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The rotating spectrometer: New biotechnology for cell separations

An instrument for biochemical studies, called the rotating spectrometer, separates previously inseparable cell cultures. The rotating spectrometer is intended for use in pharmacological studies which require fractional splitting of heterogeneous cell cultures based on cell morphology and swimming behavior. As a method to separate and concentrate cells in free solution, the rotating method requires active organism participation and can effectively split the large class of organisms known to form spontaneous patterns. Examples include the biochemical star, an organism called Tetrahymena pyriformis. Following focusing in a rotated frame, the separation is accomplished using different radial dependencies of concentrated algal and protozoan species. The focusing itself appears as concentric rings and arises from the coupling between swimming direction and Coriolis forces. A dense cut is taken at varying radii and extraction is replenished at an inlet. Unlike standard separation and concentrating techniques such as filtration or centrifugation, the instrument is able to separate motile from immotile fractions. For a single pass, typical split efficiencies can reach 200 to 300 percent compared to the inlet concentration.

Noever, David A.↗

The rotating spectrometer: Biotechnology for cell separations

An instrument for biochemical studies, called the rotating spectrometer, separates previously inseparable cell cultures. The rotating spectrometer is intended for use in pharmacological studies which require fractional splitting of heterogeneous cell cultures based on cell morphology and swimming behavior. As a method to separate and concentrate cells in free solution, the rotating method requires active organism participation and can effectively split the large class of organisms known to form spontaneous patterns. Examples include the biochemical star, an organism called Tetrahymena pyriformis. Following focusing in a rotating frame, the separation is accomplished using different radial dependencies of concentrated algal and protozoan species. The focusing itself appears as concentric rings and arises from the coupling between swimming direction and Coriolis forces. A dense cut is taken at varying radii, and extraction is replenished at an inlet. Unlike standard separation and concentrating techniques such as filtration or centrifugation, the instrument is able to separate motile from immotile fractions. For a single pass, typical split efficiencies can reach 200 to 300 percent compared to the inlet concentration.

Noever, David A.↗

Influences of Local Sea-Surface Temperatures and Large-scale Dynamics on Monthly Precipitation Inferred from Two 10-year GCM-Simulations

Two parallel sets of 10-year long: January 1, 1982 to December 31, 1991, simulations were made with the finite volume General Circulation Model (fvGCM) in which the model integrations were forced with prescribed sea-surface temperature fields (SSTs) available as two separate SST-datasets. One dataset contained naturally varying monthly SSTs for the chosen period, and the oth& had the 12-monthly mean SSTs for the same period. Plots of evaporation, precipitation, and atmosphere-column moisture convergence, binned by l C SST intervals show that except for the tropics, the precipitation is more strongly constrained by large-scale dynamics as opposed to local SST. Binning data by SST naturally provided an ensemble average of data contributed from disparate locations with same SST; such averages could be expected to mitigate all location related influences. However, the plots revealed: i) evaporation, vertical velocity, and precipitation are very robust and remarkably similar for each of the two simulations and even for the data from 1987-ENSO-year simulation; ii) while the evaporation increased monotonically with SST up to about 27 C, the precipitation did not; iii) precipitation correlated much better with the column vertical velocity as opposed to SST suggesting that the influence of dynamical circulation including non-local SSTs is stronger than local-SSTs. The precipitation fields were doubly binned with respect to SST and boundary-layer mass and/or moisture convergence. The analysis discerned the rate of change of precipitation with local SST as a sum of partial derivative of precipitation with local SST plus partial derivative of precipitation with boundary layer moisture convergence multiplied by the rate of change of boundary-layer moisture convergence with SST (see Eqn. 3 of Section 4.5). This analysis is mathematically rigorous as well as provides a quantitative measure of the influence of local SST on the local precipitation. The results were recast to examine the dependence of local rainfall on local SSTs; it was discernible only in the tropics. Our methodology can be used for computing relationship between any forcing function and its effect(s) on a chosen field.

