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1.
Proc Natl Acad Sci U S A ; 120(43): e2308741120, 2023 Oct 24.
Artigo em Inglês | MEDLINE | ID: mdl-37862383

RESUMO

Macromolecules bearing open-shell entities offer unique transport properties for both electronic and spintronic devices. This work demonstrates that, unlike their conjugated polymer counterparts, the charge carriers in radical polymers (i.e., macromolecules with nonconjugated backbones and with stable open-shell sites present at their pendant groups) are singlet cations, which opens significant avenues for manipulating macromolecular design for advanced solid-state transport in these highly transparent conductors. Despite this key point, magnetoresistive effects are present in radical polymer thin films under applied magnetic fields due to the presence of impurity sites in low (i.e., <1%) concentrations. Additionally, thermal annealing of poly(4-glycidyloxy-2,2,6,6- tetramethylpiperidine-1-oxyl) (PTEO), a nonconjugated polymer with stable open-shell pendant groups, facilitated better electron exchange and pairwise spin interactions resulting in an unexpected magnetoresistance signal at relatively low field strengths (i.e., <2 T). The addition of 4-hydroxy-2,2,6,6-tetramethylpiperidin-N-oxy (TEMPO-OH), a paramagnetic species, increased the magnitude of the MR effect when the small molecule was added to the radical polymer matrix. These macroscopic experimental observables are explained using computational approaches that detail the fundamental molecular principles. This intrinsic localized charge transport behavior differs from the current state of the art regarding closed-shell conjugated macromolecules, and it opens an avenue towards next-generation transport in organic electronic materials.

2.
Proc Natl Acad Sci U S A ; 120(8): e2216367120, 2023 Feb 21.
Artigo em Inglês | MEDLINE | ID: mdl-36791111

RESUMO

Recently, evidence for a conducting surface state (CSS) below 19 K was reported for the correlated d-electron small gap semiconductor FeSi. In the work reported herein, the CSS and the bulk phase of FeSi were probed via electrical resistivity ρ measurements as a function of temperature T, magnetic field B to 60 T, and pressure P to 7.6 GPa, and by means of a magnetic field-modulated microwave spectroscopy (MFMMS) technique. The properties of FeSi were also compared with those of the Kondo insulator SmB6 to address the question of whether FeSi is a d-electron analogue of an f-electron Kondo insulator and, in addition, a "topological Kondo insulator" (TKI). The overall behavior of the magnetoresistance of FeSi at temperatures above and below the onset temperature TS = 19 K of the CSS is similar to that of SmB6. The two energy gaps, inferred from the ρ(T) data in the semiconducting regime, increase with pressure up to about 7 GPa, followed by a drop which coincides with a sharp suppression of TS. Several studies of ρ(T) under pressure on SmB6 reveal behavior similar to that of FeSi in which the two energy gaps vanish at a critical pressure near the pressure at which TS vanishes, although the energy gaps in SmB6 initially decrease with pressure, whereas in FeSi they increase with pressure. The MFMMS measurements showed a sharp feature at TS ≈ 19 K for FeSi, which could be due to ferromagnetic ordering of the CSS. However, no such feature was observed at TS ≈ 4.5 K for SmB6.

3.
Proc Natl Acad Sci U S A ; 119(45): e2208505119, 2022 Nov 08.
Artigo em Inglês | MEDLINE | ID: mdl-36322772

RESUMO

The linear positive magnetoresistance (LPMR) is a widely observed phenomenon in topological materials, which is promising for potential applications on topological spintronics. However, its mechanism remains ambiguous yet, and the effect is thus uncontrollable. Here, we report a quantitative scaling model that correlates the LPMR with the Berry curvature, based on a ferromagnetic Weyl semimetal CoS2 that bears the largest LPMR of over 500% at 2 K and 9 T, among known magnetic topological semimetals. In this system, masses of Weyl nodes existing near the Fermi level, revealed by theoretical calculations, serve as Berry-curvature monopoles and low-effective-mass carriers. Based on the Weyl picture, we propose a relation [Formula: see text], with B being the applied magnetic field and [Formula: see text] the average Berry curvature near the Fermi surface, and further introduce temperature factor to both MR/B slope (MR per unit field) and anomalous Hall conductivity, which establishes the connection between the model and experimental measurements. A clear picture of the linearly slowing down of carriers, i.e., the LPMR effect, is demonstrated under the cooperation of the k-space Berry curvature and real-space magnetic field. Our study not only provides experimental evidence of Berry curvature-induced LPMR but also promotes the common understanding and functional designing of the large Berry-curvature MR in topological Dirac/Weyl systems for magnetic sensing or information storage.

