INVESTIGATION OF THE SCATTERING OF GAS MOLECULES ON VARIOUS SURFACES
Gas dynamics - scattering of gas molecules on various surfaces
RAREFIED GAS DYNAMICS↗
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Surface-Enhanced Raman Scattering Optophysiology Nanofibers for the Detection of Heavy Metals in Single Breast Cancer Cells
Mercury(II) ions (Hg2+) and silver ions (Ag+) are two of the most hazardous pollutants causing serious damage to human health. Here, we constructed surface enhanced Raman scattering (SERS)-active nanofibers covered with 4-mercaptopyridine (4-Mpy)-modified gold nanoparticles (AuNPs) to detect Hg2+ and Ag+. Experimental evidence suggests that the observed spectral changes originate from the combined effect of (i) the coordination between the nitrogen on 4-Mpy and the metal ions and (ii) the 4-Mpy molecular orientation (from flatter to more perpendicular with respect to the metal surface). The relative intensity of a pair of characteristic Raman peaks (at ~428 and ~708 cm-1) was used to quantify the metal ion concentration, greatly increasing the reproducibility of the measurement compared to signal-on or signal-off detection based on a single SERS peak. The detection limit of this method for Hg2+ is lower than that for the Ag+ (5 nM vs 100 nM), which can be explained by the stronger interaction energy between Hg2+ and N compared to Ag+ and N, as demonstrated by density functional theory (DFT) calculations. The Hg2+ and Ag+ ions can be masked by adding ethylenediaminetetraacetate (EDTA) and Cl-, respectively, to the Hg2+ and Ag+ samples. The good sensitivity, high reproducibility and excellent selectivity of these nanosensors were also demonstrated. Furthermore, detection of Hg2+ in living breast cancer cells at the subcellular level is possible thanks to the nanometric size of the herein described SERS nanosensors, allowing high spatial resolution and minimal cell damage.
Zhao, Xingjuan↗
Differentiation and classification of bacterial endotoxins based on surface enhanced Raman scattering and advanced machine learning
Bacterial endotoxin, a major component of the Gram-negative bacterial outer membrane leaflet, is a lipopolysaccharide shed from bacteria during their growth and infection and can be utilized as a biomarker for bacterial detection. Here, the surface enhanced Raman scattering (SERS) spectra of eleven bacterial endotoxins with an average detection amount of 8.75 pg per measurement have been obtained based on silver nanorod array substrates, and the characteristic SERS peaks have been identified. With appropriate spectral pre-processing procedures, different classical machine learning algorithms, including support vector machine, k-nearest neighbor, random forest, etc., and a modified deep learning algorithm, RamanNet, have been applied to differentiate and classify these endotoxins. It has been found that most conventional machine learning algorithms can attain a differentiation accuracy of >99%, while RamanNet can achieve 100% accuracy. Such an approach has the potential for precise classification of endotoxins and could be used for rapid medical diagnoses and therapeutic decisions for pathogenic infections.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Surface-Enhanced Raman Scattering Using Silica Whispering-Gallery Mode Resonators
The motivation of this work was to have robust spectroscopic sensors for sensitive detection and chemical analysis of organic and molecular compounds. The solution is to use silica sphere optical resonators to provide surface-enhanced spectroscopic signal. Whispering-gallery mode (WGM) resonators made from silica microspheres were used for surface-enhanced Raman scattering (SERS) without coupling to a plasmonic mechanism. Large Raman signal enhancement is observed by exclusively using 5.08-micron silica spheres with 785-nm laser excitation. The advantage of this non-plasmonic approach is that the active substrate is chemically inert silica, thermally stable, and relatively simple to fabricate. The Raman signal enhancement is broadly applicable to a wide range of molecular functional groups including aliphatic hydrocarbons, siloxanes, and esters. Applications include trace organic analysis, particularly for in situ planetary instruments that require robust sensors with consistent response.
Anderson, Mark S.↗
Sinusoidal reaction formulation for radiation and scattering from conducting surfaces
The piecewise-sinusoidal reaction technique was developed for low-frequency scattering and radiation from perfectly conducting bodies of arbitrary shape. The theory and numerical results for scattering patterns of rectangular plates and radiation patterns of corner-reflector antennas are presented.
