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1.
Nanoscale ; 12(3): 2047-2056, 2020 Jan 23.
Artigo em Inglês | MEDLINE | ID: mdl-31912844

RESUMO

Defect engineering is important for tailoring the electronic and optical properties of two-dimensional materials, and the capability of generating defects of certain types at specific locations is meaningful for potential applications such as optoelectronics and quantum photonics. In this work, atomic defects are created in single-layer WSe2 using focused ion beam (FIB) irradiation, with defect densities spanning many orders of magnitude. The influences of defects are systematically characterized. Raman spectroscopy can only discern defects in WSe2 for a FIB dose higher than 1 × 1013 cm-2, which causes blue shifts of both A'1 and E' modes. Photoluminescence (PL) of WSe2 is more sensitive to defects. At cryogenic temperature, the low-energy PL induced by defects can be revealed, which shows redshifts and broadenings with increased FIB doses. Similar Raman shifts and PL spectrum changes are observed for the WSe2 film grown by chemical vapor deposition (CVD). A four microsecond-long lifetime is observed in the PL dynamics and is three orders of magnitude longer than the often observed delocalized exciton lifetime and becomes more dominant for WSe2 with increasing FIB doses. The ultra-long lifetime of PL in single-layer WSe2 is consistent with first-principles calculation results considering the creation of both chalcogen and metal vacancies by FIB, and can be valuable for photo-catalytic reactions, valleytronics and quantum light emissions owing to the longer carrier separation/manipulation time.

2.
Adv Mater ; 31(49): e1904132, 2019 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31621963

RESUMO

Spin-dependent contrasting phenomena at K and K' valleys in monolayer semiconductors have led to addressable valley degree of freedom, which is the cornerstone for emerging valleytronic applications in information storage and processing. Tunable and active modulation of valley dynamics in a monolayer WSe2 is demonstrated at room temperature through controllable chiral Purcell effects in plasmonic chiral metamaterials. The strong spin-dependent modulation on the spontaneous decay of valley excitons leads to tunable handedness and spectral shift of valley-polarized emission, which is analyzed and predicted by an advanced theoretical model and further confirmed by experimental measurements. Moreover, large active spectral tuning (≈24 nm) and reversible ON/OFF switching of circular polarization of emission are achieved by the solvent-controllable thickness of the dielectric spacer in the metamaterials. With the on-demand and active tunability in valley-polarized emission, chiral Purcell effects can provide new strategies to harness valley excitons for applications in ultrathin valleytronic devices.

3.
ACS Nano ; 13(3): 3341-3352, 2019 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-30758945

RESUMO

A defect-controlled approach for the nucleation and epitaxial growth of WSe2 on hBN is demonstrated. The WSe2 domains exhibit a preferred orientation of over 95%, leading to a reduced density of inversion domain boundaries (IDBs) upon coalescence. First-principles calculations and experimental studies as a function of growth conditions and substrate pretreatment confirm that WSe2 nucleation density and orientation are controlled by the hBN surface defect density rather than thermodynamic factors. Detailed transmission electron microscopy analysis provides support for the role of single-atom vacancies on the hBN surface that trap W atoms and break surface symmetry leading to a reduced formation energy for one orientation of WSe2 domains. Through careful control of nucleation and extended lateral growth time, fully coalesced WSe2 monolayer films on hBN were achieved. Low-temperature photoluminescence (PL) measurements and transport measurements of back-gated field-effect transistor devices fabricated on WSe2/hBN films show improved optical and electrical properties compared to films grown on sapphire under similar conditions. Our results reveal an important nucleation mechanism for the epitaxial growth of van der Waals heterostructures and demonstrate hBN as a superior substrate for single-crystal transition-metal dichalcogenide (TMD) films, resulting in a reduced density of IDBs and improved properties. The results motivate further efforts focused on the development of single crystal hBN substrates and epilayers for synthesis of wafer-scale single crystal TMD films.

