Laser-photophoretic migration and fractionation of human blood cells

Laser photophoretic migration behavior of human blood cells in saline solution was investigated under the irradiation of Nd:YAG laser beam (532 nm) in the absence and the presence of the flow in a fused silica capillary. Red blood cells (RBC) were migrated faster than white blood cells (WBC) and blood pellets to the direction of propagation of laser light. The observed photophoretic velocity of RBC was about 11 times faster than those of others. This was understood from the larger photophoretic efficiency of RBC than that of WBC, which was simulated based on the Mie scattering theory. Furthermore, it was found that, during the photophoretic migration, RBCs spontaneously orientated parallel to the migration direction so as to reduce the drag force. Finally, it was demonstrated that RBC and WBC were separated in a micro-channel flow system by the laser photophoresis.     

Photophoretic assembly and migration of dielectric particles and Escherichia coli in liquids using a subwavelength diameter optical fiber

We demonstrate a photophoretic assembly and migration of dielectric (SiO(2) and TiO(2)) particles and bacteria (Escherichia coli) in liquids by using a subwavelength diameter fiber. With a lightwave at 1.55 μm launched into the fiber, the objects are radiated by the leaking light of the fiber to yield negative photophoretic forces which drive the objects to move toward the fiber, with an average assembling/migrating speed of 5-15 individuals per second (ind/s). The influences of laser-on duration, optical power, and size of particles on the photophoretic velocities are also investigated.     

Cavity ring-down spectroscopy measurements of single aerosol particle extinction. I. The effect of position of a particle within the laser beam on extinction

A continuous wave distributed feedback diode laser operating in the near infrared at wavelengths close to 1650 nm has been used to measure the extinction of light by single aerosol particles. The technique of optical feedback cavity ring-down spectroscopy (CRDS) was used for measurement of CRDS events at a repetition rate of 1.25 kHz. This very high repetition rate enabled multiple measurements of the extinction of light by single aerosol particles for the first time and demonstrated the dependence of light scattering on the position of a particle within the laser beam. A model is proposed to explain quantitatively this phenomenon. The minimum detectable dimensionless extinction coefficient epsilonmin was determined to be 3x10(-6). Extinction values obtained for single spherical polymer beads from a monodisperse sample of particles of diameter of 4 microm are in near-quantitative agreement with the values calculated by the Mie scattering theory. The deviations from the Mie theory expected for measurement of extinction by CRDS using a continuous wave laser are discussed in the companion paper.     

Photophoretic velocimetry--a new way for the in situ determination of particle size distribution and refractive index of hydrocolloids

The migration of particles induced by the forces of light is known as photophoresis. The photophoretic velocity of particles under the influence of a strong light source, e.g. a laser beam, is recorded and measured by means of digital image processing which is called photophoretic velocimetry (PPV). The photophoretic velocity depends on the particle size as well as on its refractive index. By applying PPV, we show the determination of the intrinsic properties of polystyrene (PS), melamine resin (MF) and SiO(2) particles, deduced from velocity distributions of both monodisperse as well as polydisperse suspensions. Especially the continuous determination of the refractive index of single hydrocolloids is of great interest for quality assurance and the discrimination of polydisperse biological or inorganic samples. Also, PPV is not restricted to in water dispersed samples only.     

Separation and detection of individual submicron particles by capillary electrophoresis with laser-light-scattering detection

Separation and detection of individual submicron polystyrene spheres using capillary electrophoresis with laser-light-scattering detection has been demonstrated. Electrophoretically separated particles were passed through a focused laser beam and light scattered from individual particles was collected at 90 degrees. Each diameter of polystyrene spheres injected (from 110 to 992 nm) resulted in the observation of a well-defined migration window containing multiple peaks, each arising from the light scattered by an individual particle. The migration time window for individual particles of a particular size corresponded well to the migration time of a peak from a population of particles of the same size detected using a UV absorbance detector. The electrophoretic mobility and scattered light intensity were determined for each particle detected. The average scattered light intensity for each particle size was consistent with Mie scattering theory. Particles as small as 110 nm in diameter were detected individually using this method, but particles with a diameter of 57 nm could not be individually detected. The number of single particle scattering events was counted and compared to the theoretical number of particles injected electrokinetically, and the detection efficiency determined ranged from 38 to 57% for polystyrene spheres of different sizes. The laser-light-scattering detection method was directly compared to laser-induced fluorescence detection using fluorescent polystyrene microspheres. The number of particles detected individually by each method was in agreement.     