Richmond, J. H.↗
Stern layers on RuO2 (100) and (110) in electrolyte: Surface X-ray scattering studies
Electrochemical Stern layers are observed on the surfaces of RuO 2 single crystals in 0.1 M CsF electrolyte. The Stern layers formed at the interfaces of RuO 2 (110) and (100) are compared to the previously reported Stern layer on Pt (111) [Liu et al., J. Phys. Chem. Lett., 9 (2018) 1265]. While the Cs + density profiles at the potentials close to hydrogen evolution reactions are similar, the hydration layers intervening the surface and the Cs + layer are significantly denser on RuO 2 surfaces than that on Pt(111) surface, reflecting the oxygen termination of RuO 2 surfaces. The overall similarities between Stern layers on ruthenium surfaces and platinum surface suggest the universal presence of Stern layers in all well-defined solid-electrolyte interfaces.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Surface reconstruction from scattered data through pruning of unstructured grids
This paper describes an algorithm for reconstructing a surface from a randomly digitized object. Scan data (treated as a cloud of points) is first tesselated out to its convex hull using Delaunay triangulation. The line-of-sight between each surface point and the scanning device is traversed, and any tetrahedra which are pierced by it are removed. The remaining tetrahedra form an approximate solid model of the scanned object. Due to the inherently limited resolution of any scan, this algorithm requires two additional procedures to produce a smooth, polyhedral surface: one process removes long, narrow tetrahedra which span indentations in the surface between digitized points; the other smooths sharp edges. The results for a moderately resolved sample body and a highly resolved aircraft are displayed.
Maksymiuk, C. M.↗
Controlling the Aspect Ratios of Au Nanocrystals with Ag+ Addition Time in Seed-Mediated Synthesis: Implications for Surface-Enhanced Raman Scattering
Among various factors playing pivotal roles in the typical seed-mediated growth of Au nanocrystals (NCs), the role of Ag (AgNO3) has remained debatable over time and seminal research efforts have helped us in reaching a consensus, albeit from the standpoint of [Ag+] concentration. This study aims to provide an understanding of the role of Ag+ from the perspective of time. Here, we show that different Au NCs with tunable aspect ratios (ARs) can be generated in one system in high yield simply by varying the time of addition of Ag+ in the growth solution. The generality of the method has been demonstrated in tuning the ARs of anisotropic Au NCs like concave cuboid (CCB, AR = 2) and elongated tetrahexahedra (AR = 2.5), where the delayed addition of Ag+ leads to the formation of their isotropic counterpart concave cube (CC, AR = 1) and tetrahexahedra (AR = 1), respectively. This work, apart from establishing timed addition of Ag+ as a crucial parameter in controlling the AR, may also help in the realization of a universal growth mechanism of Au NCs. The Au NCs with varying ARs (CCB, AR = 2 and CC, AR = 1) have been further explored as potential substrates for surface-enhanced Raman scattering (SERS) due to the presence of their high-index facets and sharp tips.