Sud, Y. C.↗

Third-body stabilization of supercritical CO 2 in CO oxidation: development and application of a ReaxFF force field for the CO/O/CO 2 system

Supercritical CO 2 (scCO 2 ) plays a crucial role as a solvent in separation processes, advanced power cycles, and materials processing. Nonetheless, the atomistic comprehension of how the dense scCO 2 matrix influences the fundamental reaction of carbon monoxide (CO) is still insufficiently explored. Experimental studies and molecular dynamics (MD) simulations frequently fail to detect the highly reactive, transient intermediates, such as atomic oxygen (O), that drive these reactions. Here, to address this issue, we have developed a novel ReaxFF reactive force field for the CO 2 /CO/O system. The force field parameters were calibrated using density functional theory and second-order Møller-Plesset calculations to model CO 2 crystal properties, intermolecular interactions, bond dissociation curves, and reaction energy barriers. The force field reproduces the cohesive energy of the CO 2 crystal, the pressure characteristics of bulk scCO 2 , the equation-of-state behavior over a wide pressure–density range, the pressure dependence of the C–O bond length under compression, and the structural properties of liquid and scCO 2 , as documented by experiments, ab-initio MD, and prominent non-reactive models. The force field was subsequently applied to study the CO + O → CO 2 reaction. In a dilute environment, the reaction is inefficient as the newly formed CO 2 rapidly dissociates due to excess kinetic and potential energy acquired from the exothermic reaction. Conversely, in a dense scCO 2 environment, the surrounding matrix acts as an efficient third body, stabilizing the emerging CO2 product via molecular collisions. Statistical analysis confirms an average excess energy dissipation of 133.9 ± 3.6 kcal/mol over 112.4 ± 17.9 ps. Kinetic energy decomposition reveals that ∼ 92% of the excess kinetic energy is stored in internal (rotational and vibrational) degrees of freedom. This ReaxFF force field establishes a mechanistic foundation for third-body stabilization in dense reactive environments.

Chowdhury, Emdadul Haque [Pennsylvania State Univ.↗

"Coulombic Viscosity" In Granular Materials: Planetary and Astrophysical Implications

