to discreminate the TE/TM polarized data decoding with an nearly 9-dB extinction ratio. The TE/TM polarized decoding performance is comparable with a state-of-the-art fiberized in-line polarizer. The complementary transmission in the bus waveguide port facilitates the dual-port Kerr switching for data format conversion/inversion in both add/drop channels. Owing to the TE/TM polarization discriminated throughput, the asymmetric add-drop waveguide micro-ring also permits all-optical AND logic gating functions, where the ON-state outputs only if the pump bit is set at ON state and the probe bit with matched polarization. These results reveal the multi-functionality of the nanoscale SiC add-drop micro-ring waveguide for future photonic logics on chip.

8.
ACS Nano ; 12(10): 9721-9732, 2018 10 23.
Artigo em Inglês | MEDLINE | ID: mdl-30160102

RESUMO

Foundry-compatible materials and processing approaches serve as the foundations for advanced, active implantable microsystems that can dissolve in biofluids into biocompatible reaction products, with broad potential applications in biomedicine. The results reported here include in vitro studies of the dissolution kinetics and nanoscale bioresorption behaviors of device-grade thin films of Si, SiN x, SiO2, and W in the presence of dynamic cell cultures via atomic force microscopy and X-ray photoemission spectroscopy. In situ investigations of cell-extracellular mechanotransduction induced by cellular traction provide insights into the cytotoxicity of these same materials and of microcomponents formed with them using foundry-compatible processes, indicating potential cytotoxicity elicited by W at concentrations greater than 6 mM. The findings are of central relevance to the biocompatibility of modern Si-based electronics technologies as active, bioresorbable microsystems that interface with living tissues.


Assuntos
Materiais Biocompatíveis/farmacologia , Mecanotransdução Celular/efeitos dos fármacos , Compostos de Silício/farmacologia , Tungstênio/farmacologia , Materiais Biocompatíveis/química , Sobrevivência Celular/efeitos dos fármacos , Células Cultivadas , Humanos , Cinética , Microscopia de Força Atômica/instrumentação , Espectroscopia Fotoeletrônica/instrumentação , Semicondutores , Compostos de Silício/química , Tungstênio/química
9.
Nat Commun ; 9(1): 169, 2018 01 12.
Artigo em Inglês | MEDLINE | ID: mdl-29330430

RESUMO

Photocatalytic formation of hydrocarbons using solar energy via artificial photosynthesis is a highly desirable renewable-energy source for replacing conventional fossil fuels. Using an L-cysteine-based hydrothermal process, here we synthesize a carbon-doped SnS2 (SnS2-C) metal dichalcogenide nanostructure, which exhibits a highly active and selective photocatalytic conversion of CO2 to hydrocarbons under visible-light. The interstitial carbon doping induced microstrain in the SnS2 lattice, resulting in different photophysical properties as compared with undoped SnS2. This SnS2-C photocatalyst significantly enhances the CO2 reduction activity under visible light, attaining a photochemical quantum efficiency of above 0.7%. The SnS2-C photocatalyst represents an important contribution towards high quantum efficiency artificial photosynthesis based on gas phase photocatalytic CO2 reduction under visible light, where the in situ carbon-doped SnS2 nanostructure improves the stability and the light harvesting and charge separation efficiency, and significantly enhances the photocatalytic activity.

10.
Adv Mater ; 30(11)2018 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-29349821

RESUMO

Biodegradable electronic systems represent an emerging class of technology with unique application possibilities, from temporary biomedical implants to "green" consumer gadgets. This paper introduces materials and processing methods for 3D, heterogeneously integrated devices of this type, with various functional examples in sophisticated forms of silicon-based electronics. Specifically, techniques for performing multilayer assembly by transfer printing and for fabricating layer-to-layer vias and interconnects by lithographic procedures serve as routes to biodegradable, 3D integrated circuits composed of functional building blocks formed using specialized approaches or sourced from commercial semiconductor foundries. Demonstration examples range from logic gates and analog circuits that undergo functional transformation by transience to systems that integrate multilayer resistive sensors for in situ, continuous electrical monitoring of the processes of transience. The results significantly expand the scope of engineering options for biodegradable electronics and other types of transient microsystem technologies.


