Distinct Particle Research Articles

Laboratory Studies of the Cloud Droplet Activation Properties and Corresponding Chemistry of Saline Playa Dust.

Playas emit large quantities of dust that can facilitate the activation of cloud droplets. Despite the potential importance of playa dusts for cloud formation, most climate models assume that all dust is nonhygroscopic; however, measurements are needed to clarify the role of dusts in aerosol-cloud interactions. Here, we report measurements of CCN activation from playa dusts and parameterize these results in terms of both κ-Köhler theory and adsorption activation theory for inclusion in atmospheric models. κ ranged from 0.002 ± 0.001 to 0.818 ± 0.094, whereas Frankel-Halsey-Hill (FHH) adsorption parameters of AFHH = 2.20 ± 0.60 and BFHH = 1.24 ± 0.14 described the water uptake properties of the dusts. Measurements made using aerosol time-of-flight mass spectrometry (ATOFMS) revealed the presence of halite, sodium sulfates, and sodium carbonates that were strongly correlated with κ underscoring the role that mineralogy, including salts, plays in water uptake by dust. Predictions of κ made using bulk chemical techniques generally showed good agreement with measured values. However, several samples were poorly predicted suggesting that chemical heterogeneities as a function of size or chemically distinct particle surfaces can determine the hygroscopicity of playa dusts. Our results further demonstrate the importance of dust in aerosol-cloud interactions.

Deterministic droplet-based co-encapsulation and pairing of microparticles via active sorting and downstream merging.

Co-encapsulation of two distinct particles within microfluidic droplets provides the means to achieve various high-throughput single-cell assays, such as biochemical reactions and cell-cell interactions in small isolated volumes. However, limited by the Poisson statistics, the co-encapsulation rate of the conventional co-flow approach is low even under optimal conditions. Only up to 13.5% of droplets precisely contain a pair of two distinct particles, while the rest, either being empty or encapsulating unpaired particles become wastes. Thus, the low co-encapsulation efficiency makes droplet-based assays impractical in biological applications involving low abundant bioparticles. In this paper, we present a highly promising droplet merging strategy to increase the co-encapsulation efficiency. Our method first enriches droplets exactly encapsulating a single particle via fluorescence or scattering-light activated sorting. Then, two droplets, each with a distinct particle, are precisely one-to-one paired and merged in a novel microwell device. This deterministic approach overcomes the Poisson statistics limitation facing conventional stochastic methods, yielding an up to 90% post-sorting particle capture rate and an overall 88.1% co-encapsulation rate. With its superior single-particle pairing performance, our system provides a promising technological platform to enable highly efficient microdroplet assays.

Design of Tumor Acidity-Responsive Sheddable Nanoparticles for Fluorescence/Magnetic Resonance Imaging-Guided Photodynamic Therapy.

Imaging-guided cancer therapy, which integrates diagnostic and therapeutic functionalities into a single system, holds great promise to enhance the accuracy of diagnosis and improve the efficacy of therapy. Specifically, for photodynamic therapy (PDT), it is highly desirable to precisely focus laser light onto the tumor areas to generate reactive oxygen species (ROS) that are cytotoxic tumor cells and avoid light-associated side effects. Herein, a distinct three-layer nanostructured particle with tumor acidity-responsiveness (S-NP) that encapsulates the photosensitizer chlorin e6 (Ce6) and chelates Gd3+ is successfully developed for fluorescence/magnetic resonance (MR) dual-model imaging-guided precision PDT. We show clear evidence that the outer PEG layer significantly prolongs circulation time, and the inner poly(ε-caprolactone) (PCL) core can physically encapsulate Ce6. More interestingly, the middle layer of the S-NP, acting as a molecular fence to keep Ce6 in the circulation system, was dismantled by the slightly acidic tumor microenvironment. Afterwards, the PEG shell is deshielded from the S-NP at the tumor tissue, resulting in improved cell uptake, enlarged MR signal intensity, rapid release of Ce6 within tumor cells, and elevated PDT efficacy. Our results suggest that tumor-acidity-responsive nanoparticles with fine design could serve as a theranostic platform with great potential in imaging-guided PDT treatment of cancer.