The term "Coulombic viscosity" is introduced here to define an empirically observed phenomenon from experiments conducted in both microgravity, and in ground-based 1-g conditions. In the latter case, a sand attrition device was employed to test the longevity of aeolian materials by creating two intersecting grain-circulation paths or cells that would lead to most of the grain energy being expended on grain-to-grain collisions (simulating dune systems). In the areas in the device where gravitationally-driven grain-slurries recycled the sand, the slurries moved with a boundary-layer impeded motion down the chamber walls. Excessive electrostatic charging of the grains during these experiments was prevented by the use of an a.c. corona (created by a Tesla coil) through which the grains passed on every cycle. This created both positive and negative ions which neutralized the triboelectrically-generated grain charges. When the corona was switched on, the velocity of the wall-attached slurries increased by a factor of two as approximately determined by direct observation. What appeared to be a freely-flowing slurry of grains impeded only by intergranular mechanical friction, had obviously been significantly retarded in its motion by electrostatic forces between the grains; with the charging reduced, the grains were able to move past one another without a flow "viscosity" imposed by the Coulombic intergranular forces. A similar phenomenon was observed during microgravity experiments aboard Space Shuttle in USML-1 & USML-2 spacelabs where freely-suspended clouds of sand were being investigated for their potential to for-m aggregates. In this environment, the grains were also charged electrostatically (by natural processes prior to flight), but were free from the intervention of gravity in their interactions. The grains were dispersed into dense clouds by bursts of air turbulence and allowed to form aggregates as the ballistic and turbulent motions damped out. During this very brief (30-60 sec) damping period, motion of the grains was observed to be retarded by the electrostatic interactions. The fact that the grains almost instantly formed aggregates was evidence that their ballistic motions had been constrained and redirected by the dipole-dipole interactions that led to filamentary aggregate development. Undoubtedly, the "Coulombic viscosity" of the cloud assisted in damping grain motion so rapidly. The electrostatically-induced grain-cloud viscosity or drag exerted on grain motion, is a complex function of three major parameters: charge magnitude, charge sign, and mean intergranular distance. The above experiments illustrate one particular type of granular behavior. The discussion here will therefore be restricted to drag relationships: (a) between grains that are naturally charged triboelectrically and thus exhibit dipole-dipole attractions between one another even if there are slight net charges present (which can be overwhelmed by dipole coupling at short distances), and (b) between grains that are densely spaced where the intergranular distance varies between zero and some value (usually tens or hundreds of grain diameters) that permits each grain to detect the dipole moment of another grain -- the distance is not so great that other grains appears as neutral electrical "singularities. I. Aeolian transport: During motion of grains in a saltation cloud (on Earth, Mars, or Venus), triboelectric charging must occur as a result of multiple grain contacts, and by friction with the entraining air. A situation might develop that is similar to the one described above in the attrition device: grain motion becoming significantly retarded (reduced flux) as grains find it increasingly difficult to either separate from the surface, or to pass one another without Coulombic retarding forces. A "Coulombic drag" will exist at flux initiation and increase with time to work in direct opposition to the aerodynamic drag that drives the grain motion. It is predicted that this will lead to an increase with time of both the aerodynamic and bed-dilatancy thresholds (3). Because of Paschen discharge effects in the martian atmosphere, the electrostatic charging in a saltation cloud may be partially abated, but this will lead to greater grain mobility, more charging, and thus to a charge-discharge steady state mediated by mechanical interactions. II. Dry colluvial systems: Sand avalanches on dunes, dry debris flows, talus flows, avalanches, and pyroclastic surges are examples of gravity-driven, dense granular flows where rock/grain fragmentation and grain-to-grain interactions cause triboelectrification (sometimes augmented by other electrical charging processes), and where the grain densities of the systems are such that strong dipole-dipole interactions between grains might be expected to be present. Because it is expected that the Coulombic forces between grains will cause a sluggishness or enhanced granular-flow viscosity, the motion of a grain mass will be retarded or damped so that this will assist, ultimately, in terminating the flow. The greatest Coulombic viscosity will be created in the most highly charged systems, which will also be the most energetic. Thus, grain flows have some tendency to be self-limiting by internal energy partitioning; gravitational potential is converted to Coulombic potential, which manifests itself as a drag force between the grains. III. Volcanic eruption plumes and impact ejecta curtains: The violence of these systems leads to powerful electrical charging of particulates. Lightning storms emanating from volcanic plumes are a testimony to the levels of charging. As pyroclastic grains interact forcefully and frequently within eruption plumes, it is reasonable to predict that the internal turbulent motions of the plume will be significantly damped by the Coulombic viscosity exerted by grain charges. Additional information is contained in the original.

Marshall, J. R.↗

Ion Association in AlCl3 Aqueous Solutions from Constrained First-Principles Molecular Dynamics

Ab initio molecular dynamics was used to investigate the ion pairing behavior between Cl- and the Al3+ ion in an aqueous AlCl3 solution containing 63 water molecules. A series of constrained simulations was carried out at 300 K for up to 16 ps each, by fixing the inter-nuclear separation (rAl-Cl) between the Al3+ ion and one of the Cl- ions. The calculated potential of mean force of the Al3+-Cl- ion pair shows a pronounced minimum at rAl-Cl = 2.3 Å corresponding to a contact ion pair (CIP). Two local minima assigned to solvent separated ion pairs (SSIP) are identified at rAl-Cl= 4.4 and 6.0 Å. The positions of the free energy minima coincide with the hydration shell intervals of the Al3+ cation suggesting that the Cl- ion is inclined to reside in regions of low concentration of waters, i.e. between the 1st and 2nd shells of Al3+ and between the 2nd shell and bulk. A detailed analysis of solvent structure around the Al3+ and Cl- ions as a function of rAl-Cl is presented. The results are compared to structure data from X-ray measurements and unconstrained AIMD simulations of single ions Al3+ and Cl- and AlCl3 solutions. The dipole moment of the water molecules inside the 1st and 2nd hydration shells of Al3+ and in the bulk region and those of the Clion were calculated as a function of rAl-Cl. Major changes in the electronic structure of the system result from the removal of Cl- from the 1st hydration shell of the Al3+ cation. Finally, two unconstrained AIMD simulations of aqueous AlCl3 solutions corresponding to CIP and SSIP configurations were performed (17 ps, 300 K). Only minor structural changes are observed in these systems, confirming their stability.