Measurements of extinction by aerosol particles in the near-infrared using continuous wave cavity ring-down spectroscopy

Cavity ring-down spectroscopy using a fiber-coupled continuous wave distributed feedback laser at a wavelength of 1520 nm has been used to measure extinction of light by samples of nearly monodisperse aerosol particles <1 μm in diameter. A model is tested for the analysis of the sample extinction that is based on the Poisson statistics of the number of particles within the intracavity laser beam: variances of measured extinction are used to derive values of the scattering cross section for size-selected aerosol particles, without need for knowledge of the particle number density or sample length. Experimental parameters that influence the performance of the CRD system and the application and limitations of the statistical model are examined in detail. Determinations are reported of the scattering cross sections for polystyrene spheres (PSSs), sodium chloride, and ammonium sulfate, and, for particles greater than 500 nm in diameter, are shown to be in agreement with the corresponding values calculated using Mie theory or Discrete Dipole Approximation methods. For smaller particles, the experimentally derived values of the scattering cross section are larger than the theoretical predictions, and transmission of a small fraction of larger particles into the cavity is argued to be responsible for this discrepancy. The effects of cubic structure on the determination of optical extinction efficiencies of sodium chloride aerosol particles are examined. Values are reported for the real components of the refractive indices at 1520 nm of PSS, sodium chloride, and ammonium sulfate aerosol particles.     

Resonant effects in evanescent wave scattering of polydisperse colloids

Measurements and predictions are reported to understand large variations in evanescent wave (EW) scattering intensities between different particles from the same batch of single mode, polydisperse colloids. Measured EW scattering intensity distributions are obtained for three different micrometer sized latex particles irreversibly deposited onto glass surfaces. Predicted EW scattering intensity distributions are obtained using measured particle size distributions as input in a Mie theory for the three-dimensional scattering of a sphere under EW illumination. Good agreement is observed between measured and predicted EW scattering intensity distributions using no adjustable parameters. Our results indicate how finite polydispersity together with resonant effects produce large, nonlinear intensity variations between particles that appear to be physically and chemically uniform. Our findings allow such resonant effects to be understood and exploited in EW based particle-surface characterization techniques (e.g., using total internal reflections, surface plasmons) and chemical and biomolecular sensing applications (e.g., using whispering gallery modes).     

Capillary electrochromatography with macroporous particles.

The performance of macro-porous particles in capillary electrochromatography is studied. Three reversed-phase stationary phases with pore diameters between 500 A and 4000 A have been tested for separation efficiency and mobile phase velocity. With these stationary phases, a large portion of the total flow appears to be through the pores of particles, thereby increasing the separation efficiency through a further decrease of the flow inhomogeneity and through enhancement of the mass transfer kinetics. The effects of pore size and mobile phase composition on the plate height and mobile phase velocity have been studied. With increasing buffer concentrations and larger pore diameters, higher mobile phase velocities and higher separation efficiencies have been obtained. Columns packed with 7 microns particles containing pores with a diameter of 4000 A generated up to 430,000 theoretical plates/m for retained compounds. Reduced plate heights as low as 0.34 have been observed, clearly demonstrating that a significant portion of the flow is through the pores. For the particles containing 4000 A pores no minimum was observed in the H-u plot up to linear velocities of 3.3 mm/s, suggesting that the separation efficiency is dominated by axial diffusion. On relatively long (72 cm) columns, efficiencies of up to 230,000 theoretical plates/column have been obtained under non-optimal running conditions. On short (8.3 cm) columns fast separations could be performed with approximately 15,000 theoretical plates generated in less than 30 s.     

