(2017). Calibration of a multi-pass photoacoustic spectrometer cell using light-absorbing aerosols. Atmospheric Measurement Techniques. 10:(3)1203-1213. Abstract
The multi-pass photoacoustic spectrometer (PAS) is an important tool for the direct measurement of light absorption by atmospheric aerosol. Accurate PAS measurements heavily rely on accurate calibration of their signal. Ozone is often used for calibrating PAS instruments by relating the photoacoustic signal to the absorption coefficient measured by an independent method such as cavity ring down spectroscopy (CRD-S), cavity-enhanced spectroscopy (CES) or an ozone monitor. We report here a calibration method that uses measured absorption coefficients of aerosolized, light-absorbing organic materials and offer an alternative approach to calibrate photoacoustic aerosol spectrometers at 404 nm. To implement this method, we first determined the complex refractive index of nigrosin, an organic dye, using spectroscopic ellipsometry and then used this well-characterized material as a standard material for PAS calibration.
(2015). Wettability Stabilizes Fluid Invasion into Porous Media via Nonlocal, Cooperative Pore Filling. Physical Review Letters. 115:(16) Abstract
We study the impact of the wetting properties on the immiscible displacement of a viscous fluid in disordered porous media. We present a novel pore-scale model that captures wettability and dynamic effects, including the spatiotemporal nonlocality associated with interface readjustments. Our simulations show that increasing the wettability of the invading fluid (the contact angle) promotes cooperative pore filling that stabilizes the invasion and that this effect is suppressed as the flow rate increases, due to viscous instabilities. We use scaling analysis to derive two dimensionless numbers that predict the mode of displacement. By elucidating the underlying mechanisms, we explain classical yet intriguing experimental observations. These insights could be used to improve technologies such as hydraulic fracturing, CO2 geosequestration, and microfluidics.
(2015). Ant trophallactic networks: simultaneous measurement of interaction patterns and food dissemination. Scientific Reports. 5. Abstract
Eusocial societies and ants, in particular, maintain tight nutritional regulation at both individual and collective levels. The mechanisms that underlie this control are far from trivial since, in these distributed systems, information about the global supply and demand is not available to any single individual. Here we present a novel technique for non-intervening frequent measurement of the food load of all individuals in an ant colony, including during trophallactic events in which food is transferred by mouth-to-mouth feeding. Ants are imaged using a dual camera setup that produces both barcode-based identification and fluorescence measurement of labeled food. This system provides detailed measurements that enable one to quantitatively study the adaptive food distribution network. To demonstrate the capabilities of our method, we present sample observations that were unattainable using previous techniques, and could provide insight into the mechanisms underlying food exchange.
(2015). Volatility of Atmospherically Relevant Alkylaminium Carboxylate Salts. Journal of Physical Chemistry A. 119:(19)4336-4346. Abstract
Heterogeneous neutralization reactions of ammonia and alkylamines with sulfuric acid play an important role in aerosol formation and particle growth. However, little is known about the physical and chemical properties of alkylaminium salts of organic acids. In this work we studied the thermal stability and volatility of alkylaminium carboxylate salts of short aliphatic alkylamines with monocarboxylic and dicarboxylic acids. The enthalpy of vaporization and saturation vapor pressure at 298 K were derived using the kinetic model of evaporation and the Clausius-Clapeyron relation. The vapor pressure of alkylaminium dicarboxylate salts is similar to 10(-6) Pa, and the vaporization enthalpy ranges from 73 to 134 kJ mol(-1). Alkylaminium monocarboxylate salts show high thermal stability, and their thermograms do not follow our evaporation model. Hence, we inferred their vapor pressure from their thermograms as comparable to that of ammonium sulfate (similar to 10(-9) Pa). Further characterization showed that alkylaminium monocarboxylates are room temperature protic ionic liquids (RTPILs) that are more hygroscopic than ammonium sulfate (AS). We suggest that the irregular thermograms result from an incomplete neutralization reaction leading to a mixture of ionic and nonionic compounds. We conclude that these salts are expected to contribute to new particle formation and particle growth under ambient conditions and can significantly enhance the CCN activity of mixed particles in areas where SO2 emissions are regulated