ab initio↗

Effects of Frothers and Oil at Saltwater–Air Interfaces for Oil Separation: Molecular Dynamics Simulations and Experimental Measurements

Separating oil from saltwater is a process relevant to some industries and may be aided by bubble and froth generation. Simulating saltwater–air interfaces adsorbed with surfactants and oil molecules can assist in understanding froth stability to improve separation. Here, combining with surface tension experimental measurements, in this work we employ molecular dynamics with a united-atom force field to linear alkane oil and three surfactant frothers, methyl isobutyl carbinol (MIBC), terpineol, and ethyl glycol butyl ether (EGBE), to investigate their synergistic behaviors for oil separation. The interfacial phenomena were measured for a range of frother surface coverages on saltwater. Density profiles of the hydrophilic and hydrophobic portions of the frothers show an expected orientation of alcohol groups adsorbing to the polar water. A decrease in surface tension with increasing surface coverage of MIBC and terpineol was observed and reflected in experiments where the frother concentration increased. Relations between surface coverage and bulk concentration were observed by comparing the surface tension decreases. Additionally, a range of oil surface coverages was explored when the interface has a thin layer of adsorbed frother molecules. Finally, the obtained results indicate that an increase in surface coverage of oil molecules led to an increase in surface tension for all frother types and the pair correlation functions depicted MIBC and terpineol as having higher distributions with water at closer distances than with oil.

54 ENVIRONMENTAL SCIENCES↗

Remote and Ground Truth Spectral Measurement Comparisons

FORMOSAT III are a set of six research satellites from Taiwan that were launched in April 2006. The satellites are in 800 km, 71 degree inclination orbits and separated by 24 degrees in ascending node. Ground truth spectral measurements were taken of outer surface materials on FORMOSAT III. From those measurements, a computer model was built to predict the spectral reflectance, which included phase angle and orientation of the spacecraft relative to the observer. However, materials exposed to the space environment have exhibited spectral changes including a darkening and a reddening of the spectra. This reddening was seen as an increase in slope of the reflectance as the wavelength increases. Therefore, the model of pristine materials was augmented to include the space weathering effects. Remote data were collected on two of the six FORMOSAT satellites using the 1.6 meter telescope at AMOS (Air Force Maui Optical and Supercomputing) site with the Spica spectrometer. Due to the separation in ascending node, observations were made on whichever one of the six satellites was visible on that specific night. Three nights of data were collected using the red (6000 9500 angstroms) filter and two nights of data were collected using the blue (3200 -6600 angstroms) filter. A comparison of the data showed a good match to the pristine model for the blue filter region. The absorption feature near 5500 angstroms due to the copper colored Kapton multi-layer insulation (MLI) was very apparent in the remote samples and a good fit to the data was seen in both satellites observed. The features in the red filter regime agreed with the pristine model up through 7000 angstroms where the reddening begins and the slope of the remote sample increases. A comparison of the two satellites showed similar features in the red and blue filter regions, i.e. the satellites were aging at the same rate. A comparison of the pristine model to the first month of remote measurements showed the amount by which the satellite had reddened. This information was used in the space weathered model to predict the second month s reflectance measurement. The results showed that the reddening did not increase from the first month of observations to the second. A third month of data will be necessary to determine if the reddening occurs instantly and then stabilizes with time or if the effect continues to increase with time.