4.
ACS Appl Mater Interfaces ; 10(47): 40831-40837, 2018 Nov 28.
Artigo em Inglês | MEDLINE | ID: mdl-30384598

RESUMO

The utilization of alkali salts, such as NaCl and KI, has enabled the successful growth of large single domain and fully coalesced polycrystalline two-dimensional (2D) transition-metal dichalcogenide layers. However, the impact of alkali salts on photonic and electronic properties is not fully established. In this work, we report alkali-free epitaxy of MoS2 on sapphire and benchmark the properties against alkali-assisted growth of MoS2. This study demonstrates that although NaCl can dramatically increase the domain size of monolayer MoS2 by 20 times, it can also induce strong optical and electronic heterogeneities in as-grown, large-scale films. This work elucidates that utilization of NaCl can lead to variation in growth rates, loss of epitaxy, and high density of nanoscale MoS2 particles (4 ± 0.7/µm2). Such phenomena suggest that alkali atoms play an important role in Mo and S adatom mobility and strongly influence the 2D/sapphire interface during growth. Compared to alkali-free synthesis under the same growth conditions, MoS2 growth assisted by NaCl results in >1% tensile strain in as-grown domains, which reduces photoluminescence by ∼20× and degrades transistor performance.

5.
Nano Lett ; 18(2): 1049-1056, 2018 02 14.
Artigo em Inglês | MEDLINE | ID: mdl-29342357

RESUMO

A multistep diffusion-mediated process was developed to control the nucleation density, size, and lateral growth rate of WSe2 domains on c-plane sapphire for the epitaxial growth of large area monolayer films by gas source chemical vapor deposition (CVD). The process consists of an initial nucleation step followed by an annealing period in H2Se to promote surface diffusion of tungsten-containing species to form oriented WSe2 islands with uniform size and controlled density. The growth conditions were then adjusted to suppress further nucleation and laterally grow the WSe2 islands to form a fully coalesced monolayer film in less than 1 h. Postgrowth structural characterization demonstrates that the WSe2 monolayers are single crystal and epitaxially oriented with respect to the sapphire and contain antiphase grain boundaries due to coalescence of 0° and 60° oriented WSe2 domains. The process also provides fundamental insights into the two-dimensional (2D) growth mechanism. For example, the evolution of domain size and cluster density with annealing time follows a 2D ripening process, enabling an estimate of the tungsten-species surface diffusivity. The lateral growth rate of domains was found to be relatively independent of substrate temperature over the range of 700-900 °C suggesting a mass transport limited process, however, the domain shape (triangular versus truncated triangular) varied with temperature over this same range due to local variations in the Se/W adatom ratio. The results provide an important step toward atomic level control of the epitaxial growth of WSe2 monolayers in a scalable process that is suitable for large area device fabrication.

6.
ACS Nano ; 12(2): 965-975, 2018 02 27.
Artigo em Inglês | MEDLINE | ID: mdl-29360349

RESUMO

Atomically thin transition metal dichalcogenides (TMDs) are of interest for next-generation electronics and optoelectronics. Here, we demonstrate device-ready synthetic tungsten diselenide (WSe2) via metal-organic chemical vapor deposition and provide key insights into the phenomena that control the properties of large-area, epitaxial TMDs. When epitaxy is achieved, the sapphire surface reconstructs, leading to strong 2D/3D (i.e., TMD/substrate) interactions that impact carrier transport. Furthermore, we demonstrate that substrate step edges are a major source of carrier doping and scattering. Even with 2D/3D coupling, transistors utilizing transfer-free epitaxial WSe2/sapphire exhibit ambipolar behavior with excellent on/off ratios (∼107), high current density (1-10 µA·µm-1), and good field-effect transistor mobility (∼30 cm2·V-1·s-1) at room temperature. This work establishes that realization of electronic-grade epitaxial TMDs must consider the impact of the TMD precursors, substrate, and the 2D/3D interface as leading factors in electronic performance.