4.
Nano Lett ; 24(2): 632-639, 2024 Jan 17.
Artigo em Inglês | MEDLINE | ID: mdl-38175932

RESUMO

Electrical control of magnetism is highly desirable for energy-efficient spintronic applications. Realizing electric-field-driven perpendicular magnetization switching has been a long-standing goal, which, however, remains a major challenge. Here, electric-field control of perpendicularly magnetized ferrimagnetic order via strain-mediated magnetoelectric coupling is reported. We show that the gate voltages isothermally toggle the dominant magnetic sublattice of the compensated ferrimagnet FeTb at room temperature, showing high reversibility and good endurance under ambient conditions. By implementing this strategy in FeTb/Pt/Co spin valves with giant magnetoresistance (GMR), we demonstrate that the distinct high and low resistance states can be selectively controlled by the gate voltages with assisting magnetic fields. Our results provide a promising route to use ferrimagnets for developing electric-field-controlled, low-power memory and logic devices.

5.
Nano Lett ; 24(5): 1471-1476, 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-38216142

RESUMO

We study current-induced switching of the Néel vector in CoO/Pt bilayers to understand the underlying antiferromagnetic switching mechanism. Surprisingly, we find that for ultrathin CoO/Pt bilayers electrical pulses along the same path can lead to an increase or decrease of the spin Hall magnetoresistance signal, depending on the current density of the pulse. By comparing these results to XMLD-PEEM imaging of the antiferromagnetic domain structure before and after the application of current pulses, we reveal the details of the reorientation of the Néel vector in ultrathin CoO(4 nm). This allows us to understand how opposite resistance changes can result from a thermomagnetoelastic switching mechanism. Importantly, our spatially resolved imaging shows that regions where the current pulses are applied and regions further away exhibit different switched spin structures, which can be explained by a spin-orbit torque-based switching mechanism that can dominate in very thin films.

6.
Nano Lett ; 24(8): 2496-2502, 2024 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-38350134

RESUMO

A major challenge for magnetic skyrmions in atomically thin van der Waals (vdW) materials is reliable skyrmion detection. Here, based on rigorous first-principles calculations, we show that all-electrical skyrmion detection is feasible in two-dimensional vdW magnets via scanning tunneling microscopy (STM) and in planar tunnel junctions. We use the nonequilibrium Green's function method for quantum transport in planar junctions, including self-energy due to electrodes and working conditions, going beyond the standard Tersoff-Hamann approximation. We obtain a very large tunneling anisotropic magnetoresistance (TAMR) around the Fermi energy for a graphite/Fe3GeTe2/germanene/graphite vdW tunnel junction. For atomic-scale skyrmions, the noncollinear magnetoresistance (NCMR) reaches giant values. We trace the origin of the NCMR to spin mixing between spin-up and -down states of pz and dz2 character at the surface atoms. Both TAMR and NCMR are drastically enhanced in tunnel junctions with respect to STM geometry due to orbital symmetry matching at the interface.

7.
Nano Lett ; 24(14): 4158-4164, 2024 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-38557108

RESUMO

As a quasi-layered ferrimagnetic material, Mn3Si2Te6 nanoflakes exhibit magnetoresistance behavior that is fundamentally different from their bulk crystal counterparts. They offer three key properties crucial for spintronics. First, at least 106 times faster response compared to that exhibited by bulk crystals has been observed in current-controlled resistance and magnetoresistance. Second, ultralow current density is required for resistance modulation (∼5 A/cm2). Third, electrically gate-tunable magnetoresistance has been realized. Theoretical calculations reveal that the unique magnetoresistance behavior in the Mn3Si2Te6 nanoflakes arises from a magnetic field induced band gap shift across the Fermi level. The rapid current induced resistance variation is attributed to spin-orbit torque, an intrinsically ultrafast process (∼nanoseconds). This study suggests promising avenues for spintronic applications. In addition, it highlights Mn3Si2Te6 nanoflakes as a suitable platform for investigating the intriguing physics underlying chiral orbital moments, magnetic field induced band variation, and spin torque.