Bubble nucleation in polymeric liquids. I. Bubble nucleation in concentrated polymer solutions

Laser light scattering, with the aid of Mie's scattering theory, was used to investigate bubble nucleation in concentrated polymer solutions. Solutions with 40, 50 and 60 wt % polystyrene in toluene were used. A test solution in a high-pressure optical cell made of strain-free quartz was heated to a predetermined temperature under pressure. Upon release of the pressure in the cell, both scattered and transmitted light fluxes were measured with photomultipliers, and the variation of system pressure with time was measured using a piezoelectric pressure transducer. The measurement of the light scattering flux and control of the experiment were performed by means of a microcomputer with a general-purpose data acquisition interface. Data reduction was done using the same microcomputer. The critical bubble size was determined by obtaining a one-to-one correspondence between the extrema of the experimental and theoretical scattering curves. While the Mie scattering theory is for monodisperse particles, the experimental scattering curves indicated that the bubbles had a distribution of sizes. Therefore, the log-normal distribution function was used to represent the size distribution; and theoretical scattering curves were computed by varying the breadth parameter in the log-normal distribution function, until we had a one-to-one correspondence between the extrema of the experimental and theoretical scattering curves. In this way, we were able to determine (a) the size distribution of bubbles in the optical cell, (b) the critical bubble size, (c) the total number of bubbles nucleated, and (d) the critical pressure for bubble nucleation, as functions of temperature, the initial equilibrium pressure in the optical cell, and the concentration of the polymer solution.     

Angle‐dependent light scattering by highly uniform colloidal rod‐shaped microparticles: Experiment and simulation

While extensive theoretical work has been devoted to analyzing scattering behavior for nonspherical particles, few experimental studies of the light‐scattering properties of such particles are available, largely because of the difficulty of synthesizing such particles with uniform geometries. Here we report the synthesis of highly uniform, volume‐equivalent rod‐shaped colloidal particles prepared from their commercial spherical counterparts, on which we performed light scattering experiments as a function of scattering angle for micro rods with varying aspect ratio and volume. These results were compared to values calculated using the T‐Matrix method. Good agreement with theoretical predictions was found for the experimentally measured scattering cross sections and the angular dependence of the scattering intensity. An increase in the forward scattering intensity is observed and predicted for particles with larger aspect ratios relative to their volume equivalent spheres, with only minor differences observed at both mid‐range and backscattering angles. Furthermore, the light scattering results for the rod‐shaped particles did not show the scattering fringes seen in scattering by the spheres, indicating that as three‐dimensional symmetry is broken, the associated Lorenz–Mie resonances are strongly attenuated. This observation also was predicted by theory. © 2016 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2016 , 54, 1889–1895     

Small-angle polarized light scattering from amorphous spheres

Small-angle light-scattering measurements have been made using micron-diameter isotropic and spherical polymer latex particles placed between crossed polarizers. Four-leaf clover patterns are obtained, reminiscent of those commonly found for spherical birefringent scatterers. The experimental results compare closely with predictions of Mie scattering theory for isotropic spheres.     

Dendron-like growth of silver nanoparticles using a water-soluble oligopeptide

A dendron-like nanostructure of silver was grown in solution using a water-soluble tetrapeptide Tyr-Aib-Tyr-Val (Aib, alpha-amino isobutyric acid), silver nitrate, and methanol. These structures are composed of silver nanoparticles having a bimodal size distribution with the median diameters around 2.0 and 19.5 nm, respectively. The dendron-like growth is ascribed to the effect of the local electric field generated by the dipoles associated with the peptide molecules. The optical absorption spectra have been analyzed by Mie scattering theory, which shows that there is a metal-nonmetal transition in silver particles having diameters less than approximately 2.0 nm.     