(2014). The possible association between exposure to air pollution and the risk for congenital malformations. Environmental Research. 135:173-180. Abstract
Background: Over the last decade, there is growing evidence that exposure to air pollution may be associated with increased risk for congenital malformations. Objectives: To evaluate the possible association between exposures to air pollution during pregnancy and congenital malformations among infants born following spontaneously conceived (SC) pregnancies and assisted reproductive technology (ART) pregnancies. Methods: This is an historical cohort study comprising 216,730 infants: 207,825 SC infants and 8905 ART conceived infants, during the periods 1997-2004. Air pollution data including sulfur dioxide (SO2), particulate matter
(2013). Thermochemical, Cloud Condensation Nucleation Ability, and Optical Properties of Alkyl Aminium Sulfate Aerosols. Journal of Physical Chemistry C. 117:(43)22412-22421. Abstract
Alkyl aminium sulfates have been postulated to constitute important components of nucleation and accumulation mode atmospheric aerosols. In this study we present laboratory data on the thermochemical, cloud condensation nuclei (CCN) activity, and optical properties of selected aminium sulfate compounds of atmospheric relevance (monomethyl aminium sulfate (MMAS), dimethyaminium sulfate (DMAS), trimethylaminium sulfate, monoethylaminium sulfate (MEAS), diethylaminium sulfate (DEAS), and triethylaminium sulfate (TEAS)). We found that the vapor pressure of these aminium salts is 1-3 orders of magnitude lower than that of ammonium sulfate and as such they can contribute to new aerosols and secondary aerosols formation. We infer that these species have very high CCN activity, with hygroscopicity parameter that is similar to that ammonium sulfate. Finally, between 360 and 420 nm, these aminium sulfate salts scatter light less efficiently than ammonium sulfate, and do not absorb light. These derived parameters can contribute to the better understanding and characterization of the role that these compounds play in atmospheric chemical reactions, gas-solid partitioning and their possible contribution to the microphysical and radiative effects of atmospheric aerosols.
(2013). Fluxes of Fine Particles Over a Semi-Arid Pine Forest: Possible Effects of a Complex Terrain. Aerosol Science and Technology. 47:(8)906-915. Abstract
Semi-arid forests are of growing importance due to expected ecosystem transformations following climatic changes. Dry deposition of atmospheric aerosols was measured for the first time in such an ecosystem, the Yatir forest in southern Israel. Size-segregated flux measurements for particles ranging between 0.25m and 0.65m were taken with an optical particle counter (OPC) using eddy covariance methodology. The averaged deposition velocity (V-d ) at this site was 3.8 +/- 4.5mm s(-1) for 0.25-0.28m particles, which is in agreement with deposition velocities measured in mid and northern latitude coniferous forests, and is most heavily influenced by the atmospheric stability and turbulence conditions, and to a lesser degree by the particle size. Both downward and upward fluxes were observed. Upward fluxes were not associated with a local particle source. The flux direction correlated strongly with wind direction, suggesting topographical effects. We hypothesize that a complex terrain and a patchy fetch affected the expected dependence of V-d on particle size and caused the observed upward fluxes of particles. The effect of topography on the deposition velocity grows greater as particle size increases, as has been shown in modeling and laboratory studies but had not been demonstrated yet in field studies. This hypothesis is consistent with the observed relationship between V-d and the friction velocity, the topography in the area of the flux tower, and the observed correlation of flux direction with wind direction. [Supplementary materials are available for this article. Go to the publisher's online edition of Aerosol Science and Technology to view the free supplementary files.] Copyright 2013 American Association for Aerosol Research
(2011). Dynamics of vesicles in shear and rotational flows: Modal dynamics and phase diagram. Physics of Fluids. 23:(4) Abstract
Despite the recent upsurge of theoretical reduced models for vesicle shape dynamics, comparisons with experiments have not been accomplished. We review the implications of some of the recently proposed models for vesicle dynamics, especially the tumbling-trembling domain regions of the phase plane, and show that they all fail to capture the essential behavior of real vesicles for excess areas Delta greater than 0.4. We emphasize new observations of shape harmonics and the role of thermal fluctuations. (C) 2011 American Institute of Physics. [doi:10.1063/1.3556439]