8.
Nano Lett ; 24(2): 584-591, 2024 Jan 17.
Artigo em Inglês | MEDLINE | ID: mdl-38165127

RESUMO

Cu2S likely plays an important role in the sharp resistivity transition of LK-99. Nevertheless, this immediately arouses an intriguing question of whether the extraordinary room-temperature colossal magnetoresistance in the initial reports, which has been less focused, originates from Cu2S as well. To resolve this issue, we have systematically investigated the electrical transport and magnetotransport properties of near-stoichiometric Cu2S pellets and thin films. Neither Cu2S nor LK-99 containing Cu2S in this study was found to exhibit the remarkable magnetoresistance effect implied by Lee et al. This implies that Cu2S could not account for all of the intriguing transport properties of the initially reported LK-99, and the initially reported LK-99 samples might contain magnetic impurities. Moreover, based on the crystal-structure-sensitive electrical properties of Cu2S, we have constructed a piezoelectric-strain-controlled device and obtained a giant and reversible resistance modulation of 2 orders of magnitude at room temperature, yielding a huge gauge factor of 160,000.

9.
Nano Lett ; 24(15): 4471-4477, 2024 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-38587318

RESUMO

van der Waals magnets are emerging as a promising material platform for electric field control of magnetism, offering a pathway toward the elimination of external magnetic fields from spintronic devices. A further step is the integration of such magnets with electrical gating components that would enable nonvolatile control of magnetic states. However, this approach remains unexplored for antiferromagnets, despite their growing significance in spintronics. Here, we demonstrate nonvolatile electric field control of magnetoelectric characteristics in van der Waals antiferromagnet CrSBr. We integrate a CrSBr channel in a flash-memory architecture featuring charge trapping graphene multilayers. The electrical gate operation triggers a nonvolatile 200% change in the antiferromagnetic state of CrSBr resistance by manipulating electron accumulation/depletion. Moreover, the nonvolatile gate modulates the metamagnetic transition field of CrSBr and the magnitude of magnetoresistance. Our findings highlight the potential of manipulating magnetic properties of antiferromagnetic semiconductors in a nonvolatile way.

10.
Nano Lett ; 24(30): 9221-9228, 2024 Jul 31.
Artigo em Inglês | MEDLINE | ID: mdl-39037057

RESUMO

We examine the coherent spin-dependent transport properties of the van der Waals (vdW) ferromagnet Fe4GeTe2 using density functional theory combined with the nonequilibrium Green's function method. Our findings reveal that the conductance perpendicular to the layers is half-metallic, meaning that it is almost entirely spin-polarized. This property persists from the bulk to a single layer, even under significant bias voltages and with spin-orbit coupling. Additionally, using dynamical mean field theory for quantum transport, we demonstrate that electron correlations are important for magnetic properties but minimally impact the conductance, preserving almost perfect spin-polarization. Motivated by these results, we then study the tunnel magnetoresistance (TMR) in a magnetic tunnel junction consisting of two Fe4GeTe2 layers with the vdW gap acting as an insulating barrier. We predict a TMR ratio of ∼500%, which can be further enhanced by increasing the number of Fe4GeTe2 layers in the junction.

11.
Small ; 20(27): e2308796, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38363026

RESUMO

A race to achieve a crossover from positive to negative magnetoresistance is intense in the field of nanostructured materials to reduce the size of memory devices. Here, the unusual complex magnetoresistance in nonmagnetic sulfur-doped Sb2Se3 nanowires is demonstrated. Intentionally, sulfur is doped in such a way to nearly achieve the charge neutrality point that is evident from switching of carrier type from p-type to n-type at 13 K as inferred from the low-temperature thermoelectric power measurements. A change from 3D variable range hopping (VRH) to power law transport with α = 0.18  in resistivity measurement signifies a Luttinger liquid transport with weak links through the nanowires. Interestingly, high magnetic field induced negative magnetoresistance (NMR) occurring in hole dominated temperature regimes can only be explained by invoking the concept of charge puddles. Spot energy dispersive spectroscopy (EDS), magnetic force microscopy (MFM) measurements, Tmott and Regel plot indicate an enhanced disorder in these sulfurized nanowires that are found to be the precursor for the formation of these charge puddles. Tunability of conducting states in these nanowires is investigated in the light of interplay of carrier type, magnetic field, temperature, and intricate intra-inter wire transport that makes this nanowires potential for large scale spintronic devices.

