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1.
ACS Nano ; 15(10): 15667-15675, 2021 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-34495639

RESUMO

Next-generation devices and systems require the development and integration of advanced materials, the realization of which inevitably requires two separate processes: property engineering and patterning. Here, we report a one-step, ink-lithography technique to pattern and engineer the properties of thin films of colloidal nanocrystals that exploits their chemically addressable surface. Colloidal nanocrystals are deposited by solution-based methods to form thin films and a local chemical treatment is applied using an ink-printing technique to simultaneously modify (i) the chemical nature of the nanocrystal surface to allow thin-film patterning and (ii) the physical electronic, optical, thermal, and mechanical properties of the nanocrystal thin films. The ink-lithography technique is applied to the library of colloidal nanocrystals to engineer thin films of metals, semiconductors, and insulators on both rigid and flexible substrates and demonstrate their application in high-resolution image replications, anticounterfeit devices, multicolor filters, thin-film transistors and circuits, photoconductors, and wearable multisensors.

2.
Nature ; 597(7877): 503-510, 2021 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-34552257

RESUMO

Large, distributed collections of miniaturized, wireless electronic devices1,2 may form the basis of future systems for environmental monitoring3, population surveillance4, disease management5 and other applications that demand coverage over expansive spatial scales. Aerial schemes to distribute the components for such networks are required, and-inspired by wind-dispersed seeds6-we examined passive structures designed for controlled, unpowered flight across natural environments or city settings. Techniques in mechanically guided assembly of three-dimensional (3D) mesostructures7-9 provide access to miniature, 3D fliers optimized for such purposes, in processes that align with the most sophisticated production techniques for electronic, optoelectronic, microfluidic and microelectromechanical technologies. Here we demonstrate a range of 3D macro-, meso- and microscale fliers produced in this manner, including those that incorporate active electronic and colorimetric payloads. Analytical, computational and experimental studies of the aerodynamics of high-performance structures of this type establish a set of fundamental considerations in bio-inspired design, with a focus on 3D fliers that exhibit controlled rotational kinematics and low terminal velocities. An approach that represents these complex 3D structures as discrete numbers of blades captures the essential physics in simple, analytical scaling forms, validated by computational and experimental results. Battery-free, wireless devices and colorimetric sensors for environmental measurements provide simple examples of a wide spectrum of applications of these unusual concepts.

3.
ACS Nano ; 15(5): 8120-8129, 2021 May 25.
Artigo em Inglês | MEDLINE | ID: mdl-33792304

RESUMO

In this study, non-temperature interference strain gauge sensors, which are only sensitive to strain but not temperature, are developed by engineering the properties and structure from a material perspective. The environmental interference from temperature fluctuations is successfully eliminated by controlling the charge transport in nanoparticles with thermally expandable polymer substrates. Notably, the negative temperature coefficient of resistance (TCR), which originates from the hopping transport in nanoparticle arrays, is compensated by the positive TCR of the effective surface thermal expansion with anchoring effects. This strategy successfully controls the TCR from negative to positive. A near-zero TCR (NZTCR), less than 1.0 × 10-6 K-1, is achieved through precisely controlled expansion. Various characterization methods and finite element and transport simulations are conducted to investigate the correlated electrical, mechanical, and thermal properties of the materials and elucidate the compensated NZTCR mechanism. With this strategy, an all-solution-processed, transparent, highly sensitive, and noninterference strain sensor is fabricated with a gauge factor higher than 5000 at 1% strain, as demonstrated by pulse and motion sensing, as well as the noninterference property under variable-temperature conditions. It is envisaged that the sensor developed herein is applicable to multifunctional wearable sensors or e-skins for artificial skin or robots.