(2010). Strong symmetrical non-Oberbeck-Boussinesq turbulent convection and the role of compressibility. Physics of Fluids. 22:(3)035108. Abstract
Strong non-Oberbeck-Boussinesq (OB) effects in turbulent convection were investigated experimentally in SF6 in the vicinity of its gas-liquid critical point (CP). The temperature and density dependencies of the thermodynamic and kinetic properties of SF6 near its CP and at the average critical density lead to strong but symmetric vertical variations of the main physical properties, which enter into the control parameters of turbulent convection. This produces an up-down symmetry in the temperature drops across the upper and lower half of the cell, while the temperature in the middle of the cell remains equal to the average value. Thus, in spite of the strong variations of the fluid properties across the cell height, the up-down symmetry remains like in the OB case. The distinctive feature of the symmetric non-OB turbulent convection is that the heat transport scales with the Rayleigh number Ra like in the OB turbulent convection. At the same time, it shows a much stronger dependence on the Prandtl number Pr. We singled out the influence of the non-OB effect on the heat transport and found that, for the same Pr, an eightfold larger non-OB effect does not alter either the value of the Nusselt number, Nu, nor its scaling with respect to the Rayleigh number, Nu(proportional to)Ra(gamma). The conclusion is that the strong symmetric non-OB effect by itself is not responsible for the strong Pr dependence of the heat transport near CP. The possible source of this Pr dependence is the strongly enhanced isothermal compressibility in the vicinity of CP, which can affect the dynamics of plumes and so the heat transport close to the CP, and manifests itself in a dependence of Nu on Pr much steeper than in the OB case. (C) 2010 American Institute of Physics. [doi: 10.1063/1.3358462]
(2010). Interaction of internally mixed aerosols with light. Physical Chemistry Chemical Physics. 12:(1)21-31. Abstract
Atmospheric aerosols scatter and absorb solar radiation leading to variable effects on Earth's radiative balance. Aerosols individually comprising mixtures of different components ("internally mixed") interact differently with light than mixtures of aerosols, each comprising a different single component ("externally mixed"), even if the relative fractions of the different components are equal. In climate models, the optical properties of internally mixed aerosols are generally calculated by using electromagnetic "mixing rules", which average the refractive indices of the individual components in different proportions, or by using coated-sphere Mie scattering codes, which solve the full light scattering problem assuming that the components are divided into two distinct layers. Because these calculation approaches are in common use, it is important to validate them experimentally. In this article, we present a broad perspective on the optical properties of internally mixed aerosols based on a series of laboratory experiments and theoretical calculations. The optical properties of homogenously mixed aerosols comprised of non-absorbing and weakly absorbing compounds, and of coated aerosols comprised of strongly absorbing, non-absorbing, and weakly absorbing compounds in different combinations are measured using pulsed and continuous wave cavity ring down aerosol spectrometry (CRD-AS). The success of electromagnetic mixing rules and Mie scattering codes in reproducing the measured aerosol extinction values is discussed.
(2009). Dynamics of a vesicle in general flow. Proceedings of the National Academy of Sciences of the United States of America. 106:(28)11444-11447. Abstract
An approach to quantitatively study vesicle dynamics as well as biologically-related micro-objects in a fluid flow, which is based on the combination of a dynamical trap and a control parameter, the ratio of the vorticity to the strain rate, is suggested. The flow is continuously varied between rotational, shearing, and elongational in a microfluidic 4-roll mill device, the dynamical trap, that allows scanning of the entire phase diagram of motions, i.e., tank-treading (TT), tumbling (TU), and trembling (TR), using a single vesicle even at lambda = eta(in)/eta(out) = 1, where eta(in) and eta(out) are the viscosities of the inner and outer fluids. This cannot be achieved in pure shear flow, where the transition between TT and either TU or TR is attained only at lambda > 1. As a result, it is found that the vesicle dynamical states in a general are presented by the phase diagram in a space of only 2 dimensionless control parameters. The findings are in semiquantitative accord with the recent theory made for a quasi-spherical vesicle, although vesicles with large deviations from spherical shape were studied experimentally. The physics of TR is also uncovered.