12.
Chemistry ; 30(28): e202400166, 2024 May 17.
Artigo em Inglês | MEDLINE | ID: mdl-38530333

RESUMO

Spin-polarized donor radicals based on tetrathiafulvalene (TTF) derivatives and nitronyl nitroxide (NN) radicals in which one-electron oxidation involves the HOMO instead of the SOMO are well known for exhibiting magnetoresistance. In particular, BTBN consists of one dibromo-TTF and one NN radical, which are linked by a phenyl coupler group. One of the key factors driving magnetoresistance is the presence of intramolecular ferromagnetic (FM) coupling between the oxidized π-donor (TTF+⋅, D unit) and NN (R unit). Here, a theoretical study is carried out to assess suitable candidates with enhanced FM coupling with respect BTBN, which is thus used as a reference. The study is conducted via in silico chemical modification of the substituents of the BTBN basic functional units (D and R radicals, C coupler) to benefit from the spin polarization mechanism to boost the intramolecular FM coupling, aiming to distort the BTBN radical arrangement within the molecular crystal as little as possible, in the event the material can be synthesized. NICSiso(1) and Wiberg's Bond Order are analyzed to further assist in identifying promising potential candidates, since the decrease in aromaticity is expected to enhance the diradical character and give rise to a larger magnetic coupling value. The most favorable diradical building block to replace the BTBN moiety results from using a hydroxyl-ethylene (-(H)C=C(OH)-) as a coupler preserving BTBN original radicals, namely, NN and TTF+⋅ units. This study aims at illustrating the feasibility of improving the intramolecular FM interaction between radical moieties, which is fully realized, as a first step towards the synthesis of new materials with (possibly) enhanced magnetoresistance properties.

13.
Nanotechnology ; 35(20)2024 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-38286015

RESUMO

A transfer-free graphene with high magnetoresistance (MR) and air stability has been synthesized using nickel-catalyzed atmospheric pressure chemical vapor deposition. The Raman spectrum and Raman mapping reveal the monolayer structure of the transfer-free graphene, which has low defect density, high uniformity, and high coverage (>90%). The temperature-dependent (from 5 to 300 K) current-voltage (I-V) and resistance measurements are performed, showing the semiconductor properties of the transfer-free graphene. Moreover, the MR of the transfer-free graphene has been measured over a wide temperature range (5-300 K) under a magnetic field of 0 to 1 T. As a result of the Lorentz force dominating above 30 K, the transfer-free graphene exhibits positive MR values, reaching ∼8.7% at 300 K under a magnetic field (1 Tesla). On the other hand, MR values are negative below 30 K due to the predominance of the weak localization effect. Furthermore, the temperature-dependent MR values of transfer-free graphene are almost identical with and without a vacuum annealing process, indicating that there are low density of defects and impurities after graphene fabrication processes so as to apply in air-stable sensor applications. This study opens avenues to develop 2D nanomaterial-based sensors for commercial applications in future devices.