Low-Knudsen-number photophoresis of aerosol spheroids

The photophoretic motion of a freely suspended aerosol spheroid exposed to a radiative heat flux that is oriented arbitrarily with respect to its axis of revolution is analytically studied. The Knudsen number is assumed to be so small that the fluid flow can be described by a continuum model with a thermal slip at the particle surface. In the limit of small Peclet and Reynolds numbers, the appropriate energy and momentum equations are solved using the bifocal-coordinate transformations. Expressions for the photophoretic velocity and force are obtained in closed form for various cases of prolate and oblate spheroidal particles. The average photophoretic velocity and force for an ensemble of identical, noninteracting spheroids with random orientation distribution are also determined. The results indicate that the aspect ratio and relative thermal conductivity of a spheroidal particle and its orientation with respect to the incident light can have significant effects on its photophoretic behavior.     

Binary clusters: homogeneous alloys and nucleus-shell structures

Extinction spectra of Ag_x-Au_(1?x)-alloy particles embedded in glass are compared to spectra of gold coated silver clusters and silver coated gold clusters. It is shown, that the optical extinction of alloy particles is described by the Mie theory applying the homogeneous dielectric function \(\hat \varepsilon \) (ω,R, x) measured by Paquet. The absorption of core-shell clusters was calculated deriving an extension of the Mie theory to spheres with arbitrary numbers of shells of arbitrary materials. Comparison to measured spectra points to s-electron motion in the clusters with only slight scattering at the interior interface. The appearance of two distinct Mie peaks however proves the existence of the sharp Ag-Au interface. The extended Mie formalism was also applied to a multilayer system consisting of sodium and a dielectric substance as an example for a spherical hetero structure.     

Estimation of morphological characteristics of single particles from light scattering data in flow cytometry

Numerical methods for solving the reverse problem of light scattering for single particles and a variety of experimental results have been reviewed. In particular, the two-dimensional Mie scattering method for the estimation of sizes and refractive indices of single particles has been developed. The method of triple two-dimensional Mie scattering has been elaborated, which extends the range of particle sizes with correct solutions of the reverse light scattering problem. The flying light scattering indicatrix method, which allows the estimation of the parameters of spherical particles, is presented. The results of the use of a flow cytometer of standard design for the anaysis of milk microflora and for an AIDS immunoassay by latex agglutination are given. The design of a scanning flow cytometer is considered. The results of measuring the light scattering from polystyrene latex particles are given.Translated fromIzvestiya Akademii Nauk. Seriya Khimicheskaya, No. 7, pp. 1181–1190, July, 1994.The author is grateful to A. K. Petrov and M. A. Kamkhe for supporting the work on cytometry, E. G. Saprykin for useful discussion and comments, G. Alm (Swedish Agricultural Univ.) for initiating the interest to immunological studies, and A. V. Chernyshev, T. S. Mashnin, V. I. Prots, and A. A. Doroshkin for cooperation.     

Calibration of Polarization-Sensitive and Dual-Angle Laser Light Scattering Methods Using Standard Latex Particles

A polarization-sensitive laser light scattering (PSLLS) method and a dual-angle laser light scattering (DALLS) method have been studied for in situ measurement of submicrometer hydrosol and aerosol particles. By using standard monodisperse polystyrene latex particles suspended in water and air as test particles, calibration of systems built based on the above methods have been performed. The effects of light scattered by agglomerated aerosol particles (multiplets) were corrected by considering the fraction of multiplets as determined with an aerosol measurement technique using a differential mobility analyzer. The change in the measured intensities of scattered light with particle diameter was then determined by calculations based on Mie theory. It was shown that the PSLLS system can determine particle diameters as small as approximately 60 nm for the test hydrosol particles and approximately 100 nm for test aerosol particles, respectively. The DALLS system can determine smaller diameters than the PSLLS system for test particles with no light absorption. The change in scattered light intensities with particle diameter was also investigated by theoretical calculations with various refractive indexes and scattering angles. The PSLLS and DALLS systems promise to become routine measurement tools for absorbing and nonabsorbing particles, respectively. Copyright 2001 Academic Press.     