Contamination of exosome preparations, isolated from biological fluids

The aim of our study was to attract the attention of researchers at the problem of contamination of exosome preparations. Using a transmission electron microscope JEM-1400 (“JEOL”, Japan) we have examined exosome preparations, isolated according to the conventional scheme of sequential centrifugation from different biological fluids: plasma and urine of healthy persons and patients with oncologic diseases, bovine serum, and culture fluid (MDCK, MDA-MB и MCF-7 cells). All exosome preparations (over 200) contained exosomes, which were identified by immuno-electron microscopy using antibodies to tetraspanins CD63 or CD9. Besides exosomes, all the studied preparations contained contaminating structures: distinct particles of low electron density without limiting membrane (“non-vesicles”). Two main kinds of the “non-vesicles” species were found in exosome preparations: 20-40 nm in size, representing 10-40% of all structures in the preparations; and 40-100 nm in size (identical to exosomes by size). Morphology of the “non-vesicles” allowed to identify them as lipoproteins of intermediate and low density (20-40 nm), and very low density (40-100 nm). The highest level of the contamination was detected in exosome preparations, isolated from blood samples. The results of our study indicate the need to control the composition of exosome preparation by electron microscopy and take into account the presence of contaminating structures in analysis of experimental data.

Addressing the characterisation challenge to understand catalysis in MOFs: the case of nanoscale Cu supported in NU-1000.

We explore the dynamic structure and reactivity of Cu species supported on NU-1000. By combining pair distribution function (PDF) analysis and difference envelope density (DED) analysis of in situ synchrotron-based X-ray scattering data, we simultaneously probe the local structure of supported Cu-species, their distribution within NU-1000 and distortions of the NU-1000 lattice under conditions relevant to catalysis and catalyst activation. These analyses show that atomic layer deposition (ALD) of Cu in NU-1000 (Cu-AIM) leads to the formation of Cu-oxo clusters within the small pores that connect the triangular and hexagonal channels. Exposure of Cu-AIM to a reducing atmosphere at 200 °C produces metallic Cu0 of two distinct particle sizes: ∼4 nm nanoparticles and small sub-nanometer clusters. The size of these nanoparticles appears to be constrained by NU-1000 pore dimensions, with evidence of the sub-nanometer clusters being bound within the triangular channels flanked by pyrene rings. This supported Cu0-NU-1000 system is catalytically active for gas-phase ethylene hydrogenation. Exposure of the catalyst to oxidative atmosphere re-oxidises the Cu species to a Cu2O cuprite phase. The dynamic restructuring of the system in different chemical environments underscores the importance of probing these systems in situ.

WavePacket: A Matlab package for numerical quantum dynamics. I: Closed quantum systems and discrete variable representations

WavePacket is an open-source program package for the numerical simulation of quantum-mechanical dynamics. It can be used to solve time-independent or time-dependent linear Schrödinger and Liouville–von Neumann-equations in one or more dimensions. Also coupled equations can be treated, which allows to simulate molecular quantum dynamics beyond the Born–Oppenheimer approximation. Optionally accounting for the interaction with external electric fields within the semiclassical dipole approximation, WavePacket can be used to simulate experiments involving tailored light pulses in photo-induced physics or chemistry. The graphical capabilities allow visualization of quantum dynamics ‘on the fly’, including Wigner phase space representations. Being easy to use and highly versatile, WavePacket is well suited for the teaching of quantum mechanics as well as for research projects in atomic, molecular and optical physics or in physical or theoretical chemistry. The present Part I deals with the description of closed quantum systems in terms of Schrödinger equations. The emphasis is on discrete variable representations for spatial discretization as well as various techniques for temporal discretization. The upcoming Part II will focus on open quantum systems and dimension reduction; it also describes the codes for optimal control of quantum dynamics. The present work introduces the MATLAB version of WavePacket 5.2.1 which is hosted at the Sourceforge platform, where extensive Wiki-documentation as well as worked-out demonstration examples can be found. Program summaryProgram Title: WavePacketProgram Files doi:http://dx.doi.org/10.17632/tc5mrhx9sb.1Licensing provisions: GPLv3Programming language:MatlabNature of problem:Schrödingerś equations are of fundamental importance in non-relativistic quantum mechanics of distinguishable particles. The solutions of the time-independent equation (TISE) are wavefunctions in coordinate space, the absolute squares of which are usually interpreted as probability density. The time-dependent equation (TDSE) describes the dynamics of a quantum system evolving in time. It plays a crucial role for the simulation, understanding, and prediction of modern experiments in atomic, molecular and optical physics where systems are driven by temporally shaped external fields.Solution method:All numerical methods compiled in WavePacket are based on discrete variable representations. Currently implemented are Gauss–Hermite, Gauss–Legendre and FFT-based schemes. The TISE is solved either by direct diagonalization or by propagation in imaginary time. For the TDSE there is a choice between second order differencing, operator splitting and Chebychev polynomial methods.Additional comments including Restrictions and Unusual features:The WavePacket program package is rather easy and intuitive to use, providing visualization of quantum dynamics ‘on the fly’. It is mainly intended for low-dimensional systems, typically not exceeding three to five degrees of freedom. Detailed user guides and reference manuals are available through numerous Wiki pages hosted at the SourceForge platform where also a large number of well documented demonstration examples can be found.