Assuntos
Implantes Absorvíveis , Impressão , Semicondutores , Silício
11.
Small ; 14(2)2018 01.
Artigo em Inglês | MEDLINE | ID: mdl-29134759

RESUMO

One of the key challenges in artificial photosynthesis is to design a photocatalyst that can bind and activate the CO2 molecule with the smallest possible activation energy and produce selective hydrocarbon products. In this contribution, a combined experimental and computational study on Ni-nanocluster loaded black TiO2 (Ni/TiO2[Vo] ) with built-in dual active sites for selective photocatalytic CO2 conversion is reported. The findings reveal that the synergistic effects of deliberately induced Ni nanoclusters and oxygen vacancies provide (1) energetically stable CO2 binding sites with the lowest activation energy (0.08 eV), (2) highly reactive sites, (3) a fast electron transfer pathway, and (4) enhanced light harvesting by lowering the bandgap. The Ni/TiO2[Vo] photocatalyst has demonstrated highly selective and enhanced photocatalytic activity of more than 18 times higher solar fuel production than the commercial TiO2 (P-25). An insight into the mechanisms of interfacial charge transfer and product formation is explored.

12.
Sci Rep ; 7(1): 16857, 2017 12 04.
Artigo em Inglês | MEDLINE | ID: mdl-29203831

RESUMO

In this work, we demonstrate for the first time an ultra-low contact resistance few-layered black phosphorus (BP) transistor with metallic PGex contacts formed by rapid thermal annealing (RTA). The on-state current of the transistor can be significantly improved and the ION/IOFF ratio increases by almost 2 order. The hole mobility is enhanced by 25 times to 227 cm2V-1s-1. The contact resistance extracted by the transfer length method is 0.365 kΩ∙µm, which is the lowest value in black phosphorus transistors without degradation of ION/IOFF ratio. In addition, the I-V curve of the transistor with PGex contact is linear compared to that with Ti contact at 80 K, indicating that a metallic ohmic contact is successfully formed. Finally, X-ray photoelectron spectroscopy is used to characterize the PGex compound. A signal of P-Ge bond is first observed, further verifying the doping of Ge into BP and the formation of the PGex alloy.

13.
Nanoscale ; 9(48): 19227-19235, 2017 Dec 14.
Artigo em Inglês | MEDLINE | ID: mdl-29188264

RESUMO

We report the long-term stability of water-sensitive hybrid perovskites CH3NH3PbI3 that were protected with monolayer graphene. This successful passivation was enabled by our development of a new water-free and polymer-free graphene transfer method. Monolayer graphene samples grown by plasma-enhanced chemical vapor deposition and transferred onto different substrates with the water/polymer-free method were found to preserve their high-quality characteristics after the transfer, as manifested by the studies of Raman, X-ray and ultraviolet photoemission spectroscopy (XPS and UPS), optical absorption, and sheet resistance. Additionally, XPS, UPS and optical absorption studies of fully graphene-covered CH3NH3PbI3 thin films showed spectral invariance even after 3 months, which was in sharp contrast to the drastic spectral changes after merely one week in control CH3NH3PbI3 samples without graphene protection. This successful demonstration of the graphene-enabled passivation and long-term stability of CH3NH3PbI3 thin films therefore opens up a new pathway towards realistic photovoltaic applications of hybrid perovskites.

