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The exceptional optical, electrical, and mechanical capabilities of layered transition metal carbides, nitrides, and carbonitrides, called MXenes, revolutionized materials science. Among them, Ti3C2 received the most attention owing to the developed synthesis and processing methods, high conductivity, and pronounced plasmonic response. The latter, however, remains controversial with the open question of whether the peak around 800â nm has plasmonic or interband transition origin. To address this issue, we combine spectroscopic ellipsometry and transmittance results with first-principle computations. Their combination reveals that although Ti3C2 is a metal, its optical response becomes plasmonic (Re ε < 0) above 1415â nm, in contrast to the previous understanding. In addition to fundamental significance, this dual dielectric/plasmonic optical response opens a path for theranostic applications, as we demonstrated on the example of Ti3C2 nanospheres. Thus, our study revisits broadband (300-3300â nm) optical constants of Ti3C2 and broadens its application scope in photonics.
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The physics of electrons, photons, and their plasmonic interactions change dramatically when one or more dimensions are reduced to atomic-level thicknesses. For example, graphene exhibits unique electrical, plasmonic, and optical properties. Likewise, atomic-thick metal films are expected to exhibit extraordinary quantum optical properties. Several methods of growing ultrathin metal films were demonstrated, but the quality of the obtained films was much worse compared to bulk films. In this work, we propose a new method of making ultrathin gold films that are close in their properties to bulk gold films. Excellent plasmonic properties are revealed by directly observing quasi-short- and quasi-long-range plasmons in such a film via scanning near-field optical microscopy. The results pave the way for the use of ultrathin gold films in flexible and transparent nanophotonics and optoelectronic applications.
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With the advance of on-chip nanophotonics, there is a high demand for high-refractive-index and low-loss materials. Currently, this technology is dominated by silicon, but van der Waals (vdW) materials with a high refractive index can offer a very advanced alternative. Still, up to now, it was not clear if the optical anisotropy perpendicular to the layers might be a hindering factor for the development of vdW nanophotonics. Here, we studied WS2-based waveguides in terms of their optical properties and, particularly, in terms of possible crosstalk distance. Surprisingly, we discovered that the low refractive index in the direction perpendicular to the atomic layers improves the characteristics of such devices, mainly due to expanding the range of parameters at which single-mode propagation can be achieved. Thus, using anisotropic materials offers new opportunities and novel control knobs when designing nanophotonic devices.
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We propose and study a microstructure based on a dielectric cuboid placed on a thin metal film that can act as an efficient plasmonic lens allowing the focusing of surface plasmons at the subwavelength scale. Using numerical simulations of surface plasmon polariton (SPP) field intensity distributions, we observe high-intensity subwavelength spots and formation of the plasmonic nanojet (PJ) at the telecommunication wavelength of 1530 nm. The fabricated microstructure was characterized using amplitude and phase-resolved scattering-type scanning near-field optical microscopy. We show the first experimental observation of the PJ effect for the SPP waves. Such a novel, to the best of our knowledge, and simple platform can provide new pathways for plasmonics, high-resolution imaging, and biophotonics, as well as optical data storage.
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This publisher's note contains corrections to Opt. Lett.45, 3244 (2020)OPLEDP0146-959210.1364/OL.391861.
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Plasmonic biosensing has been demonstrated to be a powerful technique for quantitative determination of molecular analytes and kinetic analysis of biochemical reactions. However, interfaces of most plasmonic biosensors are made of noble metals, such as gold and silver, which are not compatible with industrial production technologies. This greatly limits biosensing applications beyond biochemical and pharmaceutical research. Here, we propose and investigate copper-based biosensor chips fully fabricated with a standard complementary metal-oxide-semiconductor (CMOS) process. The protection of thin copper films from oxidation is achieved with SiO2 and Al2O3 dielectric films deposited onto the metal surface. In addition, the deposition of dielectric films with thicknesses of only several tens of nanometers significantly improves the biosensing sensitivity, owing to better localization of electromagnetic field above the biosensing surface. According to surface plasmon resonance (SPR) measurements, the copper biosensor chips coated with thin films of SiO2 (25 nm) and Al2O3 (15 nm) show 55% and 75% higher sensitivity to refractive index changes, respectively, in comparison to pure gold sensor chips. To test biomolecule immobilization, the copper-dielectric biosensor chips are coated with graphene oxide linking layers and used for the selective analysis of oligonucleotide hybridization. The proposed plasmonic biosensors make SPR technology more affordable for various applications and provide the basis for compact biosensors integrated with modern electronic devices.