Impacts of Surface Site Coordination on Arsenate Adsorption: Macroscopic Uptake and Binding Mechanisms on Aluminum Hydroxide Surfaces.

Aluminum hydroxides play important roles in regulating the fate and transport of contaminants and nutrients in soils and aquatic systems. Like many metal oxides, these minerals display surface functional groups in a series of coordination states, each of which may differ in its affinity for adsorbates. The distribution of functional group types varies among distinct surfaces of aluminum hydroxides, and we thus hypothesize that the adsorption behavior and mechanisms will show a dependence on particle morphology. To test this hypothesis, we investigate arsenate adsorption on two aluminum hydroxide polymorphs with distinct particle morphologies, gibbsite [γ-Al(OH)3] and bayerite [α-Al(OH)3], at pH 4 and 7. Synthetic gibbsite platelets expose large (001) basal surfaces predicted to be terminated by doubly coordinated functional groups (>Al2OH). In contrast, synthetic bayerite microrods display mainly edge surfaces (parallel to the c axis) containing abundant singly coordinated functional groups (>AlOH2). Macroscopic adsorption studies show that gibbsite adsorbs less arsenate per unit surface area than bayerite at both pH values and suggest that two surface complexes form on each material. Similar electrokinetic behavior is displayed at the same relative coverages of arsenate, suggesting that similar reactive surface groups (>AlOH2) control the surface charging on both particles. EXAFS spectroscopy shows that there is no variation in arsenate surface speciation on a given mineral with surface coverage or pH. Whereas bidentate binuclear inner-sphere species are the dominant complexes present, the EXAFS result suggest that outer-sphere species also occur on both minerals, with a greater abundance on gibbsite. This binding mode likely involves adsorption to >Al2OH sites, which have a slow ligand exchange rate that inhibits inner-sphere binding. These results demonstrate that adsorption mechanisms and capacity, even when normalized for specific surface area, vary with metal oxide particle morphology because of the distribution of distinct functional groups.

Random Bosonic States for Robust Quantum Metrology

We study how useful random states are for quantum metrology, i.e., surpass the classical limits imposed on precision in the canonical phase estimation scenario. First, we prove that random pure states drawn from the Hilbert space of distinguishable particles typically do not lead to super-classical scaling of precision even when allowing for local unitary optimization. Conversely, we show that random states from the symmetric subspace typically achieve the optimal Heisenberg scaling without the need for local unitary optimization. Surprisingly, the Heisenberg scaling is observed for states of arbitrarily low purity and preserved under finite particle losses. Moreover, we prove that for such states a standard photon-counting interferometric measurement suffices to typically achieve the Heisenberg scaling of precision for all possible values of the phase at the same time. Finally, we demonstrate that metrologically useful states can be prepared with short random optical circuits generated from three types of beam-splitters and a non-linear (Kerr-like) transformation.