14.
Sci Technol Adv Mater ; 25(1): 2388503, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-39156882

RESUMO

A current-perpendicular-to-plane giant magnetoresistive (CPP-GMR) device with a half-metallic electrode is one of the most promising candidates of next-generation read head for hard disk drive. In this study, we fabricate [001]-oriented polycrystalline CPP-GMR devices with the normal ferromagnet (NFM) CoFe/half-metallic ferromagnet (HMFM) Co2FeGa0.5Ge0.5 (CFGG) bilayer electrodes to enhance the magnetoresistance (MR) ratio by large interfacial spin-dependent scattering at the NFM/HMFM interface. The CoFe/CFGG bilayer electrode provides the additional large interfacial spin-dependent scattering and achieves high MR ratio of 22.7% with the CoFe(4.5 nm)/CFGG(2.5 nm) bilayer electrodes, which is almost three(two) times larger than the MR ratio with the single CoFe(CFGG) (7 nm) electrodes. The bias voltage dependent study revealed an additional advantage of increasing the output voltage |ΔV| by using the CoFe/CFGG bilayer due to the improvement of the endurance against spin-transfer torque under high bias current. A maximum output voltage Δ V max of 6.5 mV was obtained with the CoFe(5.5 nm)/CFGG(1.5 nm) electrodes, which is the highest ever reported in the CPP-GMR devices with a uniform metallic spacer including high-quality epitaxial devices.


Large improvement of MR ratio and the highest output voltage has been achieved in the poly-crystalline CPP-GMR with the half-metallic Co2FeGa0.5Ge0.5 and normal ferromagnetic CoFe bilayer electrodes.

15.
Sensors (Basel) ; 24(10)2024 May 11.
Artigo em Inglês | MEDLINE | ID: mdl-38793901

RESUMO

The main purpose of the paper is to show how a magnetoresistive (MR) element can work as a current sensor instead of using a Wheatstone bridge composed by four MR elements, defining the concept of a magnetoresistive shunt (MR-shunt). This concept is reached by considering that once the MR element is biased at a constant current, the voltage drop between its terminals offers information, by the MR effect, of the current to be measured, as happens in a conventional shunt resistor. However, an MR-shunt has the advantage of being a non-dissipative shunt since the current of interest does not circulate through the material, preventing its self-heating. Moreover, it provides galvanic isolation. First, we propose an electronic circuitry enabling the utilization of the available MR sensors integrated into a Wheatstone bridge as sensing elements (MR-shunt). This circuitry allows independent characterization of each of the four elements of the bridge. An independently implemented MR element is also analyzed. Secondly, we propose an electronic conditioning circuit for the MR-shunt, which allows both the bridge-integrated element and the single element to function as current sensors in a similar way to the sensing bridge. Third, the thermal variation in the sensitivity of the MR-shunt, and its temperature coefficient, are obtained. An electronic interface is proposed and analyzed for thermal drift compensation of the MR-shunt current sensitivity. With this hardware compensation, temperature coefficients are experimentally reduced from 0.348%/°C without compensation to -0.008%/°C with compensation for an element integrated in a sensor bridge and from 0.474%/°C to -0.0007%/°C for the single element.

16.
Sensors (Basel) ; 24(3)2024 Feb 04.
Artigo em Inglês | MEDLINE | ID: mdl-38339727

RESUMO

Magnetic position sensors have extensive applications in various industrial sectors and consumer products. However, measuring angles in the full range of 0-360° in a wide field range using a single magnetic sensor remains a challenge. Here, we propose a magnetic position sensor based on a single Wheatstone bridge structure made from a single ferromagnetic layer. By measuring the anisotropic magnetoresistance (AMR) signals from the bridge and two sets of anomalous Nernst effect (ANE) signals from the transverse ports on two perpendicular Wheatstone bridge arms concurrently, we show that it is possible to achieve 0-360° angle detection using a single bridge sensor. The combined use of AMR and ANE signals allows a mean angle error in the range of 0.51-1.05° within a field range of 100 Oe-10,000 Oe to be achieved.

17.
Sensors (Basel) ; 24(18)2024 Sep 19.
Artigo em Inglês | MEDLINE | ID: mdl-39338816

RESUMO

In technology and industrial production, many applications require wide-bandwidth current measurements. In this paper, a signal fusion scheme for a current sensor comprising tunneling magnetoresistance and a current transformer is proposed, achieving a flat frequency response in the DC to MHz range. The measurement principles in different cases of the scheme are introduced, and the total transfer function of the entire scheme is derived by analyzing each section separately. Furthermore, the feasibility and selected parameters of the scheme are verified through a systematic simulation utilizing the MATLAB software. Based on the proposed scheme, a group of principal prototypes are built to experimentally evaluate the bandwidth, amplitude and phase flatness, accuracy, sensitivity, and impulse response. The relative amplitude variation in the passband of the fusion sensor is less than 4%, and the estimated bandwidth of the fusion sensor is close to 17 MHz. The accuracy is better than 0.6%, even when measuring the current at 1 MHz, and the relative standard deviation is 5% when measuring the impulse signal. The sensors developed using this scheme, with a low financial cost, have advantages in many wide-bandwidth current measuring scenarios.