4.
Adv Mater ; 33(20): e2007346, 2021 May.
Artigo em Inglês | MEDLINE | ID: mdl-33739558

RESUMO

Soft neuroprosthetics that monitor signals from sensory neurons and deliver motor information can potentially replace damaged nerves. However, achieving long-term stability of devices interfacing peripheral nerves is challenging, since dynamic mechanical deformations in peripheral nerves cause material degradation in devices. Here, a durable and fatigue-resistant soft neuroprosthetic device is reported for bidirectional signaling on peripheral nerves. The neuroprosthetic device is made of a nanocomposite of gold nanoshell (AuNS)-coated silver (Ag) flakes dispersed in a tough, stretchable, and self-healing polymer (SHP). The dynamic self-healing property of the nanocomposite allows the percolation network of AuNS-coated flakes to rebuild after degradation. Therefore, its degraded electrical and mechanical performance by repetitive, irregular, and intense deformations at the device-nerve interface can be spontaneously self-recovered. When the device is implanted on a rat sciatic nerve, stable bidirectional signaling is obtained for over 5 weeks. Neural signals collected from a live walking rat using these neuroprosthetics are analyzed by a deep neural network to predict the joint position precisely. This result demonstrates that durable soft neuroprosthetics can facilitate collection and analysis of large-sized in vivo data for solving challenges in neurological disorders.


Assuntos
Nervo Isquiático , Animais , Eletrodos Implantados , Nanocompostos , Polímeros , Ratos
5.
ACS Appl Mater Interfaces ; 13(5): 6394-6403, 2021 Feb 10.
Artigo em Inglês | MEDLINE | ID: mdl-33512146

RESUMO

In this study, a self-sorting sensor was developed with the ability to distinguish between different pressure regimes and translate the pressure to electrical signals. Specifically, the self-sorting sensor can distinguish between soft and hard pressure like the human skin, without any software assistance and complicated circuits. To achieve the self-sorting property, Janus-like jagged structures were prepared via an all-solution process of spontaneous chemical patterning; they comprised electrically semi-insulating vertices and highly conductive valleys. This unique structure facilitates the detection and determination of the intensities and types of pressure by providing a significant gap between the current levels of two types of states, similar to the function of fibers in the human tactile system. The fabricated sensors also exhibit high sensitivity and durability as well as low power consumption, as demonstrated by the electronic skin and ternary Morse signal applications. Compared with conventional wearable pressure sensors, this sensor can detect signals without additional programming; thus, it is highly suitable for delay-sensitive, energy-efficient sensor applications such as driverless vehicles, autonomous artificial intelligence technology, and prosthetic devices.


Assuntos
Inteligência Artificial , Nanopartículas/química , Tato , Dispositivos Eletrônicos Vestíveis , Condutividade Elétrica , Humanos , Tamanho da Partícula , Propriedades de Superfície
6.
ACS Appl Mater Interfaces ; 12(49): 54763-54772, 2020 Dec 09.
Artigo em Inglês | MEDLINE | ID: mdl-33251797

RESUMO

In this study, multifunctional light-emitting and passive radiative cooling (LEPC) materials and devices are designed by embedding chemically designed perovskite nanocrystals (NCs) into the radiative polymer layer. Lead halide perovskite NCs are chosen as the light-emitting material, owing to their high photon radiation rate and low phonon generation. To integrate the perovskite NCs into the radiative polymer layers, a surface passivation is achieved by coating the NCs with silica. The silica shell synergistically improves the chemical stability and cooling efficiency. Both outdoor experimental and simulation results demonstrate that the fabricated LEPC devices show better cooling performance than conventional cooling devices. The LEPC devices are easily patterned by utilizing pixelating, assembling, and simple cutting or drawing techniques with the LEPC materials. This study also demonstrates the potential applications of these materials as components of smart building systems, in smart window displays, or for anticounterfeiting cooling systems, thus proving the practicality of these multifunctional LEPC devices.