7.
Nanotechnology ; 29(5): 055706, 2018 Feb 02.
Artigo em Inglês | MEDLINE | ID: mdl-29239306

RESUMO

There is significant interest in the growth of single crystal monolayer and few-layer films of transition metal dichalcogenides (TMD) and other 2D materials for scientific exploration and potential applications in optics, electronics, sensing, catalysis and others. The characterization of these materials is crucial in determining the properties and hence the applications. The ultra-thin nature of 2D layers presents a challenge to the use of x-ray diffraction (XRD) analysis with conventional Bragg-Brentano geometry in analyzing the crystallinity and epitaxial orientation of 2D films. To circumvent this problem, we demonstrate the use of in-plane XRD employing lab scale equipment which uses a standard Cu x-ray tube for the analysis of the crystallinity of TMD monolayer and few-layer films. The applicability of this technique is demonstrated in several examples for WSe2 and WS2 films grown by chemical vapor deposition on single crystal substrates. In-plane XRD was used to determine the epitaxial relation of WSe2 grown on c-plane sapphire and on SiC with an epitaxial graphene interlayer. The evolution of the crystal structure orientation of WS2 films on sapphire as a function of growth temperature was also examined. Finally, the epitaxial relation of a WS2/WSe2 vertical heterostructure deposited on sapphire substrate was determined. We observed that WSe2 grows epitaxially on both substrates employed in this work under all conditions studied while WS2 exhibits various preferred orientations on sapphire substrate which are temperature dependent. In contrast to the sapphire substrate, WS2 deposited on WSe2 exhibits only one preferred orientation which may provide a route to better control the orientation and crystal quality of WS2. In the case of epitaxial graphene on SiC, no graphene-related peaks were observed in in-plane XRD while its presence was confirmed using Raman spectroscopy. This demonstrates the limitation of the in-plane XRD technique for characterizing low electron density materials.

8.
Nat Mater ; 15(11): 1166-1171, 2016 11.
Artigo em Inglês | MEDLINE | ID: mdl-27571451

RESUMO

The spectrum of two-dimensional (2D) and layered materials 'beyond graphene' offers a remarkable platform to study new phenomena in condensed matter physics. Among these materials, layered hexagonal boron nitride (hBN), with its wide bandgap energy (∼5.0-6.0 eV), has clearly established that 2D nitrides are key to advancing 2D devices. A gap, however, remains between the theoretical prediction of 2D nitrides 'beyond hBN' and experimental realization of such structures. Here we demonstrate the synthesis of 2D gallium nitride (GaN) via a migration-enhanced encapsulated growth (MEEG) technique utilizing epitaxial graphene. We theoretically predict and experimentally validate that the atomic structure of 2D GaN grown via MEEG is notably different from reported theory. Moreover, we establish that graphene plays a critical role in stabilizing the direct-bandgap (nearly 5.0 eV), 2D buckled structure. Our results provide a foundation for discovery and stabilization of 2D nitrides that are difficult to prepare via traditional synthesis.

9.
Nano Lett ; 16(9): 5742-50, 2016 09 14.
Artigo em Inglês | MEDLINE | ID: mdl-27540753

RESUMO

Unprecedented interest has been spurred recently in two-dimensional (2D) layered transition metal dichalcogenides (TMDs) that possess tunable electronic and optical properties. However, synthesis of a wafer-scale TMD thin film with controlled layers and homogeneity remains highly challenging due mainly to the lack of thermodynamic and diffusion knowledge, which can be used to understand and design process conditions, but falls far behind the rapidly growing TMD field. Here, an integrated density functional theory (DFT) and calculation of phase diagram (CALPHAD) modeling approach is employed to provide thermodynamic insight into lateral versus vertical growth of the prototypical 2D material MoS2. Various DFT energies are predicted from the layer-dependent MoS2, 2D flake-size related mono- and bilayer MoS2, to Mo and S migrations with and without graphene and sapphire substrates, thus shedding light on the factors that control lateral versus vertical growth of 2D islands. For example, the monolayer MoS2 flake in a small 2D lateral size is thermodynamically favorable with respect to the bilayer counterpart, indicating the monolayer preference during the initial stage of nucleation; while the bilayer MoS2 flake becomes stable with increasing 2D lateral size. The critical 2D flake-size of phase stability between mono- and bilayer MoS2 is adjustable via the choice of substrate. In terms of DFT energies and CALPHAD modeling, the size dependent pressure-temperature-composition (P-T-x) growth windows are predicted for MoS2, indicating that the formation of MoS2 flake with reduced size appears in the middle but close to the lower T and higher P "Gas + MoS2" phase region. It further suggests that Mo diffusion is a controlling factor for MoS2 growth owing to its extremely low diffusivity compared to that of sulfur. Calculated MoS2 energies, Mo and S diffusivities, and size-dependent P-T-x growth windows are in good accord with available experiments, and the present data provide quantitative insight into the controlled growth of 2D layered MoS2.

