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Correction for 'A novel concept of two-component dielectric function for gold nanostars: theoretical modelling and experimental verification' by Nikolai G. Khlebtsov et al., Nanoscale, 2020, 12, 19963-19981, DOI: 10.1039/D0NR02531C.
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An important direction in the development of X-ray computed tomography sensors in systems with increased scanning speed and spatial resolution is the creation of an array of miniature current sources. In this paper, we describe a new material based on gold nanostars (GNS) embedded in nanoscale diamond-like carbon (DLC) films (thickness of 20 nm) for constructing a pixel current source with photoinduced electron emission. The effect of localized surface plasmon resonance in GNS on optical properties in the wavelength range from UV to near IR, peculiarities of localization of field and thermal sources, generation of high-energy hot electrons, and mechanisms of their transportation in vacuum are investigated. The advantages of the proposed material and the prospects for using X-ray computed tomography in the matrix source are evaluated.
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Rational design of AuNST morphology requires adequate computational models. The bulk dielectric function is not applicable to sharp nanostar spikes. We suggest a two-component dielectric function in which the nanostar core is treated as a bulk material, whereas the size-corrected dielectric function of the spikes is treated by a modified Coronado-Schatz model. In addition to the strong broadening of plasmonic peaks, the simulated absorption and scattering spectra show unusual properties, which are not observed with bulk dielectric functions. The effect of NIR water absorption on nanostar spectra is small, and the absorption peak demonstrates the expected small decrease in the absorbing media. Surprisingly, however, water absorption increases the scattering peak by 30%. For the common surfactant-free Vo-Dinh AuNSTs, we report, for the first time, very intense SWIR plasmonic peaks around 1900 nm, in addition to the common strong peak in the UV-vis-NIR band (here, at 1100 nm). For bilayers of AuNSTs in air, we recorded two similarly intense peaks near 800 and 1500 nm. To simulate the experimental extinction spectra of colloids and bilayers on glass in air, we develop a statistical model that includes the major fraction of typical Vo-Dinh AuNSTs and two minor fractions of sea urchins and particles with protrusions. In contrast to the general belief, we show that the common UV-vis-NIR plasmonic peak of surfactant-free AuNSTs is related to short spikes on a spherical core, whereas long spikes produce an intense SWIR plasmonic mode. Such a structural assignment of vis-NIR and SWIR peaks does not seem to have been reported previously for surfactant-free nanostars. With our model, we demonstrate good agreement between simulated and measured spectra of colloids and bilayers on glass in air.
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Gold nanoparticles (AuNPs) of different size and shape are widely used as photosensitizers for cancer diagnostics and plasmonic photothermal (PPT)/photodynamic (PDT) therapy, as nanocarriers for drug delivery and laser-mediated pathogen killing, even the underlying mechanisms of treatment effects remain poorly understood. There is a need in analyzing and improving the ways to increase accumulation of AuNP in tumors and other crucial steps in interaction of AuNPs with laser light and tissues. In this review, we summarize our recent theoretical, experimental, and pre-clinical results on light activated interaction of AuNPs with tissues and cells. Specifically, we discuss a combined PPT/PDT treatment of tumors and killing of pathogen bacteria with gold-based nanocomposites and atomic clusters, cell optoporation, and theoretical simulations of nanoparticle-mediated laser heating of tissues and cells.
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Ouro/química , Nanopartículas Metálicas/química , Nanotubos/química , Fotoquimioterapia , Dióxido de Silício/químicaRESUMO
This paper discusses one of the key problems of laser-induced tissue/cell hyperthermia mediated by gold nanoparticles, namely, quantifying and precise prediction of the light exposure to provide a controllable local heating impact on living organisms. The distributions of such parameters as an efficiency factor of absorption, differential and integral absorbing power of a nanoparticle, temperature increment, and Arrhenius damage integral were used to quantify nanoparticle effectiveness in the two-dimensional coordinate space "laser wavelength (λ) × radius of gold nanoparticles (R)." It was found that the fulfillment of required spatial and temporal characteristics of temperature fields in the vicinity of nanoparticle determines the optimal λ and R. As a result, the area in the space (λ × R) with a minimal criticality to alterations of the local hyperthermia may be significantly displaced from the position of the plasmonic resonance. The aspects of generalization of the proposed methodology for the analysis of local hyperthermia using nanoparticles of different shapes (nanoshells, nanorods, nanostars) and short pulse laser radiation are discussed.