7.
Nanoscale Horiz ; 5(6): 960-970, 2020 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-32266901

RESUMO

Post-synthesis engineering methods that employ oriented attachment to precisely control the size and dimensionality (0D/1D/2D) of as-synthesized CsPbBr3 nanocrystals (NCs) are demonstrated. We investigated the chemical effects of the properties of polar solvents, including their immiscibility, polarity, and boiling point, on the surfaces of NCs, as well as their effect on the structural and optical properties of NCs. Appropriate exploitation of the solvent properties made it possible to use a polar solvent to mildly affect the NCs indirectly such that they discarded their ligands and became attached to proximal NCs without being destroyed. Based on our observations, we developed a method whereby a solution of the NCs in a non-polar solvent is mixed with a polar solvent to form an immiscible phase to induce epitaxial growth of CsPbBr3 NCs. The method enables the size of NCs to be easily regulated from 5 to 50 nm by controlling the engineering time. Taking advantage of the minimal effect of a mild solvent, we also developed a self-assembly method that operates at the liquid-air interface to systematically control the dimensionality. At this interface, the NCs self-assemble in the horizontal direction and grow into micron-sized, single-crystalline, defect-free nanowires (1D) and nanoplates (2D) via oriented attachment. Finally, we discuss the origin of the non-destructive oriented attachment phenomenon and the surface chemistry of a perovskite NC using density functional theory (DFT) simulations and a proposed model system.

8.
Nanoscale ; 11(37): 17498-17505, 2019 Oct 07.
Artigo em Inglês | MEDLINE | ID: mdl-31532437

RESUMO

The popularity of colloidal quantum dot (CQD) solar cells has increased owing to their tunable bandgap, multiple exciton generation, and low-cost solution processes. ZnO nanoparticle (NP) layers are generally employed as electron transport layers in CQD solar cells to efficiently extract the electrons. However, trap sites and the unfavorable band structure of the as-synthesized ZnO NPs have hindered their potential performance. Herein, we introduce a facile method of ZnO NP annealing in the colloidal state. Electrical, structural, and optical analyses demonstrated that the colloidal-annealing of ZnO NPs effectively passivated the defects and simultaneously shifted their band diagram; therefore, colloidal-annealing is a more favorable method as compared to conventional film-annealing. These CQD solar cells based on colloidal-annealed ZnO NPs exhibited efficient charge extraction, reduced recombination and achieved an enhanced power conversion efficiency (PCE) of 9.29%, whereas the CQD solar cells based on ZnO NPs without annealing had a PCE of 8.05%. Moreover, the CQD solar cells using colloidal-annealed ZnO NPs exhibited an improved air stability with 98% retention after 120 days, as compared to that of CQD solar cells using non-annealed ZnO NPs with 84% retention.

9.
Nano Converg ; 6(1): 10, 2019 Apr 02.
Artigo em Inglês | MEDLINE | ID: mdl-30937630

RESUMO

In recent times, wearable sensors have attracted significant attention in various research fields and industries. The rapid growth of the wearable sensor related research and industry has led to the development of new devices and advanced applications such as bio-integrated devices, wearable health care systems, soft robotics, and electronic skins, among others. Nanocrystals (NCs) are promising building blocks for the design of novel wearable sensors, due to their solution processability and tunable properties. In this paper, an overview of NC synthesis, NC thin film fabrication, and the functionalization of NCs for wearable applications (strain sensors, pressure sensors, and temperature sensors) are provided. The recent development of NC-based strain, pressure, and temperature sensors is reviewed, and a discussion on their strategies and operating principles is presented. Finally, the current limitations of NC-based wearable sensors are discussed, in addition to methods to overcome these limitations.

10.
ACS Appl Mater Interfaces ; 10(43): 37643-37650, 2018 Oct 31.
Artigo em Inglês | MEDLINE | ID: mdl-30288975

RESUMO

We introduce solution-based, room temperature- and atmospheric pressure-processed silver nanocrystal (Ag NC)-based electrical circuits and interconnects for radio frequency (RF)/microwave frequency applications. We chemically designed the surface and interface states of Ag NC thin films to achieve high stability, dc and ac conductivity, and minimized RF loss through stepwise ligand exchange, shell coating, and surface cleaning. The chemical and structural properties of the circuits and interconnects affect the high-frequency electrical performance of Ag NC thin films, as confirmed by high-frequency electromagnetic field simulations. An all solution-based process is developed to build coplanar structures, in which Ag NC thin films are positioned at both sides of the substrates. In addition, we fabricated flexible transmission lines and broadband electrical circuits for resistors, interdigitated capacitors, spiral and omega-shaped inductors, and patch antennas with maximum inductance and capacitance values of 3 nH and 2.5 pF at frequencies up to 20 GHz. We believe that our approach will lead to a cost-effective realization of RF circuits and devices in which sensing and wireless communication capabilities are combined for internet-of-things applications.