(2009). Complex Refractive Indices of Aerosols Retrieved by Continuous Wave-Cavity Ring Down Aerosol Spectrometer. Analytical Chemistry. 81:(5)1762-1769. Abstract
The major uncertainties associated with the direct impact of aerosols on climate call for fast and accurate characterization of their optical properties. Cavity ring down (CRD) spectroscopy provides highly sensitive measurement of aerosols' extinction coefficients from which the complex refractive index (RI) of the aerosol may be retrieved accurately for spherical particles of known size and number density, thus it is possible to calculate the single scattering albedo and other atmospherically relevant optical parameters. We present a CRD system employing continuous wave (CW) single mode laser. The single mode laser and the high repetition rate obtained significantly improve the sensitivity and reliability of the system, compared to a pulsed laser CRD setup. The detection limit of the CW-CRD system is between 6.67 x 10(-10) cm(-1) for an empty cavity and 3.63 x 10(-9) cm(-1) for 1000 particles per cm(3) inside the cavity, at a 400 Hz sampling and averaging of 2000 shots for one sample measurement taken in 5 s. For typical pulsed-CRD, the detection limit for an empty cavity is less than 3.8 x 10(-1) cm(-1) for 1000 shots averaged over 100 s at 10 Hz. The system was tested for stability, accuracy, and RI retrievals for scattering and absorbing laboratory-generated aerosols. Specifically, the retrieved extinction remains very stable for long measurement times (1 h) with an order of magnitude change in aerosol number concentration. In addition, the optical cross section (sigma(ext)) of a 400 nm polystyrene latex sphere (PSL) was determined within 2% error compared to the calculated value based on Mie theory. The complex RI of PSL, nigrosin, and ammonium sulfate (AS) aerosols were determined by measuring the extinction efficiency (Q(ext)) as a function of the size parameter ((pi D)/lambda) and found to be in very good agreement with literature values. A mismatch in the retrieved RI of Suwannee River fulvic acid (SRFA) compared to a previous study was observed and is a
(2008). Photoluminescence Ring Formation in Coupled Quantum Wells: Excitonic Versus Ambipolar Diffusion. Physical Review Letters. 101:(25) Abstract
In this Letter, we study the diffusion properties of photoexcited carriers in coupled quantum wells around the Mott transition. We find that the diffusion of unbound electrons and holes is ambipolar and is characterized by a large diffusion coefficient, similar to that found in p-i-n junctions. Correlation effects in the excitonic phase are found to significantly suppress the carriers' diffusion. We show that this difference in diffusion properties gives rise to the appearance of a photoluminescence ring pattern around the excitation spot at the Mott transition.
(2008). Bioluminescent response of individual dinoflagellate cells to hydrodynamic stress measured with millisecond resolution in a microfluidic device. Journal of Experimental Biology. 211:(17)2865-2875. Abstract
Dinoflagellate bioluminescence serves as a model system for examining mechanosensing by suspended motile unicellular organisms. The response latency, i.e. the delay time between the mechanical stimulus and luminescent response, provides information about the mechanotransduction and signaling process, and must be accurately known for dinoflagellate bioluminescence to be used as a flow visualization tool. This study used a novel microfluidic device to measure the response latency of a large number of individual dinoflagellates with a resolution of a few milliseconds. Suspended cells of several dinoflagellate species approximately 35 mu m in diameter were directed through a 200 mu m deep channel to a barrier with a 15 mu m clearance impassable to the cells. Bioluminescence was stimulated when cells encountered the barrier and experienced an abrupt increase in hydrodynamic drag, and was imaged using high numerical aperture optics and a high-speed low-light video system. The average response latency for Lingulodinium polyedrum strain HJ was 15ms (N>300 cells) at the three highest flow rates tested, with a minimum latency of 12 ms. Cells produced multiple flashes with an interval as short as 5 ms between individual flashes, suggesting that repeat stimulation involved a subset of the entire intracellular signaling pathway. The mean response latency for the dinoflagellates Pyrodinium bahamense, Alexandrium monilatum and older and newer isolates of L. polyedrum ranged from 15 to 22 ms, similar to the latencies previously determined for larger dinoflagellates with different morphologies, possibly reflecting optimization of dinoflagellate bioluminescence as a rapid anti-predation behavior.