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Ouro/química , Hipertermia Induzida/métodos , Lasers , Nanopartículas Metálicas/química , DNA/química , Temperatura Alta , Humanos , Luz , Nanopartículas/química , Nanoconchas/química , Nanosferas/química , Nanotecnologia , Óptica e Fotônica , Tamanho da Partícula , Ressonância de Plasmônio de Superfície/instrumentação , Ressonância de Plasmônio de Superfície/métodos , TemperaturaRESUMO
We present a simple scheme of narrowband terahertz (THz) generation by optical rectification in the lithium niobate crystal covered by a binary phase mask. It is shown that a single-domain crystal illumination by spatiotemporal shaped fs-laser pulses is equivalent to the formation of a transversally patterned, quasi-phase-matching structure. Decrease of the optical beam size on the mask leads to an increase of the THz-wave linewidth from 17 GHz to a few THz. The frequency of the generation was tuned in the range of 0.4-1.0 THz by building images of the mask in the crystal with various magnifications. Application results of the presented THz source for measuring transmittance of the superconducting NbN thin film in the 4.2-15 K temperature range are also presented.
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It is theoretically shown that application of a phase mask in optical rectification scheme is equivalent to spatial modulation of the crystal's nonlinear coefficient in cross-section plane of the laser beam. It allows using the technique of quasi-phase-matching for efficient noncollinear terahertz (THz) generation by using high-power wide-aperture optical beam. According to calculations, the linewidth of THz generation can be varied from 10 GHz to a few THz by changing the optical beam size. It is shown that the frequency of THz generation can be also tuned by building the image of the phase mask in the crystal with variable magnification.
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Heating of composite plasmon-resonant nanoparticles (spherical gold nanoshells) under pulse laser illumination is considered. The numerical solution of the time-dependent heat conduction equation accounting for spatial inhomogeneities of absorbed laser radiation is performed. Important features of temperature kinetics and thermal flux inside nanoparticles are analyzed. Possible applications of the observed effects in nanotechnology and medicine are discussed.
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Transferência de Energia , Lasers , Nanopartículas Metálicas , Ressonância de Plasmônio de Superfície , OuroRESUMO
A new scheme of optical rectification (OR) of femtosecond laser pulses in a periodically poled lithium niobate (PPLN) crystal, which generates high energy and bandwidth tunable multicycle THz pulses, is proposed and demonstrated. We show that the number of the oscillation cycles of the THz electric field and therefore bandwidth of generated THz spectrum can easily and smoothly be tuned from a few tens of GHz to a few THz by changing the pump optical spot size on PPLN crystal. The minimal bandwidth is 17 GHz that is smallest ever of reported in scheme of THz generation by OR at room temperature. Similar to the case of Cherenkov-type OR in single-domain LiNbO3, the spectrum of THz generation extends from 0.1 THz to 3 THz when laser beam is focused to a size close to half-period of PPLN structure. The energy spectral density of narrowband THz generation is almost independent of the bandwidth and is typically 220 nJ/THz for ~1 W pump power at 1 kHz repetition rate.
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Photonic nanotechnologies have good perspectives to be widely used in biophotonics. In this study we have developed an approach for calculation of nanoparticle temperature field accounting for absorbed local intensity at pulse laser radiation of composite spherical nanoparticles (nanoshells). This approach allowed us to analyze spatial inhomogeneities of light field diffracted into a nanoshell and corresponding distribution of the absorption energy and to provide numerical solution of time-dependent heat conduction equation accounting for corresponding spatially inhomogeneous distribution of heating sources. We were able to predict the appearance of a novel thermal effect - hoop-shaped hot zone on the nanoshell surface. The observed effect has potential applications in cell biology and medicine for controlled cell optoporation and nanosurgery, as well as cancer cell killing.
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Lasers , Nanopartículas/química , Temperatura , Absorção , Pesquisa Biomédica , Elétrons , Fatores de TempoRESUMO
A scheme of terahertz (THz)-wave surface-emitted difference-frequency generation (SEDFG), which lacks the drawbacks associated with the usage of periodically orientation-inverted structures, is proposed. It is shown that both material birefringence of the bulk LiNbO(3) crystal and modal birefringence of GaAs/AlAs waveguide are sufficient to obtain SEDFG up to a frequency of approximately 3THz. The simplicity of the proposed scheme, along with the fact that there is a much smaller THz-wave decay in nonlinear crystal, makes it a good candidate for the practical realization of efficient THz generation. The use of a GaAs waveguide with an oxidized AlAs layer is proposed for enhanced THz-wave SEDFG in the vicinity of the GaAs polariton resonance at 8THz.
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We report on the demonstration of surface-emitted terahertz- (THz-) wave difference-frequency generation from two-dimensional (2D) periodically poled lithium niobate (PPLN). The two orthogonal periodic structures individually compensate for both the phase mismatch of the launched lasers and the generated THz wave. Tunable 1.5-1.8 THz wave generation with a bandwidth of 10-GHz was obtained by use of two 2D PPLN crystals. We also confirmed that THz waves were simultaneously generated into two opposite directions, which suggests the possibility of higher THz-wave output power.