Intonation and Particles as Speech Act Modifiers: A Syntactic Analysis

AbstractThis study investigates how discourse particles and intonation contribute to the modification of speech act. In particular, it focuses on the interplay between the speaker’s and the addressee’s commitment toward the proposition in assertions, biased questions, and requests for confirmation. A syntactic analysis is proposed, in whichspeaker commitmentandcall on addresseeare represented as two functional projections of the speech act structure. Data from nontonal (Canadian English) and tonal languages (Cantonese and Medumba) are analyzed for cross-linguistic comparison. In Canadian English, the particle “eh” and rising intonation are associated with speaker commitment and call on addressee, respectively. In Cantonese, a single particle associates with these. In Medumba, the two positions are occupied by two distinct particles. This neo-performative approach toward speech act structure differs from Ross’s 1970 original insight by positing a high functional layer calledgrounding, rather than a higher matrix clause of the familiar type.

Exploring the Different Roles of Particle Size in Photoelectrochemical and Photocatalytic Water Oxidation on BiVO4.

Water oxidation on visible-light-active bismuth vanadate (BiVO4) has commonly been demonstrated to be viable in powder suspension (PS) and particulate photoelectrochemical (PEC) systems. Here, we demonstrate that particle size reduction, which is known to be efficacious in promoting charge carrier extraction and boosting surface active sites, has an opposite effect on BiVO4's photoactivity in the two systems. With three BiVO4 samples of distinctive particle sizes, smaller BiVO4 particle size is shown to be beneficial for enhancing PEC photocurrent generation, but deleterious for photocatalytic O2 evolution on suspended BiVO4. Such contrary effect of particle size in the PEC and PS systems is revealed to be due to the different governing factors of the systems: charge transport in the former and charge separation in the latter. Smaller particle size was found to enrich the interparticle and the particle/FTO substrate contacts which improve charge transport and charge collection efficiency in BiVO4 particulate electrode. On the contrary, larger particle size is necessary for improved photocatalytic O2 evolution because of increased crystallinity and greater band bending, which are essential for charge separation.

Dissociation and coagulation of caseins and whey proteins in concentrated skim milk heated by direct steam injection

Heat treatment of concentrated milk systems for preservation and long shelf life or at least a sufficient removal of food pathogens prior to spray drying is a crucial step due to the decreasing stability of these systems toward heat compared to unconcentrated milk. Heat-induced coagulation is observed when temperature-time combinations for the achievement of certain microbial inactivation effects are higher than the heat and colloidal stability of the concentrated milk system allows. In this work, the effects of direct steam injection on the stability of casein micelles in concentrated skim milk (CSM) of 18, 23, and 27% total non-fat solids, heat-treated by direct steam injection (DSI), were investigated. Quantitative differential centrifugation for the separation of aggregates, casein micelles, dissociated submicellar particles, and soluble proteins and subsequent analysis of caseins and whey proteins within these fractions by RP-HPLC were applied. Quantitative separation was monitored by particle size measurements. The dissociation of κ-casein as well as an increase in casein micelle hydrodynamic radius were observed to increase with increasing total solid content of CSM, heat treatment time, and temperature. Heat-induced dissociation of β-Lg-κ-casein complexes at a critical level of 30–35% was found to induce severe coagulation of κ-casein-depleted calcium-sensitive casein micelles in CSM heated by DSI. Dissociated and aggregated proteins were found to be present as distinct colloidal particle classes differing in size from casein micelles.

Heteronuclear Efimov Scenario with Positive Intraspecies Scattering Length.

We investigate theoretically and experimentally the heteronuclear Efimov scenario for a three-body system that consists of two bosons and one distinguishable particle with positive intraspecies scattering lengths. The three-body parameter at the three-body scattering threshold and the scaling factor between consecutive Efimov resonances are found to be controlled by the scattering length between the two bosons, approximately independent of short-range physics. We observe two excited-state Efimov resonances in the three-body recombination spectra of an ultracold mixture of fermionic ^{6}Li and bosonic ^{133}Cs atoms close to a Li-Cs Feshbach resonance, where the Cs-Cs interaction is positive. Deviation of the obtained scaling factor of 4.0(3) from the universal prediction of 4.9 and the absence of the ground state Efimov resonance shed new light on the interpretation of the universality and the discrete scaling behavior of heteronuclear Efimov physics.

