Estimating and correcting mie scattering in synchrotron-based microscopic fourier transform infrared spectra by extended multiplicative signal correction

We present an approach for estimating and correcting Mie scattering occurring in infrared spectra of single cells, at diffraction limited probe size, as in synchrotron based microscopy. The Mie scattering is modeled by extended multiplicative signal correction (EMSC) and subtracted from the vibrational absorption. Because the Mie scattering depends non-linearly on alpha, the product of the radius and the refractive index of the medium/sphere causing it, a new method was developed for estimating the Mie scattering by EMSC for unknown radius and refractive index of the Mie scatterer. The theoretically expected Mie contributions for a range of different alpha values were computed according to the formulae developed by Van de Hulst (1957). The many simulated spectra were then summarized by a six-dimensional subspace model by principal component analysis (PCA). This subspace model was used in EMSC to estimate and correct for Mie scattering, as well as other additive and multiplicative interference effects. The approach was applied to a set of Fourier transform infrared (FT-IR) absorbance spectra measured for individual lung cancer cells in order to remove unwanted interferences and to estimate ranges of important alpha values for each spectrum. The results indicate that several cell components may contribute to the Mie scattering.     

Biological imaging of HEK293 cells expressing PLCgamma1 using surface-enhanced Raman microscopy

Surface-enhanced Raman scattering (SERS) imaging has been used for the targeting and imaging of specific cancer markers in live cells. For this purpose, Au/Ag core-shell nanoparticles, conjugated with monoclonal antibodies, were prepared. The procedures to label live cells with those bimetallic nanoprobes have been developed and used for highly sensitive SERS imaging of live cells. In the present study, live HEK293 cells expressing PLCgamma1 have been used as the optical imaging target. Our results demonstrate the potential feasibility of SERS imaging technology for the highly sensitive imaging of cancer biomarkers in live cells.     

Alloyed Mn-Cu-In-S nanocrystals: a new type of diluted magnetic semiconductor quantum dots

A new type of Mn-Cu-In-S diluted magnetic semiconductor quantum dots was synthesized and reported for the first time. The quantum dots, with no highly toxic elements, not only show the same classic diluted magnetic behavior as Mn-doped CdSe, but also exhibit tunable luminescent properties in a relatively large window from 542 to 648?nm. An absolute photoluminescence quantum yield up to 20% was obtained after the shell growth of ZnS. This kind of magnetic/luminescent bi-functional Mn-Cu-In-S/ZnS core/shell quantum dot might serve as promising nanoprobes for use in dual-mode optical and magnetic resonance imaging techniques.     

Circularly symmetric light scattering from nanoplasmonic spirals

In this paper, we combine experimental dark-field imaging, scattering, and fluorescence spectroscopy with rigorous electrodynamics calculations in order to investigate light scattering from planar arrays of Au nanoparticles arranged in aperiodic spirals with diffuse, circularly symmetric Fourier space. In particular, by studying the three main types of Vogel's spirals fabricated by electron-beam lithography on quartz substrates, we demonstrate polarization-insensitive planar light diffraction in the visible spectral range. Moreover, by combining dark-field imaging with analytical multiparticle calculations in the framework of the generalized Mie theory, we show that plasmonic spirals support distinctive structural resonances with circular symmetry carrying orbital angular momentum. The engineering of light scattering phenomena in deterministic structures with circular Fourier space provides a novel strategy for the realization of optical devices that fully leverage on enhanced, polarization-insensitive light-matter coupling over planar surfaces, such as thin-film plasmonic solar cells, plasmonic polarization devices, and optical biosensors.     

Aptamer‐Directed Synthesis of Multifunctional Lanthanide‐Doped Porous Nanoprobes for Targeted Imaging and Drug Delivery

Multifunctional lanthanide‐doped porous nanoparticles are prepared via a facile one‐step solvothermal route by employing aptamers as the biotemplate. The nanoparticles feature excellent aqueous dispersibility and biospecific properties and could work as effective nanoprobes for targeted imaging and drug delivery. With aptamer being in principle available for any kind of target, this synthetic strategy may open the door to a new generation of nanoprobes for bioapplications such as time‐resolved biodetection, multimode bioimaging/biolabeling, and targeted cancer therapy.     