KEYWORDS:Au nanoparticles seed-mediated growth hig↗
Retrieval of Soil Moisture and Roughness from the Polarimetric Radar Response
The main objective of this investigation was the characterization of soil moisture using imaging radars. In order to accomplish this task, a number of intermediate steps had to be undertaken. In this proposal, the theoretical, numerical, and experimental aspects of electromagnetic scattering from natural surfaces was considered with emphasis on remote sensing of soil moisture. In the general case, the microwave backscatter from natural surfaces is mainly influenced by three major factors: (1) the roughness statistics of the soil surface, (2) soil moisture content, and (3) soil surface cover. First the scattering problem from bare-soil surfaces was considered and a hybrid model that relates the radar backscattering coefficient to soil moisture and surface roughness was developed. This model is based on extensive experimental measurements of the radar polarimetric backscatter response of bare soil surfaces at microwave frequencies over a wide range of moisture conditions and roughness scales in conjunction with existing theoretical surface scattering models in limiting cases (small perturbation, physical optics, and geometrical optics models). Also a simple inversion algorithm capable of providing accurate estimates of soil moisture content and surface rms height from single-frequency multi-polarization radar observations was developed. The accuracy of the model and its inversion algorithm is demonstrated using independent data sets. Next the hybrid model for bare-soil surfaces is made fully polarimetric by incorporating the parameters of the co- and cross-polarized phase difference into the model. Experimental data in conjunction with numerical simulations are used to relate the soil moisture content and surface roughness to the phase difference statistics. For this purpose, a novel numerical scattering simulation for inhomogeneous dielectric random surfaces was developed. Finally the scattering problem of short vegetation cover above a rough soil surface was considered. A general scattering model for grass-blades of arbitrary cross section was developed and incorporated in a first order random media model. The vegetation model and the bare-soil model are combined and the accuracy of the combined model is evaluated against experimental observations from a wheat field over the entire growing season. A complete set of ground-truth data and polarimetric backscatter data were collected. Also an inversion algorithm for estimating soil moisture and surface roughness from multi-polarized multi-frequency observations of vegetation-covered ground is developed.
Sarabandi, Kamal↗
A model of diffuse radar scattering from Martian surface rocks
Two physically plausible surface rock-orientation models are presently used to characterize the depolarized component of diffuse radar energy scattering on Mars, and plots of scattering cross-section are derived as a function of Doppler shift. The spectral shapes thus modeled exhibit similarities to observed spectra; their magnitudes are generally within a factor of about 2 of measured values. While surface inhomogeneities could account for the degree of discrepancy, subsurface element scattering may also be implicated.
Calvin, Wendy M.↗
A numerical study of electromagnetic scattering from ocean like surfaces
The integral equations describing electromagnetic scattering from one dimensional conducting surfaces are formulated and numerical results are presented. The results are compared with those obtained using approximate methods such as physical optics, geometrical optics, and perturbation theory. The integral equation solutions show that the surface radius of curvature must be greater than 2.5 wavelengths for either the physical optics or geometric optics to give satisfactory results. It has also been shown that perturbation theory agrees with the exact fields as long as the root mean square surface roughness is less than one-tenth of a wavelength.
Lentz, R. R.↗
A measurement of the angular distribution of 5 eV atomic oxygen scattered off a solid surface in earth orbit
The angular distribution of 5 eV atomic oxygen scattered off a polished vitreous carbon surface was measured on a recent Space Shuttle flight. The experimental apparatus was of novel design, completely passive, and used thin silver films as the recording device for oxygen atoms. Most of the incident oxygen was contained in the reflected beam and remained in an active form and probably still atoms. Allowance was made for 12 percent loss of incident atoms which are converted to CO at the carbon surface. The scattered distribution which is wide lobular, peaking 15 deg in the forward direction, shows almost but not quite full accommodation.
Gregory, John C.↗
C-1 surface interpolation for scattered data on a sphere
An algorithm is described for constructing a smooth computable function, f, defined over the surface of a sphere and interpolating a set of n data values, u sub i, associated with n locations, P sub i, on the surface of the sphere. The interpolation function, f, will be continuous and have continuous first partial derivatives. The locations, p sub i, are not required to lie on any type of regular grid.