A Round Robin study for Selective Laser Sintering of polyamide 12: Microstructural origin of the mechanical properties

The mechanical and microstructural investigation of polymer parts (polyamide 12) fabricated by Selective Laser Sintering as part of a Round Robin initiative is presented. The paper focuses on the microstructural analysis of the Round Robin samples and their evaluation regarding their effect on mechanical properties with respect to each other. Therefore optical microscopy on microtomed samples, X-ray computed tomography and Differential Scanning Calorimetry is used to determine the morphology of residual particle cores and of internal pores.The mechanical tensile testing revealed a high variability of the ductility of the samples among the used machines and a distinctive anisotropic mechanical response. Especially the quite brittle characteristic along the building direction has shown to be still a crucial challenge for the process. However, one machine delivered samples with outstanding ductility with total elongation values of about 21% along the building direction and of about 32% planar to the layer. This result was back traced to a distinctive pore and residual particle morphology which is characterized by low pore concentration, the absence of coplanar pore or residual particle arrangements and the highest degree of particle melting measured. Furthermore, the analysis depicts that both features, pores and residual particles, contribute to the mechanical properties significantly and that they are not necessarily linked since they can vary independently in a certain range depending on the machine configuration.

Head-on collision of two dust ion acoustic solitary waves in a weakly relativistic multicomponent superthermal plasma

A head-on collision between two dust ion acoustic solitary waves (DIASWs) travelling in the opposite direction in a weakly relativistic plasma composed of four distinct particle populations, namely, weakly relativistic ion fluid, superthermal electrons as well as positrons, and immobile dust, is investigated. By employing extended Poincaré-Lighthill-Kuo method, two Korteweg-de Vries (KdV) equations are derived. The analytical phase shift after a head-on collision of two dust ion acoustic (DIA) solitary waves is also obtained. The combined effects of relativistic factor (β), electron to positron temperature ratio (α), ion to electron temperature ratio (σ), positron to electron density ratio (P), dust density ratio (d), and superthermality of electrons as well as positrons (via κ) on the phase shifts are numerically studied. All these physical parameters have also changed the potential amplitude and the width of colliding solitary waves. It is found that the presence of superthermal electrons as well as positrons and dust grains has emphatic influence on the phase shifts and potential pulse profiles of compressive DIA solitons. Our results are general and may be helpful in understanding a head-on collision between two DIASWs in astrophysical and laboratory plasmas, especially the interaction of pulsar relativistic winds with supernova ejecta that produces the superthermal particles and relativistic ions.

How to observe duality in entanglement of two distinguishable particles

The entanglement between two bosons or fermions can be accessed if there exists an auxiliary degree of freedom which can be used to label and effectively distinguish the two particles. For some types of entanglement between two indistinguishable particles one can observe duality, i.e., if the entanglement is present in the Hilbert space H and an auxiliary Hilbert space H' is used to label the particles, then if we used H as a label the entanglement would be present in H'. For distinguishable particles this effect does not occur because of superselection rules which prevent superpositions of different types of particles. However, it is known that superselection rules can be bypassed if one uses special auxiliary states that are known as reference frames. Here we study properties of reference frames which allow for an observation of a duality in entanglement between two distinguishable particles. Finally, we discuss the consequences of this result from the resource-theoretic point of view.

Insights into the inner structure of high-nickel agglomerate as high-performance lithium-ion cathodes

In this paper, the intrinsic impact of inner structure features on the electrochemical performances of LiNi0.6Co0.2Mn0.2O2 cathodes is for the first time systematically investigated. Three different spherical Ni0.6Co0.2Mn0.2(OH)2 precursors are successfully synthesized by controlling pH values and ammonia concentrations. Interestingly, via a further lithiation process, the final cathodes can gradually inherit the structural features, showing distinct particle arrangement and genetic orientation characteristics in the inner structures. Such a hereditary property can be well reined for customizing the grain-orientation, helping the growth of the inert crystal direction, reducing cation mixing and exposing the high active (100) or (010) lattice planes for lithiation/delithiation processes via an intrinsical way. The degree of grain-orientation of the primary particles turns out to be a critical factor in determining the long-term stability and power performances. Due to the reduced cation mixing degree and favorable lithium diffusion pathways, the ordered agglomerates with the grain growth along with [003] direction exhibit superior rate capability and good cycle stability.