10.
Nanotechnology ; 27(13): 135605, 2016 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-26900836

RESUMO

Aluminum-catalyzed silicon nanowire growth under low-pressure chemical vapor deposition conditions requires higher reactor pressures than gold-catalyzed growth, but the reasons for this difference are not well understood. In this study, the effects of reactor pressure and hydrogen partial pressure on silicon nanowire growth using an aluminum catalyst were studied by growing nanowires in hydrogen and hydrogen/nitrogen carrier gas mixtures at different total reactor pressures. Nanowires grown in the nitrogen/hydrogen mixture have faceted catalyst droplet tips, minimal evidence of aluminum diffusion from the tip down the nanowire sidewalls, and significant vapor-solid deposition of silicon on the sidewalls. In comparison, wires grown in pure hydrogen show less well-defined tips, evidence of aluminum diffusion down the nanowire sidewalls at increasing reactor pressures and reduced vapor-solid deposition of silicon on the sidewalls. The results are explained in terms of a model wherein the hydrogen partial pressure plays a critical role in aluminum-catalyzed nanowire growth by controlling hydrogen termination of the silicon nanowire sidewalls. For a given reactor pressure, increased hydrogen partial pressures increase the extent of hydrogen termination of the sidewalls which suppresses SiH4 adsorption thereby reducing vapor-solid deposition of silicon but increases the surface diffusion length of aluminum. Conversely, lower hydrogen partial pressures reduce the hydrogen termination and also increase the extent of SiH4 gas phase decomposition, shifting the nanowire growth window to lower growth temperatures and silane partial pressures.

11.
Nanoscale ; 7(16): 7267-74, 2015 Apr 28.
Artigo em Inglês | MEDLINE | ID: mdl-25811140

RESUMO

Single wire p(+)-n(+) radial junction nanowire solar cell devices were fabricated by low pressure chemical vapor deposition of n(+) silicon shell layers on p(+) silicon nanowires synthesized by vapor-liquid-solid growth. The n(+)-shell layers were deposited at two growth temperatures (650 °C and 950 °C) to study the impact of shell crystallinity on the device properties. The n-type Si shell layers deposited at 650 °C were polycrystalline and resulted in diodes that were not rectifying. A pre-coating anneal at 950 °C in H2 improved the structural quality of the shell layers and yielded diodes with a dark saturation current density of 3 × 10(-5) A cm(-2). Deposition of the n-type Si shell layer at 950 °C resulted in epitaxial growth on the nanowire core, which lowered the dark saturation current density to 3 × 10(-7) A cm(-2) and increased the solar energy conversion efficiency. Temperature-dependent current-voltage measurements demonstrated that the 950 °C coated devices were abrupt junction p(+)-n(+) diodes with band-to-band tunneling at high reverse-bias voltage, while multi-step tunneling degraded the performance of devices fabricated with a 950 °C anneal and 650 °C coating. The higher trap density of the 950 °C annealed 650 °C coated devices is believed to arise from the polycrystalline nature of the shell layer coating, which results in an increased density of dangling bonds at the p(+)-n(+) junction interface.

12.
ACS Nano ; 9(2): 2080-7, 2015 Feb 24.
Artigo em Inglês | MEDLINE | ID: mdl-25625184

RESUMO

Tungsten diselenide (WSe2) is a two-dimensional material that is of interest for next-generation electronic and optoelectronic devices due to its direct bandgap of 1.65 eV in the monolayer form and excellent transport properties. However, technologies based on this 2D material cannot be realized without a scalable synthesis process. Here, we demonstrate the first scalable synthesis of large-area, mono and few-layer WSe2 via metal-organic chemical vapor deposition using tungsten hexacarbonyl (W(CO)6) and dimethylselenium ((CH3)2Se). In addition to being intrinsically scalable, this technique allows for the precise control of the vapor-phase chemistry, which is unobtainable using more traditional oxide vaporization routes. We show that temperature, pressure, Se:W ratio, and substrate choice have a strong impact on the ensuing atomic layer structure, with optimized conditions yielding >8 µm size domains. Raman spectroscopy, atomic force microscopy (AFM), and cross-sectional transmission electron microscopy (TEM) confirm crystalline monoto-multilayer WSe2 is achievable. Finally, TEM and vertical current/voltage transport provide evidence that a pristine van der Waals gap exists in WSe2/graphene heterostructures.