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We report a comprehensive experimental study of optical and electrical properties of thin polycrystalline gold films in a wide range of film thicknesses (from 20 to 200 nm). Our experimental results are supported by theoretical calculations based on the measured morphology of the fabricated gold films. We demonstrate that the dielectric function of the metal is determined by its structural morphology. Although the fabrication process can be absolutely the same for different films, the dielectric function can strongly depend on the film thickness. Our studies show that the imaginary part of the dielectric function of gold, which is responsible for optical losses, rapidly increases as the film thickness decreases for thicknesses below 80 nm. At the same time, we do not observe a noticeable dependence of optical constants on the film thickness for thicker samples. These findings establish design rules for thin-film plasmonic and nanophotonic devices.
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Surface plasmon polaritons can give a unique opportunity to manipulate light at a scale well below the diffraction limit reducing the size of optical components down to that of nanoelectronic circuits. At the same time, plasmonics is mostly based on noble metals, which are not compatible with microelectronics manufacturing technologies. This prevents plasmonic components from integration with both silicon photonics and silicon microelectronics. Here, we demonstrate ultralow-loss copper plasmonic waveguides fabricated in a simple complementary metal-oxide semiconductor (CMOS) compatible process, which can outperform gold plasmonic waveguides simultaneously providing long (>40 µm) propagation length and deep subwavelength (â¼λ(2)/50, where λ is the free-space wavelength) mode confinement in the telecommunication spectral range. These results create the backbone for the development of a CMOS plasmonic platform and its integration in future electronic chips.
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The lattice geometry of natural materials and the structural geometry of artificial materials are crucial factors determining their physical properties. Most materials have predetermined geometries that lead to fixed physical characteristics. Here, the demonstration of a carbon nanotube network serves as an example of a system with controllable orientation achieving on-demand optical properties. Such a network allows programming their optical response depending on the orientation of the constituent carbon nanotubes and leads to the switching of its dielectric tensor from isotropic to anisotropic. Furthermore, it also allows for the achievement of wavelength-dispersion for their principal optical axes - a recently discovered phenomenon in van der Waals triclinic crystals. The results originate from two unique carbon nanotubes features: uniaxial anisotropy from the well-defined cylindrical geometry and the intersection interaction among individual carbon nanotubes. The findings demonstrate that shaping the relative orientations of carbon nanotubes or other quasi-one-dimensional materials of cylindrical symmetry within a network paves the way to a universal method for the creation of systems with desired optical properties.
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The plasmonic sensors based on silver nanoparticles are limited in application due to their relatively fast degradation in the ambient atmosphere. The technology of ion-beam modification for the creation of monocrystalline silver nanoparticles (NPs) with stable plasmonic properties will expand the application of silver nanostructures. In the present study, highly-stable monocrystalline NPs were formed on the basis of a thin silver film by low-energy ion irradiation. Combined with lithography, this technique allows the creation of nanoparticle ensembles in variant forms. The characterization of the nanoparticles formed by ion-beam modification showed long-term outstanding for Ag nanoparticles stability of their plasmonic properties due to their monocrystalline structure. According to optical spectroscopy data, the reliable plasmonic properties in the ambient atmosphere are preserved for up to 39 days. The mapping of crystal violet dye via surface-enhanced Raman spectroscopy (SERS) revealed a strong amplification factor sustaining at least thrice as long as the one of similarly sized polycrystalline silver NPs formed by annealing. The plasmonic properties sustain more than a month of storage in the ambient atmosphere. Thus, ion-beam modification of silver film makes it possible to fabricate NPs with stable plasmonic properties and form clusters of NPs for sensor technology and SERS applications.