Abercromby, Kira Jorgensen↗

The Effect of QBO Phase on the Atmospheric Response to Projected Arctic Sea Ice Loss in Early Winter

Recent modeling studies have shown an important role for stratosphere-troposphere coupling in the large-scale atmospheric response to Arctic sea ice loss. Evidence is growing that the Quasi-biennial Oscillation (QBO) can contribute to or even mitigate teleconnections from surface forcing. Here, the influence of QBO phase on the atmospheric response to projected Arctic sea ice loss is examined using an atmospheric general circulation model with a well-resolved stratosphere and a QBO prescribed from observations. The role of the QBO is determined by compositing seasons with easterly phase (QBO-E) separately from seasons with westerly phase (QBO-W). In response to the sea ice forcing in early winter, the polar vortex during QBO-E weakens with strong stratosphere-troposphere wave-1 coupling and a negative Northern Annular Mode-type response. At the surface, this results in more severe Siberian cold spells. For QBO-W, the polar vortex strengthens in response to the sea ice forcing.

58 GEOSCIENCES↗

Forced Synchronization of Electroconvective Roll Oscillations in Nematic Liquid Crystals

The forced phase locking in a system of the oscillating electroconvective rolls that form in a nematic liquid crystal layer in a dc electric field is studied. As a result of the action of an additive ac electric field with a small amplitude, the system of oscillators is found to be divided into clusters, where oscillations are fully phase locked. The electroconvective rolls in neighboring clusters oscillate in antiphase and the clusters are separated by Ising walls. The phase locking is shown to be maximal at the forcing frequency that is close to the double frequency of the natural oscillations of rolls. A model is proposed to describe spatially distributed phase oscillators, and it takes into account the symmetries of a system of electroconvective rolls and external forcing. The results of numerical simulations agree well with the experimental data.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Remote and Ground Truth Spectral Measurement Comparisons of FORMOSAT III

FORMOSAT III are a set of six research satellites from Taiwan that were launched in April 2006. The satellites are in 800 km, 71 degree inclination orbits and separated by 24 degrees in ascending node. Laboratory spectral measurements were taken of outer surface materials on FORMOSAT III. From those measurements, a computer model was built to predict the spectral reflectance accounting for both solar phase angle and orientation of the spacecraft relative to the observer. However, materials exposed to the space environment have exhibited spectral changes including a darkening and a "reddening" of the spectra. This "reddening" is characterized by an increase in slope of the reflectance as the wavelength increases. Therefore, the model of pre-flight materials was augmented to include the presumed causative agent: space weathering effects. Remote data were collected on two of the six FORMOSAT satellites using the 1.6 meter telescope at the AMOS (Air Force Maui Optical and Supercomputing) site with the Spica spectrometer. Due to the separation in ascending node, observations were acquired of whichever one of the six satellites was visible on that specific night. Three nights of data were collected using the red (6000 - 9500 angstroms) filter and five nights of data were collected using the blue (3200 - 6600 angstroms) filter. A comparison of the data showed a good match to the pre-flight models for the blue filter region. The absorption feature near 5500 angstroms due to the copper colored Kapton multi-layer insulation (MLI) was very apparent in the remote samples and a good fit to the data was seen in all satellites observed. The features in the red filter regime agreed with the pre-flight model up through 7000 angstroms where the reddening begins and the slope of the remote sample increases. A comparison of the satellites showed similar features in the red and blue filter regions, i.e. the satellite surfaces were aging at the same rate. A comparison of the pre-flight model to the first month of remote measurements showed the amount by which the satellite had reddened. The second month of data observed a satellite at a higher altitude and was therefore, not compared to the first month. A third month of data was collected but of satellites at the lower altitude regime and can only be compared to the first month. One cause of the reddening that was ruled out in early papers was a possible calibration issue.

Abercromby, Kira Jorgensen↗

Application of the vortex-lattice technique to the analysis of thin wings with vortex separation and thick multi-element wings

Two techniques for extending the range of applicability of the basic vortex-lattice method are discussed. The first improves the computation of aerodynamic forces on thin, low-aspect-ratio wings of arbitrary planforms at subsonic Mach numbers by including the effects of leading-edge and tip vortex separation, characteristic of this type wing, through use of the well-known suction-analogy method of E. C. Polhamus. Comparisons with experimental data for a variety of planforms are presented. The second consists of the use of the vortex-lattice method to predict pressure distributions over thick multi-element wings (wings with leading- and trailing-edge devices). A method of laying out the lattice is described which gives accurate pressures on the top and part of the bottom surface of the wing. Limited comparisons between the result predicted by this method, the conventional lattice arrangement method, experimental data, and 2-D potential flow analysis techniques are presented.