Structural Interpretations of Static Light Scattering Patterns of Fractal Aggregates

A method based on static light scattering by fractal aggregates is introduced to extract structural information. In this study, we determine the scattered intensity by a fractal aggregate calculating the Structure and the Form factors noted, respectively, S(q) and F(q). We use the approximation of the mean field Mie scattering by fractal aggregates (R. Botet, P. Rannou, and M. Cabane, appl. opt. 36, 8791, 1997). This approximation is validated by a comparison of the scattering and extinction cross sections values calculated using, on the one hand, Mie theory with a mean optical index n) and, on the other hand, the mean field approximation. Scattering and extinction cross sections values differ by about 5%. We show that the mean environment of primary scatterers characterized by the optical index n(s) must be taken into account to interpret accurately the scattering pattern from fractal aggregates. Numerical simulations were done to evaluate the influence of the fractal dimension values (D(f)>2) and of the radius of gyration or the number of primary particles within the aggregates (N=50 to 250) on the scatterers' mean optical contrast (n(s)/n). This last parameter plays a major role in determining the Form factor F(q) which corresponds to the primary particles' scattering. In associating the mean optical index (n) to structural characteristics, this work provides a theoretical framework to be used to provide additional structural information from the scattering pattern of a fractal aggregate (cf. Part II). Copyright 2000 Academic Press.     

Evaluation of light scattering data from bimodal turbid suspensions: a simple fit procedure

Whereas correlation spectroscopy gives reliable information on the size of immersed particles in those cases where the size distribution is narrow, large problems arise for more complex particle distributions. For instance, samples containing distinctly different particles of rather similar size lead to correlation functions which are very close to those of monodisperse samples. We present a measurement technique which is based on angle dependent measurements of 3D cross correlation functions and an evaluation scheme which uses the results of the Mie theory. The experimental technique warrants applications to strongly scattering samples. Having tested this procedure with mixtures containing standard latex particles we applied it to a sample of skimmed, homogenized milk.     

Particle-bubble collision models--a review

A critical review of the various models existing in the literature for the calculation of the collision efficiency between particles and single, rising gas bubbles is presented. Although all of these collision models predict that the collision efficiency increases with particle size, their dependence on the latter is different because of the various assumptions and hydrodynamic conditions used in each model. Collision efficiencies of quartz particles with single bubbles have been obtained from experimental flotation experiments under conditions where the attachment and stability efficiencies were at, or near, unity. These collision efficiencies were then used to test various collision models. Good agreement between the experimental and calculated collision efficiencies was only obtained with the Generalised Sutherland Equation. The differences in collision efficiencies obtained between the various models were mainly explained in terms of, firstly, the degree of mobility of the bubble surface and, secondly, a consideration of the inertial forces acting on the particles.     

Effects of the menstrual cycle on the red and near-infrared optical properties of the human breast

Time-resolved reflectance and transmittance spectroscopy was applied to measure in vivo the absorption and transport scattering spectra of the female breast from 610 to 1010 nm. Three measurement configurations were used to probe different breast regions, and data were collected two or three times in each of the five phases of the menstrual cycle. The absorption spectra were best-fitted with a linear combination of the spectra of the main tissue constituents (water, lipids, oxy- and deoxyhemoglobin). This allowed us to evaluate percentage contents of water and lipids, total hemoglobin content and hemoglobin oxygen saturation. The scattering spectra were interpreted with a function derived from Mie theory, providing information on the density and average size of the tissue scatterers. Significant changes in the estimated variables were observed with measurement geometry, reflecting the heterogeneous nature of the breast, and with time, in agreement with expected physiological changes over the menstrual cycle.