Electrostatic aggregation and formation of core-shell suprastructures in binary mixtures of charged metal nanoparticles

Electrostatic aggregation of oppositely charged silver and gold nanoparticles leads to the formation of core-shell clusters in which the shell is formed by the nanoparticles, which are in excess. Arguments based on Debye screening of interactions between like-charged particles help explain why these clusters are stable despite possessing net electric charge. The core-shell aggregates exhibit unusual optical properties with the resonance absorption of the shell particles enhanced by the particles in the core and that of the core suppressed by the shell. Experimental UV-vis absorption spectra are faithfully reproduced by Mie theory. The modeling allows for estimation of the numbers of particles forming the shell and of the shell's effective thickness. These theoretical predictions are substantiated by experiments using nanoparticles covered with different combinations of charged groups and performed at different values of pH.     

pH-stimuli-responsive near-infrared optical imaging nanoprobe based on poly(γ-glutamic acid)/poly(β-amino ester) nanoparticles

pH-stimuli-responsive near-infrared optical imaging nanoprobes are designed and synthesized in this study in a facile one-step synthesis process based on the use of the biocompatible and biodegradable polymer poly(γ-glutamic acid) (γ-PGA)/poly(β-amino ester) (PBAE). PBAE has good transfection efficiency and promotes degradation properties under acidic conditions. This pH-responsive degradability can be used for the effective release of encapsulating materials after cellular uptake. As an optical imaging probe, indocyanine green (ICG) is an FDA-approved near-infrared fluorescent dye with a quenching property at a high concentration. In this regard, we focus here on the rapid degradation of PBAE in an acidic environment, in which the nanoparticles are disassembled. This allows the ICG dyes to show enhanced fluorescence signals after being releasing from the particles. We demonstrated this principle in cellular uptake experiments. We expect that the developed pH-stimuli-responsive smart nanoprobes can be applied in intracellular delivery signaling applications.     

Synthesis and characterisation of iron oxide nanoparticles conjugated with epidermal growth factor receptor (EGFR) monoclonal antibody as MRI contrast agent for cancer detection

The aim of this study is to synthesise superparamagnetic iron oxide nanoparticles conjugated with anti‐epidermal growth factor receptor monoclonal antibody (ANTI‐EGFR‐SPION) and investigate its physicochemical characterisation and biocompatibility as a targeted magnetic resonance imaging (MRI) contrast agent for the EGFR‐specific detection in EGFR expressing tumour cells. These particles employed biocompatible polymers, poly(D,L‐lactide‐co‐glycolide) (PLGA) and polyethylene glycol aldehyde (PEG‐aldehyde), to increase the half‐life of particles in circulation and reduce their side effects. The Fe₃ O₄ ‐loaded PLGA‐PEG‐aldehyde nanoparticles were prepared by a modified water‐in‐oil‐in‐water double emulsion method. The EGFR antibody was conjugated to the surface of SPIONs using the aldehyde‐amine reaction. Synthesised conjugates (nanoprobes) were characterised using Fourier transform infrared spectrophotometry, dynamic light scattering, transmission electron microscopy images, and vibrating‐sample magnetometery, and the results showed that the conjugation was successful. The mean diameter of nanoprobes was about 25 nm. These nanoprobes exhibited excellent water‐solubility, stability, and biocompatibility. Meanwhile, MR susceptibility test proved that synthesised nanoprobes can be managed for negative contrast enhancement. The results of this study suggested the potential use of these nanoprobes for non‐invasive molecular MRI in EGFR detection in the future.Inspec keywords: solubility, nanomedicine, cancer, spectrophotometry, emulsions, biomedical MRI, nanomagnetics, nanofabrication, tumours, nanoparticles, magnetic particles, molecular biophysics, light scattering, proteins, cellular biophysics, Fourier transform spectra, superparamagnetism, polymers, transmission electron microscopy, iron compoundsOther keywords: physicochemical characterisation, superparamagnetic iron oxide nanoparticles, novel targeting cancer detection, anti‐epidermal growth factor receptor monoclonal antibody, ANTI‐EGFR‐SPION, biocompatibility, targeted magnetic resonance imaging contrast agent, EGFR‐specific detection, EGFR expressing tumour cells, biocompatible polymers, PLGA‐PEG‐aldehyde nanoparticles, modified water‐in‐oil‐in‐water double emulsion method, EGFR antibody, aldehyde‐amine reaction, synthesised conjugates were characterised using Fourier, transmission electron microscopy images, synthesised nanoprobes, EGFR detection, size 25.0 nm, Fe₃ O₄      