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Nature is abundant in material platforms with anisotropic permittivities arising from symmetry reduction that feature a variety of extraordinary optical effects. Principal optical axes are essential characteristics for these effects that define light-matter interaction. Their orientation - an orthogonal Cartesian basis that diagonalizes the permittivity tensor, is often assumed stationary. Here, we show that the low-symmetry triclinic crystalline structure of van der Waals rhenium disulfide and rhenium diselenide is characterized by wandering principal optical axes in the space-wavelength domain with above π/2 degree of rotation for in-plane components. In turn, this leads to wavelength-switchable propagation directions of their waveguide modes. The physical origin of wandering principal optical axes is explained using a multi-exciton phenomenological model and ab initio calculations. We envision that the wandering principal optical axes of the investigated low-symmetry triclinic van der Waals crystals offer a platform for unexplored anisotropic phenomena and nanophotonic applications.
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Ultrathin metal films are an essential platform for two-dimensional (2D) material compatible and flexible optoelectronics. Characterization of thin and ultrathin film-based devices requires a thorough consideration of the crystalline structure and local optical and electrical properties of the metal-2D material interface since they could be dramatically different from the bulk material. Recently, it was demonstrated that the growth of gold on the chemical vapor deposited monolayer MoS2 leads to a continuous metal film that preserves plasmonic optical response and conductivity even at thicknesses below 10 nm. Here, we examined the optical response and morphology of ultrathin gold films deposited on exfoliated MoS2 crystal flakes on the SiO2/Si substrate via scattering-type scanning near-field optical microscopy (s-SNOM). We demonstrate a direct relationship between the ability of thin film to support guided surface plasmon polaritons (SPP) and the s-SNOM signal intensity with a very high spatial resolution. Using this relationship, we observed the evolution of the structure of gold films grown on SiO2 and MoS2 with an increase in thickness. The continuous morphology and superior ability with respect to supporting SPPs of the ultrathin (≤10 nm) gold on MoS2 is further confirmed with scanning electron microscopy and direct observation of SPP fringes via s-SNOM. Our results establish s-SNOM as a tool for testing plasmonic films and motivate further theoretical research on the impact of the interplay between the guided modes and the local optical properties on the s-SNOM signal.
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Metal-Organic CVD method (MOCVD) allows for deposition of ultrathin 2D transition metal dichalcogenides (TMD) films of electronic quality onto wafer-scale substrates. In this work, the effect of temperature on structure, chemical states, and electronic qualities of the MOCVD MoS2 films were investigated. The results demonstrate that the temperature increase in the range of 650 °C to 950 °C results in non-monotonic average crystallite size variation. Atomic force microscopy (AFM), transmission electron microscopy (TEM), and Raman spectroscopy investigation has established the film crystal structure improvement with temperature increase in this range. At the same time, X-Ray photoelectron spectroscopy (XPS) method allowed to reveal non-stoichiometric phase fraction increase, corresponding to increased sulfur vacancies (VS) concentration from approximately 0.9 at.% to 3.6 at.%. Established dependency between the crystallite domains size and VS concentration suggests that these vacancies are form predominantly at the grain boundaries. The results suggest that an increased Vs concentration and enhanced charge carriers scattering at the grains' boundaries should be the primary reasons of films' resistivity increase from 4 kΩ·cm to 39 kΩ·cm.