Lawson, C. L.↗
Surface Enhanced Raman Scattering Selectivity in Proteins Arises from Electron Capture and Resonant Enhancement of Radical Species
Plasmon-enhanced Raman scattering is a powerful approach to detecting and characterizing proteins in live and dynamic biological systems. However, the selective detection/enhancement of specific residues as well as spectral diffusion and fluctuations have complicated the interpretation of enhanced Raman spectra and images of biological matter. In this paper, we therefore demonstrate that the amino acid tryptophan (Trp) can capture an electron from an excited plasmon, which generates a radical anion that is resonantly enhanced: a visible excited electronic state slides into resonance upon charging. This surface enhanced resonance Raman scattering (SERRS) mechanism explains the persistence of Trp signatures in the SERS and TERS spectra of proteins. Evidence for this picture includes the observation of visible resonances in the UV-Vis extinction spectrum, changes in the ground state vibrational spectrum, and plasmon-resonance dependent behavior. DFT calculations support the experimental observations. The behavior observed from the free Trp molecule is shown to explain the SERS spectrum of the Trp-cage protein. In effect, resonant Raman scattering from radicals formed through plasmonic excitation represents an under-investigated mechanism that may be exploited for chemical sensing applications. This work was supported by the National Institutes of Health Award R01-GM109988. The authors thank Hannah Shafaat for helpful discussions and providing an azurin sample for comparison. The authors also thank Joel Harris for providing constructive comments on our manuscript.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Scattering of light from particulate surfaces. I - A laboratory assessment of multiple-scattering effects
In planetary applications it is sometimes important to know the degree to which multiple scattering is influencing the photometric properties of a surface. An investigation is conducted concerning the point at which the single-scattering approximation used in the theory developed by Hapke (1963) and Irvine (1966) breaks down. It is shown that the Hapke-Irvine photometric function provides an adequate representation of the scattering properties of particulate surfaces whose geometric albedos (or normal reflectances) do not exceed 0.3. An experiment is conducted to estimate the normal reflectance below which the Hapke-Irvine equation considered provides an adequate representation of the scattering properties of a particulate surface. The investigation makes use of a set of samples which were prepared by mixing magnesium oxide and charcoal powders. The samples have a range in normal reflectance from 0.04 to 1.04.
Veverka, J.↗
A scattering model for defoliated vegetation
A scattering model for defoliated vegetation is conceived as a layer of dielectric, finite-length cylinders with specified size and orientation distributions above an irregular ground surface. The scattering phase matrix of a single cylinder is computed, then the radiative transfer technique is applied to link volume scattering from vegetation to surface scattering from the soil surface. Polarized and depolarized scattering are computed and the effects of the cylinder size and orientation distributions are illustrated. It is found that size and orientation distributions have significant effects on the backscattered signal. The model is compared with scattering from defoliated trees and agricultural crops.
Karam, M. A.↗
Effects of surface contamination on the infrared emissivity and visible-light scattering of highly reflective surfaces at cryogenic temperatures
A technique is described for the simultaneous in situ measurement of film thickness, refractive index, total normal emissivity, visible light scattering, and reflectance of contaminant films on a highly reflective liquid nitrogen-cooled, stainless steel substrate. Emissivities and scattering data were obtained for films of water, carbon dioxide, silicone oil, and a number of aromatic and aliphatic hydrocarbons as a function of film thickness between zero and 20 microns. Water had the greatest effect on emissivity, followed by silicone oil, aliphatic hydrocarbons, aromatic hydrocarbons, and carbon dioxide. Emissivity increased more rapidly with film thickness between zero and 2.5 microns, than at thickness greater than 2.5 microns. Scattering of visible light changed little below 2-microns thickness but increased rapidly with thickness beyond 2 to 3 microns. The effect of contaminant films on passive radiation coolers is discussed.
Viehmann, W.↗
Effects of surface contamination on the infrared emissivity and visible-light scattering of highly reflective surfaces at cryogenic temperatures
A technique is described for the simultaneous in situ measurement of film thickness, refractive index, total normal emissivity, visible-light scattering, and reflectance of contaminant films on a highly reflective liquid-nitrogen cooled, stainless steel substrate. Emissivities and scattering data are obtained for films of water, carbon dioxide, silicone oil, and a number of aromatic and aliphatic hydrocarbons as a function of film thickness between zero and 20 microns. Of the contaminants investigated, water has by far the greatest effect on emissivity, followed by silicone oil, aliphatic hydrocarbons, aromatic hydrocarbons, and carbon dioxide. The emissivity increases more rapidly with film thickness between zero and 2.5 microns than at thicknesses greater than 2.5 microns. Scattering of visible light changes very little below 2 microns thickness but increases rapidly with thickness beyond 2 to 3 microns. The effect of contaminant films on passive radiation coolers is discussed.
Viehmann, W.↗