(2008). Critical dynamics of vesicle stretching transition in elongational flow. Physical Review Letters. 101:(4) Abstract
We present results on the stretching of single tubular vesicles in an elongation flow toward dumbbell shapes, and on their relaxation. A critical strain rate (is an element of)over dot(c) exists; for strain rates (is an element of)over dot <is an element of(c), the vesicle remains tubular but fluctuates, though its steady state extension increases with the strain rate (is an element of)over dot. Above (is an element of)over dot(c), first a shape transition to dumbbell occurs, and then high order shape modes become unstable, leading to a pearling state. We have quantitatively characterized the transition and found a scaling of (is an element of)over dot(c) with the system parameters. A remarkable feature of vesicle tube behavior around the critical point is a slowdown of the vesicle relaxation to the final extended state in the vesicle stretching. Such feature is similar to that found in continuous phase transitions and to the critical effects recently observed for polymer molecules near the coil-stretch transition in elongation flow.
(2008). Dynamics of interacting vesicles and rheology of vesicle suspension in shear flow. Epl. 82:(5) Abstract
We studied the dynamics of isolated vesicles as well as vesicle interactions in semidilute vesicle suspensions subjected to a shear flow. We found that the long-range hydrodynamic interactions between vesicles give rise to strong fluctuations of vesicle shape and inclination angle, empty set, though the functional dependence of empty set and the transition path to tumbling motion is preserved. The dependence of the suspension viscosity on the viscosity ratio between inner and outer fluids, lambda, was found to be non-monotonic and surprisingly growing with lambda at the fixed outer fluid viscosity for lambda <1, at odds with recent predictions made for a dilute suspension of non-interacting vesicles. Copyright (c) EPLA, 2008.
(2008). Extinction efficiencies of coated absorbing aerosols measured by cavity ring down aerosol spectrometry. Atmospheric Chemistry and Physics. 8:(6)1823-1833. Abstract
In this study, we measure the extinction efficiency at 532 nm of absorbing aerosol particles coated with a non-absorbing solid and liquid organic shell with coating thickness varying between 5 and 100 nm using cavity ring down aerosol spectrometry. For this purpose, we use nigrosin, an organic black dye, as a model absorbing core and two non-absorbing organic substances as shells, glutaric acid (GA) and Di-Ethyl-Hexyl-Sebacate (DEHS). The measured behavior of the coated particles is consistent with Mie calculations of core-shell particles. Errors between measured and calculated values for nigrosin coated with GA and DEHS are between 0.5% and 10.5% and between 0.5% and 9%, respectively. However, it is evident that the calculations are in better agreement with the measured results for thinner coatings. Possible reasons for these discrepancies are discussed.
(2007). Vesicle dynamics in time-dependent elongation flow: Wrinkling instability. Physical Review Letters. 99:(17) Abstract
We present experimental results on the relaxation dynamics of vesicles subjected to a time-dependent elongation flow. We observed and characterized a new instability, which results in the formation of higher-order modes of the vesicle shape (wrinkles), after a switch in the direction of the velocity gradient. This surprising generation of membrane wrinkles can be explained by the appearance of a negative surface tension during the vesicle deflation, which tunes itself to alternating stress. Moreover, the formation of buds in the vesicle membrane was observed in the vicinity of the dynamical transition point.