Smith, C. W.↗

A Parametric Study of the Aerodynamic Characteristics of Nose-Cylinder-Flare Bodies at a Mach Number of 6.0

Force tests were conducted at a Mach number of 6.0 on nose-cylinder-flare bodies to determine the effect of nose shape, cylinder length, flare angle, and flare length on the longitudinal aerodynamic characteristics. A particular investigation was conducted to determine the effect of flare angle for constant flare length, surface area, and diameter. Results indicated that at a Reynolds number of approximately 0.92 x l0 (exp 6) (based on body diameter), the boundary-layer separation effects were significant only with respect to the slope of the normal-force and pitching-moment curve at low angles of attack. The variations of the aerodynamic characteristics with the various parameters were, in general, similar to those predicted by Newtonian theory below a flare angle of 30 degrees and a ratio of flare base diameter to cylinder diameter of less than approximately 2.2. The limiting diameter ratio is consistent with the extent of the low-constant dynamic-pressure region near the body caused by the bow-shock influences as predicted by axisymmetric characteristic theory. The effects of the various parameters for the flares that exceeded the limiting diameter ratio follow the trends predicted by the computed flow-field properties. The axial force for these flare configurations at zero angle of attack was, in general, computed within 10 percent by using these properties. For a constant flare length and surface area the flare effectiveness increased with increasing flare angle; however, for constant flare diameter only the axial-force coefficient was affected by flare angle.

Ashby, George C., Jr.↗

Probing the core of the strong nuclear interaction

The strong nuclear interaction between nucleons (protons and neutrons) is the effective force that holds the atomic nucleus together. This force stems from fundamental interactions between quarks and gluons (the constituents of nucleons) that are described by the equations of quantum chromodynamics. However, as these equations cannot be solved directly, nuclear interactions are described using simplified models, which are well constrained at typical inter-nucleon distances but not at shorter distances. This limits our ability to describe high-density nuclear matter such as that in the cores of neutron stars. Here we use high-energy electron scattering measurements that isolate nucleon pairs in short-distance, high-momentum configurations, accessing a kinematical regime that has not been previously explored by experiments, corresponding to relative momenta between the pair above 400 mega electron volts per c (c, speed of light in vacuum). As the relative momentum between two nucleons increases and their separation thereby decreases, we observe a transition from a spin-dependent tensor force to a predominantly spin-independent scalar force. These results demonstrate the usefulness of using such measurements to study the nuclear interaction at short distances and also support the use of point-like nucleon models with two- and three-body effective interactions to describe nuclear systems up to densities several times higher than the central density of the nucleus.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Space shuttle vehicle rocket plume impingement study for separation analysis. Tasks 2 and 3: Definition and preliminary plume impingement analysis for the MSC booster

The results are presented of a space shuttle plume impingement study for the Manned Spacecraft Center configuration. This study was conducted as two tasks which were to (1) define the orbiter main stage engine exhaust plume flow field, and (2) define the plume impingement heating, force and resulting moment environments on the booster during the staging maneuver. To adequately define these environments during the staging maneuver and allow for deviation from the nominal separation trajectory, a multitude of relative orbiter/booster positions are analyzed which map the region that contains the separation trajectories. The data presented can be used to determine a separation trajectory which will result in acceptable impingement heating rates, forces, and the resulting moments. The data, presented in graphical form, include the effect of roll, pitch and yaw maneuvers for the booster. Quasi-steady state analysis methods were used with the orbiter engine operating at full thrust. To obtain partial thrust results, simple ratio equations are presented.