11.
Nanoscale ; 10(38): 18415-18422, 2018 Oct 04.
Artigo em Inglês | MEDLINE | ID: mdl-30256372

RESUMO

In this work, we introduce a low cost, room-temperature and atmospheric pressure based chemical method to produce highly transparent, conductive, and flexible nano-mesh structured electrodes using Ag nanocrystals (NCs). Sequential treatments of ligand exchange and reduction processes were developed to engineer the optoelectronic properties of Ag NC thin films. Combinatorial analysis indicates that the origin of the relatively low conductivity comes from the non-metallic compounds that are introduced during ligand exchange. The reduction process successfully removed these non-metallic compounds, yielding structurally uniform, optically more transparent, dispersive, and electrically more conductive thin films. We optimized the design of Ag NC thin film mesh structures, and achieved low sheet resistance (9.12 Ω â–¡-1), high optical transmittance (94.7%), and the highest figure of merit (FOM) of 6.37 × 10-2. Solution processed flexible transparent heaters, touch pads, and wearable sensors are demonstrated, emphasizing the potential applications of Ag NC transparent electrodes in multifunctional sensors and devices.

12.
ACS Appl Mater Interfaces ; 10(30): 25502-25510, 2018 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-29968456

RESUMO

Ligand exchange is an advanced technique for tuning the various properties of nanocrystal (NC) thin films, widely used in the NC thin-film device applications. Understanding how the NC thin films transform into functional thin-film devices upon ligand exchange is essential. Here, we investigated the process of structural transformation and accompanying property changes in the NC thin films, by monitoring the various characteristics of silver (Ag) NC thin films at each stage of the ligand-exchange process. A transition state was identified in which the ligands are partially exchanged, where the NC thin films showed unexpected electromechanical features with high gauge factors up to 300. A model system was established to explain the origin of the high gauge factors, supported by the observation of spontaneously formed nanocracks and metal-insulator transition from the structural analysis and charge transport study, respectively. Taking advantages of the unique electromechanical properties of the NC thin films, we fabricated flexible strain gauge sensor devices with high sensitivity, reliability, and stability. We introduce a one-step fabrication process, namely, "the time- and spatial-selective ligand-exchange process", for the design of low-cost and high-performance wearable sensors that effectively detect human motion, such as finger or neck muscle movement. This study provides a fundamental understanding of the ligand-exchange process in NCs, as well as an insight into the functionalities of the NC thin films for technological applications.


Assuntos
Nanopartículas , Humanos , Movimento (Física) , Reprodutibilidade dos Testes , Prata , Dispositivos Eletrônicos Vestíveis
13.
ACS Appl Mater Interfaces ; 10(30): 25652-25659, 2018 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-29979023

RESUMO

We developed a simple and systematic method to fabricate optically tunable and thermally and chemically stable Au-Ag nanocrystal-based plasmonic metamaterials. An Ag nanocrystal-based metamaterial with desirable optical properties was fabricated via nanoimprinting and ligand-exchange process. Its optical properties were controlled by selectively substituting Ag atoms with Au atoms through a spontaneous galvanic replacement reaction. The developed Au-Ag-based metamaterials provide excellent tunable plasmonic properties required for various applications in the visible and near-infrared regions by controlling the Au-Ag composition according to the conditions of the galvanic displacement. Furthermore, their thermal and chemical stabilities significantly improved because of the protective Au thin layer on the surface. Using this developed process, chemically and thermally stable and flexible plasmonic metamaterials were successfully fabricated on a flexible polyester terephthalate substrate.