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Heterogeneous nanostructures composed of metastable tetragonal 1T-MoS2 and stable hexagonal 2H-MoS2 phases are highly promising for a wide range of applications, including catalysis and ion batteries, due to the high electrical conductivity and catalytic activity of the 1T phase. However, a controllable synthesis of stabilized 1T-MoS2 films over the wafer-scale area is challenging. In this work, a metal-organic chemical vapor deposition process allowing us to obtain ultrathin MoS2 films containing both 1T and 2H phases and control their ratio through rhenium doping was suggested. As a result, Mo1-xRexS2 films with a 1T-MoS2 fraction up to ≈30% were obtained, which were relatively stable under normal conditions for a long time. X-ray photoelectron spectroscopy and Raman spectroscopy also indicated that the 1T-MoS2 phase fraction increased with rhenium concentration increase saturating at Re concentrations above 5 at. %. Also, its concentration was found to significantly affect the film resistivity. Thus, the resistivity of the film containing approximately 30% of the 1T phase was about 130 times lower than that of the film without the 1T phase.
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The balance between the mitochondrial respiratory chain activity and the cell's needs in ATP ensures optimal cellular function. Cytochrome c is an essential component of the electron transport chain (ETC), which regulates ETC activity, oxygen consumption, ATP synthesis and can initiate apoptosis. The impact of conformational changes in cytochrome c on its function is not understood for the lack of access to these changes in intact mitochondria. We have developed a novel sensor that uses unique properties of label-free surface-enhanced Raman spectroscopy (SERS) to identify conformational changes in heme of cytochrome c and to elucidate their role in functioning mitochondria. We have verified that molecule bond vibrations assessed by SERS are a reliable indicator of the heme conformation during changes in the inner mitochondrial membrane potential and ETC activity. We have demonstrated that cytochrome c heme reversibly switches between planar and ruffled conformations in response to the inner mitochondrial membrane potential (ΔΨ) and H+ concentration in the intermembrane space. This regulates the efficiency of the mitochondrial respiratory chain, thus, adjusting the mitochondrial respiration to the cell's consumption of ATP and the overall activity. We have found that under hypertensive conditions cytochrome c heme loses its sensitivity to ΔΨ that can affect the regulation of ETC activity. The ability of the proposed SERS-based sensor to track mitochondrial function opens broad perspectives in cell bioenergetics.
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Citocromos c , Heme , Citocromos c/metabolismo , Heme/metabolismo , Potencial da Membrana Mitocondrial , Mitocôndrias/metabolismo , Trifosfato de Adenosina/metabolismoRESUMO
Materials with high optical constants are of paramount importance for efficient light manipulation in nanophotonics applications. Recent advances in materials science have revealed that van der Waals (vdW) materials have large optical responses owing to strong in-plane covalent bonding and weak out-of-plane vdW interactions. However, the optical constants of vdW materials depend on numerous factors, e.g., synthesis and transfer method. Here, we demonstrate that in a broad spectral range (290-3300 nm) the refractive index n and the extinction coefficient k of Bi2Se3 are almost independent of synthesis technology, with only a ~10% difference in n and k between synthesis approaches, unlike other vdW materials, such as MoS2, which has a ~60% difference between synthesis approaches. As a practical demonstration, we showed, using the examples of biosensors and therapeutic nanoparticles, that this slight difference in optical constants results in reproducible efficiency in Bi2Se3-based photonic devices.
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Surface-enhanced Raman spectroscopy (SERS) is a promising tool that can be used in the detection of molecular changes triggered by disease development. Cardiovascular diseases (CVDs) are caused by multiple pathologies originating at the cellular level. The identification of these deteriorations can provide a better understanding of CVD mechanisms, and the monitoring of the identified molecular changes can be employed in the development of novel biosensor tools for early diagnostics. We applied plasmonic SERS nanosensors to assess changes in the properties of erythrocytes under normotensive and hypertensive conditions in the animal model. We found that spontaneous hypertension in rats leads (i) to a decrease in the erythrocyte plasma membrane fluidity and (ii) to a decrease in the mobility of the heme of the membrane-bound hemoglobin. We identified SERS parameters that can be used to detect pathological changes in the plasma membrane and submembrane region of erythrocytes.