Metal nanoshell assembly on a virus bioscaffold

Chilo iridescent virus is demonstrated as a useful core substrate in the fabrication of metallodielectric, plasmonic nanostructures. A gold shell is assembled around the wild-type viral core by attaching small, 2-5-nm gold nanoparticles to the virus surface by means of the chemical functionality found inherently on the surface of the proteinaceous viral capsid. The density of these nucleation sites was maximized by reducing the repulsive forces between the gold particles through electrolyte addition. These gold nanoparticles then act as nucleation sites for the electroless deposition of gold ions from solution around the biotemplate. The optical extinction spectra of the metalloviral complex is in quantitative agreement with Mie scattering theory. Overall, the utilization of a native virus and the inherent chemical functionality of the capsid afford the ability to grow and harvest biotemplates for metallodielectric nanoshells in large quantities, potentially providing cores with a narrower size distribution and smaller diameters (below 80 nm) than for currently used silica.     

Surface-enhanced Raman scattering-based nanoprobe for high-resolution, non-scanning chemical imaging

This work describes the development and demonstration of a non-scanning chemical imaging probe, capable of obtaining surface-enhanced Raman scattering (SERS) images of samples with which it is in direct contact. The SERS imaging arrays (i.e., nanoprobes) are used in a signal collection mode to obtain images by measuring as many as 30 000 individual sub-diffraction-limited locations on a sample's surface simultaneously. These SERS probes are fabricated from coherent fiber-optic imaging bundles, allowing for the formation of a highly ordered roughened metal surface, capable of providing uniform SERS enhancement (<2.0% relative standard deviation) across the entire imaging surface. These optimized SERS nanoprobes have potential application to a wide range of research fields from materials science to cellular biology.     

Investigation of concentrically and eccentrically layered droplets by light scattering

Two pairs of immiscible liquid compounds are chosen to prepare levitated layered droplets with and without density difference between core and layer phases. The droplets are examined by light scattering along two orthogonal directions. A layered droplet without phase density difference is unambiguously identified as a concentric sphere by matching the observed scattering spectra with those calculated from the Aden-Kerker extension of Mie theory. For layered droplets with phase density difference, only the scattering spectrum from one of the scattering directions can be matched theoretically. These observations suggest that a static layered droplet is predominantly eccentric even though the embedded core is large by volume, as predicted from fluid mechanics. The consistency of the light-scattering characterization with the diffusion theory governing the evaporation of concentrically and eccentrically layered droplets is also established.     

Optical waveguiding in suspensions of dielectric particles

An optical waveguide formed by a suspension of dielectric nanoparticles in a microchannel is described. The suspensions, chosen for their guiding and scattering properties, are silica and polystyrene particles that have diameters of 30-900 nm and are dispersed in water with volume fractions up to 10%. Changing the diameter and concentration of the particles causes the suspensions to transition from Rayleigh to Mie scattering and from single to multiple scattering. The threshold for optical guiding in a waveguide core composed of these suspensions is set by the numerical aperture of the effective refractive-index difference introduced by the suspension and not by the average interparticle distance.     