14.
Nanomaterials (Basel) ; 7(11)2017 Nov 10.
Artigo em Inglês | MEDLINE | ID: mdl-29125567

RESUMO

Gold-nanoparticle (Au-NP) non-volatile memories (NVMs) with low-damage CF4 plasma treatment on the blocking oxide (BO) layer have been investigated to present the gate injection of the holes. These holes, injected from the Al gate with the positive gate bias, were explained by the bandgap engineering of the gradually-fluorinated BO layer and the effective work function modulation of the Al gate. The Si-F complex in the BO layer was analyzed by X-ray photoelectron spectroscopy (XPS), while the depth of fluorine incorporation was verified using a secondary ion mass spectrometer (SIMS). In addition, the valence band modification of the fluorinated BO layer was examined by ultraviolet photoelectron spectroscopy (UPS) to support the bandgap engineering. The reactive power of the CF4 plasma treatment on the BO layer was modified to increase the electric field of the BO layer and raise the effective work function of the Al gate, leading to the hole-injection from the gate. The injected holes are trapped at the interface between the gold-nanoparticles (Au-NPs) and the tunneling oxide (TO) layer, resulting in superior data retention properties such as an extremely low charge loss of 5.7% at 104 s and a nearly negligible increase in charge loss at 85 °C of the CF4-plasma-treated Au-NP NVMs, which can be applied in highly reliable consumer electronics.

15.
Small ; 13(22)2017 06.
Artigo em Inglês | MEDLINE | ID: mdl-28401749

RESUMO

Interfacial engineering of perovskite solar cells (PSCs) is attracting intensive attention owing to the charge transfer efficiency at an interface, which greatly influences the photovoltaic performance. This study demonstrates the modification of a TiO2 electron-transporting layer with various amino acids, which affects charge transfer efficiency at the TiO2 /CH3 NH3 PbI3 interface in PSC, among which the l-alanine-modified cell exhibits the best power conversion efficiency with 30% enhancement. This study also shows that the (110) plane of perovskite crystallites tends to align in the direction perpendicular to the amino-acid-modified TiO2 as observed in grazing-incidence wide-angle X-ray scattering of thin CH3 NH3 PbI3 perovskite film. Electrochemical impedance spectroscopy reveals less charge transfer resistance at the TiO2 /CH3 NH3 PbI3 interface after being modified with amino acids, which is also supported by the lower intensity of steady-state photoluminescence (PL) and the reduced PL lifetime of perovskite. In addition, based on the PL measurement with excitation from different side of the sample, amino-acid-modified samples show less surface trapping effect compared to the sample without modification, which may also facilitate charge transfer efficiency at the interface. The results suggest that appropriate orientation of perovskite crystallites at the interface and trap-passivation are the niche for better photovoltaic performance.

16.
Sci Rep ; 7: 46281, 2017 04 19.
Artigo em Inglês | MEDLINE | ID: mdl-28422117

RESUMO

In this work, graphene-methylammonium lead iodide (MAPbI3) perovskite hybrid phototransistors fabricated by sequential vapor deposition are demonstrated. Ultrahigh responsivity of 1.73 × 107 A W-1 and detectivity of 2 × 1015 Jones are achieved, with extremely high effective quantum efficiencies of about 108% in the visible range (450-700 nm). This excellent performance is attributed to the ultra-flat perovskite films grown by vapor deposition on the graphene sheets. The hybrid structure of graphene covered with uniform perovskite has high exciton separation ability under light exposure, and thus efficiently generates photocurrents. This paper presents photoluminescence (PL) images along with statistical analysis used to study the photo-induced exciton behavior. Both uniform and dramatic PL intensity quenching has been observed over entire measured regions, consistently demonstrating excellent exciton separation in the devices.