13.
J Phys Chem Lett ; 5(12): 2050-7, 2014 Jun 19.
Artigo em Inglês | MEDLINE | ID: mdl-26270492

RESUMO

We simultaneously determined the charge carrier mobility and picosecond to nanosecond carrier dynamics of isolated silicon nanowires (Si NWs) and nanocrystals (Si NCs) using time-resolved terahertz spectroscopy. We then compared these results to data measured on bulk c-Si as a function of excitation fluence. We find >1 ns carrier lifetimes in Si NWs that are dominated by surface recombination with surface recombination velocities (SRV) between ∼1100-1700 cm s(-1) depending on process conditions. The Si NCs have markedly different decay dynamics. Initially, free-carriers are produced, but relax within ∼1.5 ps to form bound excitons. Subsequently, the excitons decay with lifetimes >7 ns, similar to free carriers produced in bulk Si. The isolated Si NWs exhibit bulk-like mobilities that decrease with increasing excitation density, while the hot-carrier mobilities in the Si NCs are lower than bulk mobilities and could only be measured within the initial 1.5 ps decay. We discuss the implications of our measurements on the utilization of Si NWs and NCs in macroscopic optoelectronic applications.

14.
Nanotechnology ; 23(21): 215205, 2012 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-22552162

RESUMO

Local electrode atom probe (LEAP) tomography of Al-catalyzed silicon nanowires synthesized by the vapor­liquid­solid method is presented. The concentration of Al within the Al-catalyzed nanowire was found to be 2 × 10(20) cm(-3), which is higher than the expected solubility limit for Al in Si at the nanowire growth temperature of 550°C. Reconstructions of the Al contained within the nanowire indicate a denuded region adjacent to the Al catalyst/Si nanowire interface, while Al clusters are distributed throughout the rest of the silicon nanowire.


Assuntos
Alumínio/química , Eletrodos , Teste de Materiais/métodos , Nanoestruturas/química , Nanoestruturas/ultraestrutura , Silício/química , Catálise , Tamanho da Partícula
16.
Nano Lett ; 10(12): 4813-8, 2010 Dec 08.
Artigo em Inglês | MEDLINE | ID: mdl-21073180

RESUMO

Tunnel field-effect transistors were fabricated from axially doped silicon nanowire p-n junctions grown via the vapor-liquid-solid method. Following dry thermal oxidation to form a gate dielectric shell, the nanowires have a p-n-n(+) doping profile with an abrupt n-n(+) junction, which was revealed by scanning capacitance microscopy. The lightly doped n-segment can be inverted to p(+) by modulating the top gate bias, thus forming an abrupt gated p(+)-n(+) junction. A band-to-band tunneling current flows through the electrostatically doped p(+)-n(+) junction when it is reverse biased. Current-voltage measurements performed from 375 down to 4.2 K show two different regimes of tunneling current at high and low temperatures, indicating that there are both direct band-to-band and trap-assisted tunneling paths.

17.
Nano Lett ; 9(12): 4494-9, 2009 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-19904918

RESUMO

The synthesis of epitaxially oriented Si nanowires at high growth rates (>1 microm/min) was demonstrated on (111) Si substrates using Al as the catalyst. The use of high H(2) and SiH(4) partial pressures was found to be effective at reducing problems associated with Al oxidation and nanowire nucleation, enabling growth of high aspect ratio structures at temperatures ranging from 500 to 600 degrees C with minimal tapering of the diameter. Because of the high growth rate observed, the Al catalyst is believed to be in the liquid state during the growth. Four-point resistance measurements and back-gated current-voltage measurements indicate that the wires are p-type with an average resistivity of 0.01 +/- 0.004 Omega-cm. These results suggest that Al is incorporated into the Si nanowires under these conditions at concentrations higher than the solubility limit (5-6 x 10(18) cm(-3)) for Al in Si at 550 degrees C. This work demonstrates that Al can serve as both an effective catalyst and p-type dopant for the growth of Si nanowires.