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Técnicas Biossensoriais , Hipertensão , Animais , Eritrócitos/química , Eritrócitos/metabolismo , Hemoglobinas/química , Hemoglobinas/metabolismo , Hipertensão/sangue , Hipertensão/diagnóstico , Ratos , Análise Espectral RamanRESUMO
Van der Waals (vdW) heterostructures pave the way to achieve the desired material properties for a variety of applications. In this way, new scientific and industrial challenges and fundamental questions arise. One of them is whether vdW materials preserve their original optical response when assembled in a heterostructure. Here, we resolve this issue for four exemplary monolayer heterostructures: MoS2/Gr, MoS2/hBN, WS2/Gr, and WS2/hBN. Through joint Raman, ellipsometry, and reflectance spectroscopies, we discovered that heterostructures alter MoS2 and WS2 optical constants. Furthermore, despite the similarity of MoS2 and WS2 monolayers, their behavior in heterostructures is markedly different. While MoS2 has large changes, particularly above 3 eV, WS2 experiences modest changes in optical constants. We also detected a transformation from dark into bright exciton for MoS2/Gr heterostructure. In summary, our findings provide clear evidence that the optical response of heterostructures is not the sum of optical properties of its constituents.
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Zinc oxide (ZnO) nanostructures are widely used in various fields of science and technology due to their properties and ease of fabrication. To achieve the desired characteristics for subsequent device application, it is necessary to develop growth methods allowing for control over the nanostructures' morphology and crystallinity governing their optical and electronic properties. In this work, we grow ZnO nanostructures via hydrothermal synthesis using surfactants that significantly affect the growth kinetics. Nanostructures with geometry from nanowires to hexapods are obtained and studied with photoluminescence (PL) spectroscopy. Analysis of the photoluminescence spectra demonstrates pronounced exciton on a neutral donor UV emission in all of the samples. Changing the growth medium chemical composition affects the emission characteristics sufficiently. Apart the UV emission, nanostructures synthesized without the surfactants demonstrate deep-level emission in the visible range with a peak near 620 nm. Structures synthesized with the use of sodium citrate exhibit emission peak near 520 nm, and those with polyethylenimine do not exhibit the deep-level emission. Thus, we demonstrate the correlation between the hydrothermal growth conditions and the obtained ZnO nanostructures' optical properties, opening up new possibilities for their precise control and application in nanophotonics, UV-Vis and white light sources.
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The recent severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) infection has posed a great challenge for the development of ultra-fast methods for virus identification based on sensor principles. We created a structure modeling surface and size of the SARS-CoV-2 virus and used it in comparison with the standard antigen SARS-CoV-2-the receptor-binding domain (RBD) of the S-protein of the envelope of the SARS-CoV-2 virus from the Wuhan strain-for the development of detection of coronaviruses using a DNA-modified, surface-enhanced Raman scattering (SERS)-based aptasensor in sandwich mode: a primary aptamer attached to the plasmonic surface-RBD-covered Ag nanoparticle-the Cy3-labeled secondary aptamer. Fabricated novel hybrid plasmonic structures based on "Ag mirror-SiO2-nanostructured Ag" demonstrate sensitivity for the detection of investigated analytes due to the combination of localized surface plasmons in nanostructured silver surface and the gap surface plasmons in a thin dielectric layer of SiO2 between silver layers. A specific SERS signal has been obtained from SERS-active compounds with RBD-specific DNA aptamers that selectively bind to the S protein of synthetic virion (dissociation constants of DNA-aptamer complexes with protein in the range of 10 nM). The purpose of the study is to systematically analyze the combination of components in an aptamer-based sandwich system. A developed virus size simulating silver particles adsorbed on an aptamer-coated sensor provided a signal different from free RBD. The data obtained are consistent with the theory of signal amplification depending on the distance of the active compound from the amplifying surface and the nature of such a compound. The ability to detect the target virus due to specific interaction with such DNA is quantitatively controlled by the degree of the quenching SERS signal from the labeled compound. Developed indicator sandwich-type systems demonstrate high stability. Such a platform does not require special permissions to work with viruses. Therefore, our approach creates the promising basis for fostering the practical application of ultra-fast, amplification-free methods for detecting coronaviruses based on SARS-CoV-2.