17.
ChemSusChem ; 9(12): 1433-41, 2016 06 22.
Artigo em Inglês | MEDLINE | ID: mdl-27213296

RESUMO

Two donor-acceptor-acceptor (D-A-A)-type molecules incorporating nitrobenzoxadiazole (NBO) as the A-A block and ditolylamine as the D block bridged through a phenylene (PNBO) and a thiophene (TNBO) spacer were synthesized in a one-step coupling reaction. Their electronic, photophysical, and thermal properties; crystallographic analysis; and theoretical calculations were studied to establish a clear structure-property relationship. The results indicate that the quinoidal character of the thiophene bridge strongly governs the structural features and crystal packings (herringbone vs. brickwork) and thus the physical properties of the compounds. PNBO and TNBO were utilized as electron donors combined with C70 as the electron acceptor in the active layer of vacuum-processed bulk heterojunction small-molecule organic solar cells (SMOSCs). The power conversion efficiency of both PNBO- and TNBO-based OSCs exceeded 5 %. The ease of accessibility of PNBO and TNBO demonstrates the potential for simple and economical synthesis of electron donors in vacuum-processed SMOSCs.


Assuntos
Benzeno/química , Fontes de Energia Elétrica , Dióxido de Nitrogênio/química , Energia Solar , Tiofenos/química , Eletroquímica , Transporte de Elétrons , Modelos Moleculares , Conformação Molecular , Teoria Quântica , Temperatura
19.
Opt Express ; 24(2): A414-23, 2016 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-26832593

RESUMO

In this work, we investigate blade-coated organic interlayers at the rear surface of hybrid organic-silicon photovoltaics based on two small molecules: Tris(8-hydroxyquinolinato) aluminium (Alq(3)) and 1,3-bis(2-(4-tert-butylphenyl)-1,3,4-oxadiazol-5-yl) benzene (OXD-7). In particular, soluble Alq(3) resulting in a uniform thin film with a root-mean-square roughness < 0.2nm is demonstrated for the first time. Both devices with the Alq(3) and OXD-7 interlayers show notable enhancement in the open-circuit voltage and fill-factor, leading to a net efficiency increase by over 2% from the reference, up to 11.8% and 12.5% respectively. The capacitance-voltage characteristics confirm the role of the small-molecule interlayers resembling a thin interfacial oxide layer for the Al-Si Schottky barrier to enhance the built-in potential and facilitate charge transport. Moreover, the Alq(3) interlayer in optimized devices exhibits isolated phases with a large surface roughness, in contrast to the OXD-7 which forms a continuous uniform thin film. The distinct morphological differences between the two interlayers further suggest different enhancement mechanisms and hence offer versatile functionalities to the advent of hybrid organic-silicon photovoltaics.

20.
Nanoscale ; 8(8): 4579-87, 2016 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-26842460

RESUMO

The catalytic solid-phase synthesis of self-organized nanoporous tin sulfide (SnS) with enhanced absorption, manipulative transmittance and depolarization features is demonstrated. Using an ultralow radio-frequency (RF) sputtering power, the variation of the orientation angle between the anodized aluminum oxide (AAO) membrane and the axis of the sputtered ion beam detunes the catalytically synthesized SnS from nanorod to nanoporous morphology, along the sidewall of the AAO membrane. The ultraslow catalytic sputtering synthesis on the AAO at the RF plasma power of 20 W and the orientation angle of 0° regulates the porosity and integrality of nanoporous SnS, with average pore diameter of 80-150 nm. When transferring from planar to nanoporous structure, the phase composition changes from SnS to SnS2-Sn2S3, and the optical bandgap shrinks from 1.43 to 1.16 eV, due to the preferred crystalline orientation, which also contributes to an ultralow reflectance of <1% at 200-500 nm when both the transmittance and the surface scattering remain at their maxima. The absorption coefficient is enhanced by nearly one order of magnitude with its minimum of >5 × 10(4) cm(-1) at the wavelength between 200 and 700 nm, due to the red-shifting of the absorption spectrum to at least 100 nm. The catalytically self-organized nanoporous SnS causes strong haze and beam divergence of 20°-30° by depolarized nonlinear scattering at the surface, which favors the solar energy conversion with reduced surface reflection and enhanced photon scattering under preserved transmittance.

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