Novel cellular perlite-epoxy foams: Effects of particle size

The micro-structure and mechanical properties of lightweight porous foams synthesized by dispersing expanded perlite particles (expanded siliceous volcanic glass) in a matrix of epoxy resin were examined. Foams were fabricated with three distinct particle size ranges and, within each size, samples covered a density range of 0.15–0.45 g/cm3. The effects of particle size variation on compressive strength, effective elastic modulus, and modulus of toughness were investigated. An upper and a lower bound were estimated for the elastic modulus of particles in EP/epoxy foams. EP/epoxy foams showed Reuss-like behaviour similar to metals but atypical of non-plastic materials. In addition, results illustrated the significant contribution of the expanded perlite particles in the effective elastic modulus of the foams. Micro-structure of expanded perlite particles was examined and related to their macroscopic properties via two geometrical relationships. Post-test microscopic observations coupled with macroscopic observations taken during the test were used to understand the effect of particle size on the behaviour of the foams under compressive load. Observations revealed the presence of three different failure modes for all foams regardless of their particle size and density; however, the strain to activate each mode was different for each foam type.

Bead-Based Microfluidic Sediment Analogues: Fabrication and Colloid Transport.

Mobile colloids can act as carriers for low-solubility contaminants in the environment. However, the dominant mechanism for this colloid-facilitated transport of chemicals is unclear. Therefore, we developed a bead-based microfluidic platform of sediment analogues and measured both single and population transport of model colloids. The porous medium is assembled through a bead-by-bead injection method. This approach has the versatility to build both electrostatically homogeneous and heterogeneous media at the pore scale. A T-junction at the exit also allowed for encapsulation and enumeration of colloids effluent at single particle resolution to give population dynamics. Tortuosity calculated from pore-scale trajectory analysis and its comparison with lattice Boltzmann simulations revealed that transport of colloids was influenced by the size exclusion effect. The porous media packed by positively and negatively charged beads into two layers showed distinctive colloidal particle retention and significant remobilization and re-adsorption of particles during water flushing. We demonstrated the potential of our method to fabricate porous media with surface heterogeneities at the pore scale. With both single and population dynamics measurement, our platform has the potential to connect pore-scale and macroscale colloid transport on a lab scale and to quantify the impact of grain surface heterogeneities that are natural in the subsurface environment.

Corrosion Protection of Zinc Alloy Coated Steel By Organic Coatings Pigmented with Strontium Aluminium Polyphosphate

Strontium aluminium polyphosphate (SAPP) inhibitive pigment formulated into an organic primer for corrosion protection of zinc alloy coated steel in 0.6 M sodium chloride solution was investigated by serial block face imaging using scanning electron microscopy, which provided detailed information on inhibitor releasing, transportation and reaction with zinc alloy substrate. It was found that SAPP contains at least two distinct particle types, one which is strontium rich and another which is aluminium rich. These particles have different release characteristics which are dependent on the local environment. The strontium rich particles release their components faster in near neutral and acidic environment compared with the aluminium rich particles whilst in an alkaline environment the reverse is found. The pH related inhibitor release process and the mixture of the inhibitive pigment with different strontium to aluminium ratios ensure the availability of the inhibitor at both anodic and cathodic locations, which consequently reduced/retarded the corrosion of zinc alloy coated steel.

Mean-square radii of two-component three-body systems in two spatial dimensions

We calculate root-mean-square radii for a three-body system confined to two spatial dimensions and consisting of two identical bosons ($A$) and one distinguishable particle ($B$). We use zero-range two-body interactions between each of the pairs, and focus thereby directly on universal properties. We solve the Faddeev equations in momentum space and express the mean-square radii in terms of first-order derivatives of the Fourier transforms of densities. The strengths of the interactions are adjusted for each set of masses to produce equal two-body bound-state energies between different pairs. The mass ratio, ${\cal A}=m_B/m_A$, between particles $B$ and $A$ are varied from $0.01$ to $100$ providing a number of bound states decreasing from $8$ to $2$. Energies and mean-square radii of these states are analyzed for small ${\cal A}$ by use of the Born-Oppenheimer potential between the two heavy $A$-particles. For large ${\cal A}$ the radii of the two bound states are consistent with a slightly asymmetric three-body structure. When ${\cal A}$ approaches thresholds for binding of the three-body excited states, the corresponding mean-square radii diverge inversely proportional to the deviation of the three-body energy from the two-body thresholds. The structures at these three-body thresholds correspond to bound $AB$-dimers and one loosely bound $A$-particle.