(2007). Elastic turbulence in von Karman swirling flow between two disks. Physics of Fluids. 19:(5)053104. Abstract
We discuss the role of elastic stress in the statistical properties of elastic turbulence, realized by the flow of a polymer solution between two disks. The dynamics of the elastic stress are analogous to those of a small-scale fast dynamo in magnetohydrodynamics, and to those of the turbulent advection of a passive scalar in the Batchelor regime. Both systems are theoretically studied in the literature, and this analogy is exploited to explain the statistical properties, the flow structure, and the scaling observed experimentally. The following features of elastic turbulence are confirmed experimentally and presented in this paper: (i) The rms of the vorticity (and that of velocity gradients) saturates in the bulk of the elastic turbulent flow, leading to the saturation of the elastic stress. (ii) The rms of the velocity gradients (and thus the elastic stress) grows linearly with Wi in the boundary layer, near the driving disk. The rms of the velocity gradients in the boundary layer is one to two orders of magnitude larger than in the bulk. (iii) The PDFs of the injected power at either constant angular speed or torque show skewness and exponential tails, which both indicate intermittent statistical behavior. Also the PDFs of the normalized accelerations, which can be related to the statistics of velocity gradients via the Taylor hypothesis, exhibit well-pronounced exponential tails. (iv) A new length scale, i.e., the thickness of the boundary layer, as measured from the profile of the rms of the velocity gradient, is found to be relevant for the boundary layer of the elastic stresses. The velocity boundary layer just reflects some of the features of the boundary layer of the elastic stresses (rms of the velocity gradients). This measured length scale is much smaller than the vessel size. (v) The scaling of the structure functions of the vorticity, velocity gradients, and injected power is found to be the same as that of a passive scalar advected by an elastic t
(2006). Role of elastic stress in statistical and scaling properties of elastic turbulence. Physical Review Letters. 96:(21)214502. Abstract
The role of elastic stress in statistical and scaling properties of elastic turbulence in a polymer solution flow between two disks is discussed. The analogy with a small-scale magnetodynamics and a passive scalar turbulent advection in the Batchelor regime is used to explain the experimentally observed statistical properties, the flow structure, and the scaling of elastic turbulence. The emergence of a new length scale, namely, the boundary layer thickness, is observed and studied.
(2005). Validity of the Taylor hypothesis in a random spatially smooth flow. Physics of Fluids. 17:(10)103101. Abstract
The validity of the Taylor frozen flow hypothesis in a chaotic flow of a dilute polymer solution in a regime of elastic turbulence is investigated experimentally. By accurate time-dependent measurements of the flow field we study the velocity coherence between pairs of points displaced both in time and space and quantify the degree of applicability of the Taylor hypothesis. Alternatively, the frozen flow assumption is assessed by comparison of the measured velocity structure functions with the ones derived by a frozen flow assumption. The breakdown of the Taylor hypothesis is further discussed in both the context of strong velocity fluctuations and long-range spatial correlations, which are the result of the flow smoothness and lack of scale separation. Different choices of the advection velocity are tested and discussed. (c) 2005 American Institute of Physics.
(2004). Statistics of particle pair separations in the elastic turbulent flow of a dilute polymer solution. Europhysics Letters. 68:(4)529-535. Abstract
We investigate experimentally the statistics of a chaotic flow of a dilute polymer solution in a regime of elastic turbulence by using the Lagrangian coordinates approach. We show that due to flow smoothness at small scales the Finite Time Lyapunov Exponent (FTLE) technique can be successfully used to investigate the statistics of particle pair separations at different scales. We compare the measured FTLE with the characteristics of statistical description in the Eulerian coordinate presentation, namely the velocity correlation times and the average velocity gradients. We characterize the flow intermittency by measuring high-order moments of the statistics of the particle pair separations.
(2004). Chaotic flow and efficient mixing in a microchannel with a polymer solution. Physical Review E. 69:(6)066305. Abstract
Microscopic flows are almost universally linear, laminar, and stationary because the Reynolds number, Re, is usually very small. That impedes mixing in microfluidic devices, which sometimes limits their performance. Here, we show that truly chaotic flow can be generated in a smooth microchannel of a uniform width at arbitrarily low Re, if a small amount of flexible polymers is added to the working liquid. The chaotic flow regime is characterized by randomly fluctuating three-dimensional velocity field and significant growth of the flow resistance. Although the size of the polymer molecules extended in the flow may become comparable to the microchannel width, the flow behavior is fully compatible with that in a macroscopic channel in the regime of elastic turbulence. The chaotic flow leads to quite efficient mixing, which is almost diffusion independent. For macromolecules, mixing time in this microscopic flow can be three to four orders of magnitude shorter than due to molecular diffusion.
(2004). Mixing by polymers: Experimental test of decay regime of mixing. Physical Review Letters. 92:(16)164501. Abstract
By using high molecular weight fluorescent passive tracers with different diffusion coefficients and by changing the fluid velocity we study the dependence of a characteristic mixing length on the Peclet number, Pe, which controls the mixing efficiency. The mixing length is found to be related to Pe by a power law, L(mix)proportional toPe(0.26+/-0.01), and increases faster than expected for an unbounded chaotic flow. The role of the boundaries in the mixing length abnormal growth is clarified. The experimental findings are in good quantitative agreement with recent theoretical predictions.