Assuntos
Alumínio/química , Cristalização/métodos , Nanoestruturas/química , Nanoestruturas/ultraestrutura , Nanotecnologia/métodos , Silício/química , Catálise , Impedância Elétrica , Gases/química , Substâncias Macromoleculares/química , Teste de Materiais , Conformação Molecular , Tamanho da Partícula , Soluções , Propriedades de Superfície
18.
Nanotechnology ; 20(2): 025607, 2009 Jan 14.
Artigo em Inglês | MEDLINE | ID: mdl-19417276

RESUMO

The effect of Sb addition on the growth rate and structural properties of Si nanowires synthesized by vapor-liquid-solid growth was investigated. The nanowire growth rate was reduced by an order of magnitude following the addition of a low concentration pulse of trimethylantimony (TMSb) to the gas phase during growth. Transmission electron microscopy analysis revealed that the wires had a thick amorphous coating ( approximately 8 nm) around the catalyst particle and a distorted catalyst shape. Energy-dispersive x-ray spectroscopy showed the presence of trace amounts of Sb in the amorphous coating around the catalyst and at the catalyst-wire interface. Antimony was also found to be incorporated in the Si nanowires with a peak in the Sb concentration measured at the initial point where the TMSb pulse was added to the gas stream. The significant reduction in wire growth rate was attributed to Sb segregation at the vapor-liquid and liquid-solid interfaces which results in a change in interfacial energies and a reduction in the rate of Si incorporation at these interfaces.

19.
Nanotechnology ; 20(8): 085610, 2009 Feb 25.
Artigo em Inglês | MEDLINE | ID: mdl-19417458

RESUMO

The structure and chemistry of the catalyst particles that terminate GaN nanowires grown by Ni-assisted metal-organic chemical vapor deposition were investigated using a combination of electron diffraction, high-resolution transmission electron microscopy, and x-ray energy dispersive spectrometry. The crystal symmetry, lattice parameter, and chemical composition obtained reveal that the catalyst particles are Ni(3)Ga with an ordered L 1(2) structure. The results suggest that the catalyst is a solid particle during growth and therefore favor a vapor-solid-solid mechanism for the growth of GaN nanowires under these conditions.


Assuntos
Cristalização/métodos , Gálio/química , Nanoestruturas/química , Nanoestruturas/ultraestrutura , Nanotecnologia/métodos , Níquel/química , Compostos Orgânicos/química , Catálise , Gases/química , Substâncias Macromoleculares/química , Teste de Materiais , Conformação Molecular , Tamanho da Partícula , Propriedades de Superfície
20.
Nat Nanotechnol ; 3(2): 88-92, 2008 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-18654467

RESUMO

Directed-assembly of nanowire-based devices will enable the development of integrated circuits with new functions that extend well beyond mainstream digital logic. For example, nanoelectromechanical resonators are very attractive for chip-based sensor arrays because of their potential for ultrasensitive mass detection. In this letter, we introduce a new bottom-up assembly method to fabricate large-area nanoelectromechanical arrays each having over 2,000 single-nanowire resonators. The nanowires are synthesized and chemically functionalized before they are integrated onto a silicon chip at predetermined locations. Peptide nucleic acid probe molecules attached to the nanowires before assembly maintain their binding selectivity and recognize complementary oligonucleotide targets once the resonator array is assembled. The two types of cantilevered resonators we integrated here using silicon and rhodium nanowires had Q-factors of approximately 4,500 and approximately 1,150, respectively, in vacuum. Taken together, these results show that bottom-up nanowire assembly can offer a practical alternative to top-down fabrication for sensitive chip-based detection.


Assuntos
Cristalização/métodos , Nanotecnologia/instrumentação , Nanotubos/química , Nanotubos/ultraestrutura , Ródio/química , Silício/química , Transdutores , Desenho de Equipamento , Análise de Falha de Equipamento , Substâncias Macromoleculares/química , Teste de Materiais , Conformação Molecular , Nanotecnologia/métodos , Tamanho da Partícula , Propriedades de Superfície , Vibração
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