14.
Nanotechnology ; 29(22): 225602, 2018 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-29513266

RESUMO

This study investigates the morphological change in colloidal ZnO nanoparticles (NPs) synthesized with trioctylphosphine (TOP). The addition of TOP to the synthesis causes an evolution in the shape of ZnO NPs to tadpole-like particles from quasi-spherical particles at 300 °C. The total length of the tadpole-like ZnO NPs can be modified by controlling the molar ratio of TOP to oleylamine (OLAM). The tadpole-like particles are elongated as the concentration of TOP increased but decreased when the addition of TOP is excessive. These tadpole-like ZnO NPs transform to quasi-spherical NPs regardless of the amount of TOP at a reaction time of 3 h at 300 °C. At 200 °C, the effect of TOP on the ZnO NP synthesis differs from that at 300 °C. The ZnO NPs synthesized by controlling the molar ratios of surfactant ligands (TOP:OLAM = 2:100 and 70:100) at 200 °C share similar amorphous structures, while a crystalline ZnO phase is formed when the reaction time is 3 h. X-ray photoelectron spectroscopy analysis shows that TOP influences the oxidation of ZnO and suggests that a combination of OLAM and TOP plays a role in controlling the shape of ZnO NPs. These results provide critical insights to the utilization of TOP for a shape controlling ligand in ZnO NPs and suggest a new route to design oxide NPs.

15.
ACS Appl Mater Interfaces ; 10(1): 1389-1398, 2018 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-29239175

RESUMO

With the increase in interest in wearable tactile pressure sensors for e-skin, researches to make nanostructures to achieve high sensitivity have been actively conducted. However, limitations such as complex fabrication processes using expensive equipment still exist. Herein, simple lithography-free techniques to develop pyramid-like metal/insulator hybrid nanostructures utilizing nanocrystals (NCs) are demonstrated. Ligand-exchanged and unexchanged silver NC thin films are used as metallic and insulating components, respectively. The interfaces of each NC layer are chemically engineered to create discontinuous insulating layers, i.e., spacers for improved sensitivity, and eventually to realize fully solution-processed pressure sensors. Device performance analysis with structural, chemical, and electronic characterization and conductive atomic force microscopy study reveals that hybrid nanostructure based pressure sensor shows an enhanced sensitivity of higher than 500 kPa-1, reliability, and low power consumption with a wide range of pressure sensing. Nano-/micro-hierarchical structures are also designed by combining hybrid nanostructures with conventional microstructures, exhibiting further enhanced sensing range and achieving a record sensitivity of 2.72 × 104 kPa-1. Finally, all-solution-processed pressure sensor arrays with high pixel density, capable of detecting delicate signals with high spatial selectivity much better than the human tactile threshold, are introduced.

16.
Small ; 13(47)2017 12.
Artigo em Inglês | MEDLINE | ID: mdl-29078023

RESUMO

All-solution processed, high-performance wearable strain sensors are demonstrated using heterostructure nanocrystal (NC) solids. By incorporating insulating artificial atoms of CdSe quantum dot NCs into metallic artificial atoms of Au NC thin film matrix, metal-insulator heterostructures are designed. This hybrid structure results in a shift close to the percolation threshold, modifying the charge transport mechanism and enhancing sensitivity in accordance with the site percolation theory. The number of electrical pathways is also manipulated by creating nanocracks to further increase its sensitivity, inspired from the bond percolation theory. The combination of the two strategies achieves gauge factor up to 5045, the highest sensitivity recorded among NC-based strain gauges. These strain sensors show high reliability, durability, frequency stability, and negligible hysteresis. The fundamental charge transport behavior of these NC solids is investigated and the combined site and bond percolation theory is developed to illuminate the origin of their enhanced sensitivity. Finally, all NC-based and solution-processed strain gauge sensor arrays are fabricated, which effectively measure the motion of each finger joint, the pulse of heart rate, and the movement of vocal cords of human. This work provides a pathway for designing low-cost and high-performance electronic skin or wearable devices.


Assuntos
Metais/química , Nanopartículas/química , Dispositivos Eletrônicos Vestíveis , Impedância Elétrica , Nanopartículas/ultraestrutura , Soluções , Espectroscopia de Infravermelho com Transformada de Fourier
17.
Small ; 13(24)2017 06.
Artigo em Inglês | MEDLINE | ID: mdl-28464442

RESUMO

All-nanocrystal (NC)-based and all-solution-processed wearable resistance temperature detectors (RTDs) are introduced. The charge transport mechanisms of Ag NC thin films are engineered through various ligand treatments to design high performance RTDs. Highly conductive Ag NC thin films exhibiting metallic transport behavior with high positive temperature coefficients of resistance (TCRs) are achieved through tetrabutylammonium bromide treatment. Ag NC thin films showing hopping transport with high negative TCRs are created through organic ligand treatment. All-solution-based, one-step photolithography techniques that integrate two distinct opposite-sign TCR Ag NC thin films into an ultrathin single device are developed to decouple the mechanical effects such as human motion. The unconventional materials design and strategy enables highly accurate, sensitive, wearable and motion-free RTDs, demonstrated by experiments on moving or curved objects such as human skin, and simulation results based on charge transport analysis. This strategy provides a low cost and simple method to design wearable multifunctional sensors with high sensitivity which could be utilized in various fields such as biointegrated sensors or electronic skin.