18.
Sensors (Basel) ; 24(5)2024 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-38475156

RESUMO

A new nondestructive inspection method, the magnetic hammer test (MHT), which uses a compact and highly sensitive tunnel magnetoresistance (TMR) sensor, is proposed. This method complements the magnetic flux leakage method and eliminates the issues of the hammer test. It can therefore detect weak magnetic fields generated by the natural vibration of a pipe with a high signal-to-noise ratio. In this study, several steel pipes with different wall thicknesses were measured using a TMR sensor to demonstrate the superiority of MHT. The results of the measurement show that wall thickness can be evaluated with the accuracy of several tens of microns from the change in the natural vibration frequency of the specimen pipe. The pipes were also inspected underwater using a waterproofed TMR sensor, which demonstrated an accuracy of less than 100 µm. The validity of these results was by simulating the shielding of magnetic fields and vibration of the pipes with the finite element method (FEM) analysis. The proposed noncontact, fast, and accurate method for thickness testing of long-distance pipes will contribute to unmanned, manpower-saving nondestructive testing (NDT) in the future.

19.
Sensors (Basel) ; 24(7)2024 Apr 04.
Artigo em Inglês | MEDLINE | ID: mdl-38610505

RESUMO

Magnetic Scanning Microscopy (MSM) emerged with the aim of allowing the visualization of magnetic fields of a sample or material through scanning and proved particularly useful for geology, biomedicine, characterization of magnetic materials, and in the steel industry. In this regard, the reading system of an MSM was modified using a µ-metal magnetic shielding structure to analyze remanent fields. The MSM was adapted to perform readings using two different types of sensors. The sensitive area of the sensors was evaluated, and the HQ-0811 (AKM-Asahi KaseiTM Microdevices) and STJ-010 (Micro MagneticsTM) sensors were chosen, with the HQ-0811 standardized on Printed Circuit Boards (PCBs) to facilitate handling and increase the system's robustness. In the shielded chamber, two piezoelectric ANC-150 stepper motors (Attocube Systems) were used, arranged planarly, to allow the movement of the analyzed samples under the mounted sensors. To acquire data from the sensors, the Precision Current Source Model 6220 and the Nanovoltmeter Model 2182A (both from Keithley) were used, along with Keithley's Delta-Mode integrated system. To analyze the system's effectiveness, three distinct samples were analyzed for calibration, and a MATLAB program was written to analyze the images and extract the material's magnetization. Additionally, a rock sample from the Parnaíba Basin was mapped to demonstrate the system's capabilities.

20.
Sensors (Basel) ; 24(8)2024 Apr 16.
Artigo em Inglês | MEDLINE | ID: mdl-38676164

RESUMO

There are not many high-precision, portable digital compass solutions available right now that can enhance combined navigation systems' overall functionality. Additionally, there is a dearth of writing about these products. This is why a tunnel magnetoresistance (TMR) sensor-based high-precision portable digital compass system is designed. First, the least-squares method is used to compensate for compass inaccuracy once the ellipsoid fitting method has corrected manufacturing and installation errors in the digital compass system. Second, the digital compass's direction angle data is utilized to offset the combined navigation system's mistake. The final objective is to create a high-performing portable TMR digital compass system that will enhance the accuracy and stability of the combined navigation system (abbreviated as CNS). According to the experimental results, the digital compass's azimuth accuracy was 4.1824° before error compensation and 0.4580° after it was applied. The combined navigation system's path is now more accurate overall and is closer to the reference route than it was before the digital compass was added. Furthermore, compared to the combined navigation route without the digital compass, the combined navigation route with the digital compass included is more stable while traveling through the tunnel. It is evident that the digital compass system's design can raise the integrated navigation system's accuracy and stability. The integrated navigation system's overall performance may be somewhat enhanced by this approach.

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