Determination of Particle Sizes and Crystalline Phases on Colloidal Silicon Nanoparticle Suspensions

1.IDtroductionLightscatteringpropertiesofsphericalparticlescanbedescribedbyMietheoryl1]whichcanbeaP-pliedtocolloidalparticlessuspendedinthegasorliquidphase.Withsomecarethetheorycanevenbeap-pliedtodrypowdersorparticlesonasolidsupport[2]lthoughitisstrictlyvalidonlyforisolatedsphericalparticles.Informationonparticlesizer,sizedistribu-tionandnumberdensitiesN(r),andrefractiveindexhcanberetrievedbyexperimentaldata.Theex-tinctioncoefficient7ofacolloidalsuspension,forex-ample,canbedeterminedfromthea…     

Dependence of fluorescence intensity on the spectral overlap between fluorophores and plasmon resonant single silver nanoparticles

We investigate the fluorescence from dyes coupled to individual DNA-functionalized metal nanoparticles. We use single-particle darkfield scattering and fluorescence microscopy to correlate the fluorescence intensity of the dyes with the localized surface plasmon resonance (LSPR) spectra of the individual metal nanoparticles to which they are attached. For each of three different dyes, we observe a strong correlation between the fluorescence intensity of the dye and the degree of spectral overlap with the plasmon resonance of the nanoparticle. On average, we observe the brightest fluorescence from dyes attached to metal nanoparticles that have a LSPR scattering peak approximately 40-120 meV higher in energy than the emission peak of the fluorophore. These results should prove useful for understanding and optimizing metal-enhanced fluorescence.     

Fluorescence Quenching Nanoprobes Dedicated to In Vivo Photoacoustic Imaging and High‐Efficient Tumor Therapy in Deep‐Seated Tissue

Photoacoustic imaging (PAI) and photoacoustic (PA) therapy have promising applications for treating tumors. It is known that the utilization of high‐absorption‐coefficient probes can selectively enhance the PAI target contrast and PA tumor therapy efficiency in deep‐seated tissue. Here, the design of a probe with the highest availability of optical‐thermo conversion by using graphene oxide (GO) and dyes via π–π stacking interactions is reported. The GO serves as a base material for loading dyes and quenching dye fluorescence via fluorescence resonance energy transfer (FRET), with the one purpose of maximum of PA efficiency. Experiments verify that the designed fluorescence quenching nanoprobes can produce stronger PA signals than the sum of the separate signals generated in the dye and the GO. Potential applications of the fluorescence quenching nanoprobes are demonstrated, dedicating to enhance PA contrast of targets in deep‐seated tissues and tumors in living mice. PA therapy efficiency both in vitro and in vivo by using the fluorescence quenching nanoprobes is found to be higher than with the commonly used PA therapy agents. Taken together, quenching dye fluorescence via FRET will provide a valid means for developing high‐efficiency PA probes. Fluorescence quenching nanoprobes are likely to become a promising candidate for deep‐seated tumor imaging and therapy.     

Synthesis,self-assembly,and characterization of PEG-coated iron oxide nanoparticles as potential MRI contrast agent

Aim: Investigated the self-assembly and characterization of novel antifouling polyethylene glycol (PEG)-coated iron oxide nanoparticles as nanoprobes for magnetic resonance imaging (MRI) contrast agent. Method: Monodisperse oleic acid-coated superparamagnetic iron oxide cores are synthesized by thermal decomposition of iron oleate. The self-assembly behavior between iron oxide cores and PEG-lipid conjugates in water and their characteristics are confirmed by transmission electron microscope, X-ray diffraction, thermogravimetric analysis, Fourier transform infrared spectroscopy, and vibrating sample magnetometer. Result: Dynamic light scattering shows superparamagnetic iron oxide nanoparticles coated with PEG are stable in water for pH of 3–10 and ionic strengths up to 0.3 M NaCl, and are protein resistant in physiological conditions. Additionally, in vitro MRI study demonstrates the efficient magnetic resonance imaging contrast characteristics of the iron oxide nanoparticles. Conclusion: The result indicates that the novel antifouling PEG-coated superparamagnetic iron oxide nanoparticles could potentially be used in a wide range of applications such as biotechnology, MRI, and magnetic fluid hyperthermia.     