18.
Nano Lett ; 17(3): 1387-1394, 2017 03 08.
Artigo em Inglês | MEDLINE | ID: mdl-28146634

RESUMO

We demonstrate the fabrication of hierarchical materials by controlling the structure of highly ordered binary nanocrystal superlattices (BNSLs) on multiple length scales. Combinations of magnetic, plasmonic, semiconducting, and insulating colloidal nanocrystal (NC) building blocks are self-assembled into BNSL membranes via the liquid-interfacial assembly technique. Free-standing BNSL membranes are transferred onto topographically structured poly(dimethylsiloxane) molds via the Langmuir-Schaefer technique and then deposited in patterns onto substrates via transfer printing. BNSLs with different structural motifs are successfully patterned into various meso- and microstructures such as lines, circles, and even three-dimensional grids across large-area substrates. A combination of electron microscopy and grazing incidence small-angle X-ray scattering (GISAXS) measurements confirm the ordering of NC building blocks in meso- and micropatterned BNSLs. This technique demonstrates structural diversity in the design of hierarchical materials by assembling BNSLs from NC building blocks of different composition and size by patterning BNSLs into various size and shape superstructures of interest for a broad range of applications.

19.
ACS Appl Mater Interfaces ; 8(42): 28743-28749, 2016 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-27696850

RESUMO

The competition between exciton dissociation and charge transport in organic solar cells comprising poly(3-hexylthiophene) [P3HT] and phenyl-C61-butyric acid methyl ester [PCBM] is investigated by correlated scanning confocal photoluminescence and photocurrent microscopies. Contrary to the general expectation that higher photoluminescence quenching is indicative of higher photocurrent, microscale mapping of bulk-heterojunction solar-cell devices shows that photoluminescence quenching and photocurrent can be inversely proportional to one another. To understand this phenomenon, we construct a model system by selectively laminating a PCBM layer onto a P3HT film to form a PCBM/P3HT planar junction on half of the device and a P3HT single junction on the other half. Upon thermal annealing to allow for interdiffusion of PCBM into P3HT, an inverse relationship between photoluminescence quenching and photocurrent is observed at the boundary between the PCBM/P3HT junction and P3HT layer. Incorporation of PCBM in P3HT works to increase photoluminescence quenching, consistent with efficient charge separation, but conductive atomic force microscopy measurements reveal that PCBM acts to decrease P3HT hole mobility, limiting the efficiency of charge transport. This suggests that photoluminescence-quenching measurements should be used with caution in evaluating new organic materials for organic solar cells.

20.
Science ; 352(6282): 205-8, 2016 Apr 08.
Artigo em Inglês | MEDLINE | ID: mdl-27124455

RESUMO

Synthetic methods produce libraries of colloidal nanocrystals with tunable physical properties by tailoring the nanocrystal size, shape, and composition. Here, we exploit colloidal nanocrystal diversity and design the materials, interfaces, and processes to construct all-nanocrystal electronic devices using solution-based processes. Metallic silver and semiconducting cadmium selenide nanocrystals are deposited to form high-conductivity and high-mobility thin-film electrodes and channel layers of field-effect transistors. Insulating aluminum oxide nanocrystals are assembled layer by layer with polyelectrolytes to form high-dielectric constant gate insulator layers for low-voltage device operation. Metallic indium nanocrystals are codispersed with silver nanocrystals to integrate an indium supply in the deposited electrodes that serves to passivate and dope the cadmium selenide nanocrystal channel layer. We fabricate all-nanocrystal field-effect transistors on flexible plastics with electron mobilities of 21.7 square centimeters per volt-second.

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