Wojciechowski, C. J.↗

Active Flow Control at Low Reynolds Numbers on a NACA 0015 Airfoil

Results from a low Reynolds number wind tunnel experiment on a NACA 0015 airfoil with a 30% chord trailing edge flap tested at deflection angles of 0, 20, and 40 are presented and discussed. Zero net mass flux periodic excitation was applied at the ap shoulder to control flow separation for flap deflections larger than 0. The primary objective of the experiment was to compare force and moment data obtained from integrating surface pressures to data obtained from a 5-component strain-gage balance in preparation for additional three-dimensional testing of the model. To achieve this objective, active flow control is applied at an angle of attack of 6 where published results indicate that oscillatory momentum coefficients exceeding 1% are required to delay separation. Periodic excitation with an oscillatory momentum coefficient of 1.5% and a reduced frequency of 0.71 caused a significant delay of separation on the airfoil with a flap deflection of 20. Higher momentum coefficients at the same reduced frequency were required to achieve a similar level of flow attachment on the airfoil with a flap deflection of 40. There was a favorable comparison between the balance and integrated pressure force and moment results.

Melton, LaTunia Pack↗

Advanced Modeling of Ions in Solutions, on Surfaces, and in Biological Environments (Final Scientific/Technical Report)

The research supported by this grant focused on modeling liquid water from basic microscopic theory and on developing advanced methodologies for molecular simulation and electronic structure calculation of large and disordered systems. Water is arguably the most important molecule on earth: without it there would be no life, as we know it. Water does not behave as a simple liquid. Understanding its unique and anomalous properties at the molecular level has been the focus of intense study during the entire last century and still is a major goal of research today. To address the problem we adopted a multipronged approach that included methodological and algorithmic developments as well as simulations of important model systems. We made progress on several key issues. (i) We implemented accurate electronic structure schemes for modeling water from quantum mechanical theory that make accessible in simulations processes driven by formation and breaking of chemical bonds. We studied in this way neat bulk water and simple solvated ions. We could understand, in particular, why hydronium, i.e. the positive water ion, diffuses faster than its negative counterpart, the hydroxyl, solving a 200-year-old ionic mystery of water, as reported in a news article featuring our study on Chemistry World, the magazine of the Royal Society of Chemistry (U.K.). (ii) Using advanced statistical mechanical techniques we studied water in the deeply undercooled regime, which may hold the clue to understanding many of the water anomalies. These conditions are currently only accessible to simulations based on empirical force fields. We found that deeply undercooled water, as described by the popular force field ST2, possesses a secondary critical point, below which it would spontaneously separate into two liquids, one of low-density (LDL) and one of high-density (HDL), much in the same way in which water and oil phase-separate at room temperature. The secondary critical point is supported indirectly by many experiments, but rapid ice nucleation has so far hindered direct observation. In related studies we gained new insight on the connection of the two metastable liquids with the two corresponding amorphous ice phases, LDA and HDA, which are observed experimentally. (iii) We developed and implemented several new algorithms for computing the electronic structure of large systems and to accelerate the calculation of electron exchange energies. We applied these methodologies to model nanomaterials, such as nanoribbons and nanoflakes, and to study water absorption and splitting on nanomaterials. (iv) We developed new local order descriptors. (v) In the last year of the project we developed a methodology based on deep neural networks to construct model interatomic potentials that can accurately reproduce ab-initio quantum mechanical simulations at the computational cost of empirical force fields. These potentials will make possible to access the size and time scales that are currently only accessible with empirical force fields without loosing the predictive power of ab-initio simulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Axial acoustic radiation force on a sphere in Gaussian field

Based on the finite series method, the acoustical radiation force resulting from a Gaussian beam incident on a spherical object is investigated analytically. When the position of the particles deviating from the center of the beam, the Gaussian beam is expanded as a spherical function at the center of the particles and the expanded coefficients of the Gaussian beam is calculated. The analytical expression of the acoustic radiation force on spherical particles deviating from the Gaussian beam center is deduced. The acoustic radiation force affected by the acoustic frequency and the offset distance from the Gaussian beam center is investigated. Results have been presented for Gaussian beams with different wavelengths and it has been shown that the interaction of a Gaussian beam with a sphere can result in attractive axial force under specific operational conditions. Results indicate the capability of manipulating and separating spherical spheres based on their mechanical and acoustical properties, the results provided here may provide a theoretical basis for development of single-beam acoustical tweezers.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