Determination of the scattering coefficient and the anisotropy factor from laser Doppler spectra of liquids including blood

Laser Doppler measurements were performed on scattering liquids flowing through a highly scattering static medium to determine the scattering coefficient and the anisotropy factor of the liquids. Monte Carlo simulations of light propagation in the static and moving media were used to calculate the Doppler spectra for suspensions of polystyrene spheres in water, and these spectra were in excellent agreement with experimental results. A faster Monte Carlo code was developed so that nonlinear regressions to the measured laser Doppler spectra could be used to determine the anisotropy factor of other liquids. This approach was used to deduce the scattering properties of Intralipid and blood at λ = 820 nm. It was found that the anisotropy factor of blood is well described by Mie theory in contradiction to results reported in the literature that were obtained by goniometric measurement of the phase function.     

Gold and Hairpin DNA Functionalization of Upconversion Nanocrystals for Imaging and In Vivo Drug Delivery

Although multifunctional upconversion imaging probes have recently attracted considerable interest in biomedical research, there are currently few methods for stabilizing these luminescent nanoprobes with oligonucleotides in biological systems. Herein, a method to robustly disperse upconversion nanoprobes in physiological buffers based on rational design and synthesis of nanoconjugates comprising hairpin‐DNA‐modified gold nanoparticles is presented. This approach imparts the upconversion nanoprobes with excellent biocompatibility and circumvents the problem of particle agglomeration. By combining single‐band anti‐Stokes near‐infrared emission and the photothermal effect mediated by the coupling of gold to upconversion nanoparticles, a simple, versatile nanoparticulate system for simultaneous deep‐tissue imaging and drug molecule release in vivo is demonstrated.     

Split‐GFP: SERS Enhancers in Plasmonic Nanocluster Probes

The assembly of plasmonic metal nanoparticles into hot spot surface‐enhanced Raman scattering (SERS) nanocluster probes is a powerful, yet challenging approach for ultrasensitive biosensing. Scaffolding strategies based on self‐complementary peptides and proteins are of increasing interest for these assemblies, but the electronic and the photonic properties of such hybrid nanoclusters remain difficult to predict and optimize. Here, split‐green fluorescence protein (sGFP) fragments are used as molecular glue and the GFP chromophore is used as a Raman reporter to assemble a variety of gold nanoparticle (AuNP) clusters and explore their plasmonic properties by numerical modeling. It is shown that GFP seeding of plasmonic nanogaps in AuNP/GFP hybrid nanoclusters increases near‐field dipolar couplings between AuNPs and provides SERS enhancement factors above 10⁸. Among the different nanoclusters studied, AuNP/GFP chains allow near‐infrared SERS detection of the GFP chromophore imidazolinone/exocyclic C?C vibrational mode with theoretical enhancement factors of 10⁸–10⁹. For larger AuNP/GFP assemblies, the presence of non‐GFP seeded nanogaps between tightly packed nanoparticles reduces near‐field enhancements at Raman active hot spots, indicating that excessive clustering can decrease SERS amplifications. This study provides rationales to optimize the controlled assembly of hot spot SERS nanoprobes for remote biosensing using Raman reporters that act as molecular glue between plasmonic nanoparticles.     

A New Closed-Form Solution to Light Scattering by Spherical Nanoshells

Light or electromagnetic wave scattered by a single sphere or a coated sphere has been considered as a classic Mie theory. There have been some further extensions that were made further based on the Mie theory. Recently, a closed-form analytical model of the scattering cross section of a single nanoshell has been considered. The present paper is documented further, based on the work in 2006 by Alam and Massoud, to derive another different closed-form solution to the problem of light scattered by the nanoshells using polynomials of up to order 6. Validation is made by comparing the present closed-form solution to the exact Mie scattering solution and also to the other closed-form solution by Alam and Massoud. This study is found to be, however, more generalized and also more accurate for the coated spheres of either tiny/small or medium sizes than that of Alam and Massoud. Therefore, the derived formulas can be used for accurately characterizing both surface plasmon resonances of nanoparticles (of small sizes) or nanoantenna near-field properties (of medium sizes comparable with half wavelength).